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Contents

Neutronics feasibility of using Gd2O3 particles in VVER-1000 fuel assembly


Hoang Van Khanh, Hoang Thanh Phi Hung, Tran Hoai Nam………………………………01

Design and Construction of a Preamplifier for Research Reactor Control System Using
Russia’s Neutron Detectors
Trinh Dinh Hai, Vo Van Tai, Le Van Diep, Nguyen Nhi Dien..………………………………08

Development of an MCNP5-ORIGEN2 coupling scheme for burnup calculation of VVER-


1000 fuel assemblies
Nguyen Huy Hiep, Nguyen Huu Tiep, Tran Viet Phu, Nguyen Tuan Khai………………..…16

Research and design of the moving system for the cobalt-60 industrial irradiator
Le Minh Tuan, Tran Khac An, Cao Van Chung, Phan Phuoc Thang……………………...…31

UV light induced DNA damages and the radiation protection effects of Lingzi mushrom extract
Vo Thi Thuong Lan, Dinh Ba Tuan, Ta Bich Thuan, Tran Bang Diep, Tran Minh Quynh…...40

The effect of gamma-irradiation on graphene oxide in a monoglyceride/ethanol solution


Luu Anh Tuyen, Ha Thuc Huy, Nguyen Thanh Duoc, Doan Binh, Pham Thi Thu Hong...…48

The Brandon mathematical model describing the effect of calcination and reduction
parameters on specific surface area of ex-ADU UO2 powders
Nguyen Trong Hung, Le Ba Thuan, et.al. ..………………………………………………………54

The efficient neutron-gamma pulse shape discrimination with small active volume
scintillation detector
Phan Van Chuan, Nguyen Duc Hoa, Nguyen Xuan Hai, Nguyen Ngoc Anh, Tuong Thi Thu
Huong, Nguyen Nhi Dien, Pham Dinh Khang…………...………………………………………60
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 01-07

Neutronics feasibility of using Gd2O3 particles


in VVER-1000 fuel assembly
Hoang Van Khanh1, Hoang Thanh Phi Hung2 and Tran Hoai Nam3,*
1)
Institute for Nuclear Science and Technology, VINATOM, 179 Hoang Quoc Viet, Hanoi, Vietnam
2)
Nuclear Training Center, VINATOM, 140 Nguyen Tuan, Hanoi, Vietnam
3)
Institute of Research and Development, Duy Tan University, Da Nang, Vietnam
*E-mail: tranhoainamk3@gmail.com
(Received 07 June 2016, accepted 28 August 2016)

Abstract. Neutronics feasibility of using Gd2O3 particles for controlling excess reactivity of VVER-
1000 fuel assembly has been investigated. The motivation is that the use of Gd 2O3 particles would
increase the thermal conductivity of the UO2+Gd2O3 fuel pellet which is one of the desirable
characteristics for designing future high burnup fuel. The calculation results show that the Gd 2O3
particles with the diameter of 60 µm could control the reactivity similarly to that of homogeneous
mixture with the same amount of Gd2O3. The power densities at the fuel pin with Gd2O3 particles
increase by about 10-11%, leading to the decrease of the power peak and a slightly flatter power
distribution. The power peak appears at the periphery pins at the beginning of burnup process which is
decreased by 0.9 % when using Gd2O3 particles. Further work and improvement are being planned to
optimize the high power peaking at the beginning of burnup.
Keywords: Fuel assembly, Gd2O3 particle, power distribution, and VVER.

I. INTRODUCTION Gd2O3 particles in the UO2 matrix could be a


solution. It was reported that the thermal
In LWRs, Gd2O3 is loaded in several fuel conductivity of Gd2O3-dispersed UO2 is larger
assemblies as burnable poison for controlling than that of (U,Gd)O2 solid solutions with the
excess reactivity of the fresh fuel and the same Gd2O3 content [3].
reactor core at the beginning of burnup stage.
The purpose is to avoid an excessively high Iwasaki et al. [4] conducted experiments
power peak at some fresh fuel assemblies. After to investigate the effect of Gd2O3 dispersion
a burnup level of about 10-15 GWd/t, main on the thermal conductivity. The results
absorbing isotopes, Gd155 and Gd157, which are showed that 10 wt% Gd2O3-dispersed UO2
about 30% in the natural gadolinium, are pellet with the diameter of Gd 2O3 particles of
depleted completely and the reactivity about 25-53 µm has the thermal conductivity
decreases with burnup similarly to other of about 5.8-2.7 W/mK in the temperature
assemblies without Gd2O3. In conventional range from 300 to 1273 K. This is larger than
design, an amount of Gd2O3 within a few that of homogeneous mixed solid solutions
percent is mixed homogeneously with UO2 in (3.8 to 2.6 W/mK) with the same Gd2O3
several fuel pins of a fuel assembly. Since content [4]. This means that the use of Gd2O3
Gd2O3 has a smaller thermal conductivity than particles could improve the thermal
that of UO2, its content leads to the decrease of conductivity of UO2-Gd2O3 pellets effectively.
the thermal conductivity of the fuel pellet [1]- For the purpose of the reduction of fuel costs,
[3]. In order to avoid the problem, the use of power upgrade and advanced fuel design with

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
NEUTRONICS FEASIBILITY OF USING Gd2O3 PARTICLES IN VVER-1000 FUEL ASSEMBLY

high burnup is desirable. Since power upgrade enrichment of 3.7 wt% and 12 UO2+Gd2O3
and high burnup fuel lead to the increase of the fuel pins as shown in Fig. 1. In the numerical
power density, the increase of the thermal calculation model, spherical Gd2O3 particles
conductivity of the fuel pellets would be one are assumed to be distributed randomly in the
of the desirable characteristics of fuel. UO2 matrix of the fuel pellet. The statistical
Regarding the fabrication possibility of the geometry (STG) model of the MVP code
Gd2O3-dispersed UO2 fuel pellet, as mentioned allows simulating the random distribution of
in Ref. [4] it was processed similarly to the the Gd2O3 particles. In the calculations, the
traditional fuel pellet with Gd 2O3 powder. history number of 25 ×106 is chosen to
Gd2O3 particles are weighted and mixed with achieve the relative statistic error of the k∞
UO2 powder in a mortar. The mixture was then within 0.01%. Calculations have been
pressed into a form of fuel pellet and sintered performed for two models of the fuel
under a high pressure and high temperature assembly: one with the homogeneous
condition. distribution of Gd2O3 powder in the UO 2 fuel
pins, and the other with the distribution of
In the present work, we investigated, in
Gd2O3 particles.
neutronics point of view, the feasibility of
using Gd 2O3 particles for reactivity Table I. Design parameters of the VVER-1000 fuel
controlling and the effect on the neutronics assembly [5]
performance of the VVER-1000 fuel
assembly. Spherical Gd2O3 particles were Parameters Values
distributed randomly in the UO 2 matrix of Number of central tube cell (-) 1
fuel pellet. The size of the Gd 2O3 particles
Number of guide tube cell (-) 18
was determined for controlling the reactivity
of the fuel assembly during burnup so that the Number of fuel cell with Gd (-) 12
target is to obtain the k∞ curve similarly to Number of fuel cell (-) 300
that of the conventional fuel assembly.
Fuel cell inner radius (cm) 0.3860
Comparison of the pin-wise power
Fuel cell outter radius (cm) 0.4582
distribution between the new design and the
conventional assembly has also been Central tube cell inner radius (cm) 0.5450
presented. Central tube cell outter radius (cm) 0.6323
Cell pin pitch (cm) 1.2750
II. CALCULATION MODEL
Fuel assembly pitch (cm) 23.6
Numerical calculations have been
Non-fuel zones temperature (K) 575.0
performed based on the low enriched UO 2
fuel assembly of VVER-1000 reactor core Fuel zones temperature (K) 1027.0
using the Monte Carlo neutron transport MVP UO2
code and the JENDLE-3.3 library [6],[7]. The Fuel (wt% 235U) (3.6)
configuration and the detailed design Gd2O3 density (g/cm3) 7.4
parameters of the fuel assembly are displayed
Boron concentration (g/cm3) 0.7235
in Fig.1Fig. 1 and Table . The assembly
consists of 300 UO2 fuel pins with the 235U

2
HOANG VAN KHANH, HOANG THANH PHI HUNG, TRAN HOAI NAM

Fig. 1. Configuration of fuel assembly

III. RESULTS AND DISCUSSIONS


In the calculation procedure, we assume
In the present work, we investigate the that the same Gd2O3 amount is loaded into the
use of Gd2O3 particles instead of homogeneous fuel pins, i.e. 5% of volume, as in the
distribution for the purpose of reactivity conventional assembly. Then, a parametric
controlling and improving the thermal survey was conducted to optimize the diameter
conductivity of the fuel pins. The size of the of the Gd2O3 particles for reactivity control.
shows the effect of the diameter of the Gd2O3
Gd2O3 particles is determined so that the k∞ of
particles on the reactivity curves of the fuel
the fuel assembly is controlled similarly to that
assembly in the burnup range from 0 to 10
of the conventional fuel. In the conventional
GWd/t with the diameter varying from 40 to 100
design, the k∞ of the fuel assembly is
µm. Since we aims at finding a reactivity curve
controlled from the beginning of burnup upto
close to the conventional one in this burnup
about 10 GWd/t. After this burnup level, most
range, the diameter of 60 µm was selected for
of the absorbing isotopes are depleted and the
further calculations. Fig. 3 displays the k∞ curve
k∞ decreases similar to that of the fuel
of the new fuel assembly with the Gd2O3
assembly without Gd2O3. Thus, in the first
spherical particles having the diameter of 60 µm
stage of this design, we set the target to obtain
and the packing fraction of 5% (the volume ratio
a similar k∞ curve of the new fuel assembly
of the Gd2O3 particles and the matrix base in the
compared to that of the conventional design.
STG model). This k∞ curve is similar to that of
Previous works used Gd2O3 particles for
the conventional design with homogeneous
controlling the reactivity of a fuel pebble of a mixed Gd2O3. Other neutronics characteristics
pebble bed reactor upto 60-100 GWd/t. were also computed and compared to that of the
Therefore, the radius of the particles of 820 or conventional design. Fig. 4 displays the change
950 µm was selected [8],[9]. However, in the of the 155Gd and 157Gd densities as a function of
current design of the fuel assembly we aim at bunrup in the two designs. It is noted that the
controlling the reactivity upto 10 GWd/t, so change of the Gd densities is slightly different
that the radius of the particles could be between two cases because the particles with the
predicted much smaller than 820 or 950 µm, diameter of 60 µm have small self-shielding
and therefore, the self-shielding effect of the effect and its function is slightly similar to the
particles is also smaller. homogeneous distribution.

3
NEUTRONICS FEASIBILITY OF USING Gd2O3 PARTICLES IN VVER-1000 FUEL ASSEMBLY

Fig. 2. Effect of the diameter of Gd2O3 particles on the Fig. 3. The k∞ as a function of burnup of the VVER-1000
reactivity of the fuel assembly at the beginning of burnup fuel assembly. The diameter of 60 µm was selected

Fig. 4. Densities of 155Gd and 157Gd with burnup

Fig. 5. Comparison of pin-wise power distribution at 0 GWd/t

4
HOANG VAN KHANH, HOANG THANH PHI HUNG, TRAN HOAI NAM

Fig. 6. Comparison of pin-wise power distribution at 5 GWd/t

Fig. 5 displays the pin-wise power pin-wise power distribution of the fuel
distribution at the beginning of burnup (0 assembly becomes slightly flatter.
GWd/t) in the new designed fuel assembly with
Fig. 6 and Fig. 7 show the same pin-wise
Gd2O3 particles in comparison with that of the
power distribution as Fig. 5 but at the burnup
conventional assembly. The figure shows the
levels of 5 and 10 GWd/t since in this burnup
power in the 1/6th of the fuel assembly due to
stage the Gd2O3 still has effect on the
the symmetrical geometry. One can see that at
characteristics of the fuel assembly. At these
the two UO2+Gd2O3 fuel pins, the relative
burnup steps, the relative power at the Gd2O3 -
power densities at 0 GWd/t increase about 11%
dispersed fuel pins increases upto 1.8%
when using Gd2O3 particles compared to the
compared to that of the conventional assembly.
that of fuel pin with Gd2O3 mixed
At these burnup, part of the Gd2O3 particles has
homogeneously with UO2. At other fuel pins,
been burnt, and the function of the Gd2O3
the relative power densities decrease within
particles approaches to the homogeneous
0.6% in the outer region and increase within
distribution. This means that the difference of
0.8% in the central region. As a result, the
relative power in the Gd2O3-dispersed fuel pin
power peak appearing at the periphery fuel pin
is smaller compared to that at the beginning of
decreases by 0.9% (from 1.167 to 1.156). This
burnup stage (0 GWd/t).
means that by using the Gd2O3 particles, the

5
NEUTRONICS FEASIBILITY OF USING Gd2O3 PARTICLES IN VVER-1000 FUEL ASSEMBLY

Fig. 7. Comparison of pin-wise power distribution at 10 GWd/t

Fig. 8. Pin-wise power peaking factor during burnup

Fig. 8 depicts the pin-wise power decreases with burnup and becomes slightly
peaking factor as a function of burnup of the stable around the value of 1.040-1.060 after 10
new fuel assembly in comparison with that of GWd/t. By using the Gd2O3 particles the power
the conventional design. The power peaking peaking factor decreases slightly by about 0.9%
factor is greater in the burnup stage of 0-10 at the beginning of burnup. However, the main
GWd/t when the Gd2O3 amount has effect on merit achieved for the new fuel assembly with
the reactivity. The power peaking factor Gd2O3 particles is the increase of the thermal

6
HOANG VAN KHANH, HOANG THANH PHI HUNG, TRAN HOAI NAM

conductivity of the fuel pellet [4]. The results ACKNOWLEDGEMENT


obtained in this preliminary investigation show
that in the neutronics point of view it is feasible This research is funded by Vietnam
to use Gd2O3 particles instead of powder in the National Foundation for Science and
UO2 fuel pellet for excess reactivity controlling, Technology Development (NAFOSTED) under
while the main neutronics characteristics could grant number 103.04-2014.79.
be obtained similarly to that of the conventional
REFERENCES
design. From the evolution of the power
peaking factor with burnup as shown in Fig. , it [1] S. Fukushima, T. Ohmichi, A. Maeda, H.
suggests that the further investigation should be Watanabe, "The effect of gadolinium content
conducted to flatten the power peaking in the on the thermal conductivity of near-
early burnup stage of the fuel assembly. stoichiometric (U,Gd)O2 solid solutions". J.
Nucl. Mater., 105, 201–210, 1982.
IV. CONCLUSIONS [2] M. Amaya, M. Hirai, H. Sakurai, K. Ito, M.
Sasaki, T. Nomata, K. Kamimura, R. Iwasaki,
Investigation of the neutronics feasibility "Thermal conductivities of irradiated UO2 and
of using Gd2O3 particles in the UO2 fuel pellet of (U,Gd)O2 pellets". J. Nucl. Mater., 300, 57–64,
the VVER-1000 fuel assembly has been 2002.
conducted. The motivation is that by using [3] D. Balestrieri, IAEA Technical Committee
Gd2O3 particles instead of powder the thermal Meeting on Advances in Pellet Technology for
conductivity of the UO2+ Gd2O3 fuel pellet Improved Performance at High Burnup, Paper
would increase [4]. The results show that with No. 2-1, 1996.
the same content of 5% in volume, Gd2O3 [4] K. Iwasaki, T. Matsui, K. Yanai, R. Yuda, Y.
particles with the diameter of 60 µm control Arita, T. Nagasaki, N. Yokoyama, I. Tokura, K.
reactivity similarly to the homogeneous mixture. Une, K. Harada, "Effect of Gd2O3 dispersion on
the thermal conductivity of UO2". J. Nucl. Sci.
The power density at the fuel pin with Gd2O3
Technol., 46:7, 673-676, 2009.
particles increases by about 11% at the
beginning of burnup which leads to the slight [5] NEA/NSC/DOC 10, Nuclear Energy Agency,
decrease of power peak and slightly flatter power Organization for Economic Co-operation and
Development, 2002.
distribution. The power peak appearing at the
periphery pins at the beginning of burnup [6] Nagaya, Y., Okumura, K., Mori, T., Nakagawa,
decreases by 0.9% when using Gd2O3 particles. M., MVP/GMVP II: general purpose Monte
Carlo codes for neutron and photon transport
The results demonstrate that by loading the same
calculations based on continuous energy and
amount of Gd2O3 but in form of particles with multigroup methods. JAER, I–1348, 2005.
the diameter of 60 µm instead of the powder in
[7] Shibata, K., et al., "Japanese evaluated nuclear
the UO2 fuel pellet, the neutronics properties of
data library version 3 revision-3: Jendl-3.3", J.
the new fuel assembly could be obtained Nucl. Sci. Technol. 39, 1125–1136, 2002.
similarly to that of the conventional design.
[8] H.N. Tran, Y. Kato, "An optimal loading
In the future work, further investigation principle of burnable poisons for an OTTO
are being conducted to optimize the high power refueling scheme in pebble bed HTGR cores".
peaking at the beginning of burnup using Gd2O3 Nucl. Eng. Des 239, 2357–2364, 2009.
particles. Thermal hydraulics analysis of the new [9] H.N. Tran, V.K. Hoang, "Neutronic
fuel assembly will also be investigated in order characteristics of an OTTO refueling PBMR".
to estimate the advantage of the new design. Nucl. Eng. Des. 253, 269– 276, 2012.

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Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 08-15

Design and Construction of a Preamplifier for Research


Reactor Control System Using Russia’s Neutron Detectors
Trinh Dinh Hai, Vo Van Tai, Le Van Diep, Nguyen Nhi Dien

Dalat Nuclear Research Institute, 01 Nguyen Tu Luc, Dalat, Vietnam


(Received 10 August 2016, accepted 19 August 2016)

Abstract: This paper presents the design and construction of a preamplifier device for Research
Reactor Control System, using Russia’s Neutron Detectors of ionization and fission chambers. In this
work, the preamplifier device which consists of a wide range Current to Frequency Converter block
used with a compensation ionization chamber type KNK-3 to measure the thermal neutron flux in the
range of 1x106  1x1011 n/cm2.s, a Pulse Preamplifier block used with a fission chamber type KNK-15
to measure the thermal neutron flux in the range of 1x10 0  1x106 n/cm2.s, and a Power Supply block,
was designed and tested in different conditions in the laboratory and at Dalat Nuclear Research
Reactor (DNRR). Obtained results show that, the above blocks have almost design specifications as
equivalent or better in comparison with the same function blocks of the DNRR’s Control System
which were designed by the former Soviet Union. They also meet the utilization requirements as well
as the experimental and training purposes.
Keywords: Dalat Nuclear Research Reactor (DNRR), Instrumentation and Control (I&C), Fission
Chamber (FC), Compensation Ionization Chamber (CIC), Pulse Preamplifier (PP), Current to
Frequency Converter (CFC).

individual measuring channels (3 channels in


I. INTRODUCTION
each IAPU):
The original DNRR’s I&C system was
designed and manufactured by the former - Source range (SR), 10-8  10-2% Pn;
Soviet Union and put into operation in - Intermediate range (IR), 10-3  10% Pn;
November 1983. This system is divided into
- Power range (PR), 1  120% Pn.
four main parts [2, 5]: neutron flux control
system (NFCS), reactor data display system To control the neutron flux of the
(RDDS), control logic system (CLS), and reactor, nine neutron detectors with gamma
process and instrumentation system (PIS). The compensation (6 fission chambers type KNK-
NFCS measures the power and period of the 15 and 3 compensation ionization chambers
reactor; giving out analogue signal type KNK-3) were used. The KNK-15
proportional to the unbalance between the chambers are operated in the pulse mode for
reactor and the setting powers; and giving out the SR and IR ranges, while the KNK-3
alarm and scram signals on power and period chambers are used in current mode for the
for each measuring channel. The NFCS system power range. After the modernization and
consists of three identical and independent refurbishment project during 2005-2007 with
electronic units, namely, the information the replacement of neutron measurement and
acquisition and processing units (IAPU). The signal processing parts of the original I&C
neutron flux is measured over ten decades 10-8 system, two individual measuring channels (SR
 1.2x102 %Pn, Pn = 500 kWt) and is covered and PR) of IAPUs were kept for the
by three overlapping measure ranges by nine experimental purposes.

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
TRINH DINH HAI, VO VAN TAI, LE VAN DIEP, NGUYEN NHI DIEN

In order to master the DNRR’s I&C II. DESIGN AND CONSTRUCTION OF


system not only for managing and safety THE PREAMPLIFIER DEVICE
operation of the reactor but also for the
development of human resources in serving A. The detectors
nuclear power program in the future, in the Two types of KNK-3 and KNK-15
framework of the MOST’s research project detectors of the old IAPU’s were used for
during 2013-2014, we have studied on the testing, calibration and evaluation of the new
design and construction of the new designed preamplifier device. Technical
preamplifier device consisted of a wide range specifications of these detectors are given in
Current to Frequency Converter block, a Pulse Table I and Fig. 1 [3, 4]. These detectors are
Preamplifier block and a Power Supply block, placed in the dry channels outside the reactor
and used the Russia’s Neutron Detectors of the core without the surrounding radiation
old IAPUs mentioned above. Main obtained shielding structure and tested with the different
results of the studies are presented and levels of reactor power.
discussed in this paper.

Table I. Specifications of KNK-3 and KNK-15.

Fig. 1. The diagram of KNK-3 and KNK-15 detectors.

9
DESIGN AND CONSTRUCTION OF A PREAMPLIFIER FOR …

B. Pulse Preamplifier block [1] Discriminator D7 is used for separating


useful signals from noises which amplitude is
1. Design description
less than the amplitude of useful signals. By
Pulse Preamplifier block is intended for means of discriminator D6, noise pulses
amplification of paraphrase current pulses from comparable by amplitude with useful signals
KNK-15 detector, for discrimination of noise are selected. Pulses from discriminator D6 are
pulses and for generation of pulses caused by generated at univibrator UV and interlock
neutron radiation. Its structural diagram is passing of noise signals by means of passage
shown in Fig. 2. circuit (PSC). Output signal is pulse
In order to increase its noise immunity, frequency which is in proportion with neutron
after preamplifier D1 (D1 is a voltage sensitive flux. Counting rate metter (CRM) is used for
amplifier, which used transistor common base automatically changing discrimination
configuration), amplifier is divided into two threshold Uth2 to reduce noise pulses. It plays
channels: the channel of useful signals an important role for more rejection of noise
amplification (D3, D5) and the channel of pulses caused by the pulse pile-up. This is an
noises separation (D2, D4). Amplification advanced design to expand the frequency
sections of both channels are built on range of input pulses from neutron detector.
operational amplifiers, and communications In the checking mode, generator of pulses
between them are organized in such a way that (GPch) is started by trigger from a power
in one channel useful paraphrase signals are supply (Vch).
amplified in maximum extent, and in other
channel - inphase noise pulses are separated.

-400VDC
R60 Check
1 2
Uch +Vch
KNK-15
R18 R59
1k
R64
+12v
Uth2
C4
GPch CRM
R19 10nF R58
1k

D4 D6 UV
SIGNAL D2 OUT

R4
1k D1 PSC
D3 COUNTER
D5
R1 C3 R34 D7 DT
1k 10nF

Uth1 +12v
+250VDC R63

NOTE:
D1: PREAMPLIFIER PSC: PASSAGE CIRCUIT
D2-D5: AMPLIFIER CRM: COUNTING RATE METER
D6-D7: DISCRIMINATOR Uth1,2: WORKING DISCRIMINATION THRESHOLD
DT: CIRCUIT OF SAMPLING BY DURATION GPch: GENERATOR OF PULSES OF CHECK
UV: UNIVIBRATOR +Vch: +12V CHECK

Fig. 2.The structural diagram of the pulse amplifier.


2. Testing and results etc. The Pulse Preamplifier was also tested in
In the laboratory: many conditions of temperature and humidity
in the Programmable Temperature and
The designed Pulse Preamplifier block Humidity Chamber (KEJIAN KJ2091 No.15-
has been tested and calibrated in the laboratory 226). The testing diagram is shown in Fig. 3,
for correction of important parameters such as: and the relation between input and output pulse
the gain of preamplifier, discrimination frequency is shown in Fig. 4.
thresholds and range of operating frequency,

10
TRINH DINH HAI, VO VAN TAI, LE VAN DIEP, NGUYEN NHI DIEN

Pulse Preamplifier Oscillocope

Frequency F Tek TDS1012


Generator Devide

TG501 Signal 1 Frequency meter

GFC-8131H
Signal 2

GND
-12V

+12V

+5V

GND

Fig. 3. Testing diagram for the pulse preamplifier block.

Fig. 4. The relation between input and output pulse frequency.

At the reactor: power level and output pulse frequency of the


Pulse Preamplifier block are shown in Fig. 6.
The Pulse Preamplifier block was
In the range of power levels from 10-5 Pn to 10-2
connected to the KNK-15 detector of the
%Pn, output pulse frequencies are in good
source chanel No.1 and tested at some reactor
proportion with the reactor power levels.
power levels from 10-5 to 10-2% Pn (Fig. 5).
The testing results and the relation between

Fig. 5. Testing of the Pulse Preamplifier block at the DNRR.

11
DESIGN AND CONSTRUCTION OF A PREAMPLIFIER FOR …

Fig. 6. The relation between power and frequency.


3. Main specifications of the Pulse actuates and the output signal from the Comp
Preamplifier block triggers univibrator UV.
- Sensitivity: 1 cps/n; At the output of the univibrator, pulse of
- Measurement range of thermal neutron flux: the positive polarity with the duration
0,1 ÷ 2.105 nv; determined by a resistance R1 and a capacitor
- Range of output frequency: 0.1 Hz ÷ 250 kHz; C1, starts the operation of discharge circuit and
- Pulse amplitude: +12V; the capacitor Cin is discharged. The rheostart
- Power supply: +12VDC/ 400mA, -12VDC/ Rconv is used for fine regulation of the
200mA and +5VDC/300mA. conversion coefficient.
C. Current to Frequency Converter block In “Test” mode, potential +12V is
1. Design description supplied to relay Re, through the contacts of
relay current I_ch is applied to input of
The Current to Frequency Converter (CFC) converter via resistors Rch1 and Rch2. The
block has been designed and developed based on current value is selected in such a way that
the balanced charge integrating techniques with output pulses of the converter have fixed
the structural diagram is given in Fig. 7. frequency equal to 25 kHz.
The input current (I_in) from KNK-3 Compensation resistors Rcomp1
detector is charged for capacitor Cin, included (smoothly) and Rcomp2 (discretely) are used
into negative feedback circuit of operation for compensation of background current.
amplifier (Amp). When the voltage at the
output of integrator achieves the value equal to
the threshold of the comparator, the Comp
Rch1
-400VDC +12V -12V
5
KNK-3 4
3

R18 1
1k Rcomp1 2 Test
+12V -12V
+12V
Re
Rch2
C4 Rcomp2 I_ch
R19 10nF
1k R1 C1
I_comp
R
SIGNAL
I_in Amp Comp F_out
R4
1k
UV TG ER

R1 C3
1k 10nF

+250VDC
Vref

Cin Discharge Rconv

Fig. 7. The block diagram of the current to frequency converter.

12
TRINH DINH HAI, VO VAN TAI, LE VAN DIEP, NGUYEN NHI DIEN

2. Testing and results diagram is shown in Fig. 8 and the dependence


In the laboratory: of the output pulse frequency on the input
The CFC block covers the range from 3 current value is shown in Fig. 9.
nA to 1 mA of the input current. The testing

+
- P4833
SW

R1 R2
1M 10K
KEITHLEY 614 PREAMPLIFIER FREQUENCY COUNTER
ELECTROMETER GND
+ - - GFC-8131H
I_IN F_OUT
nA uA +

Fig. 8. The testing diagram for the CFC block.

Fig. 9. The relation between input current and output pulse frequency of the CFC.
At the reactor: connected to the KNK-3 detector of the power
The maximum output current from the range No.1 and tested at some reactor power
KNK-3 detector at power of 500 kW is only levels from 10-1 to 102% Pn (Fig. 10.a). Fig. 10.b
about 400μA, so that the CFC block was shows the relation between the power levels and
calibrated for working in the range from 1 nA to the output frequencies of the CFC block.
400 μA of the input current. The CFC was

(a) (b)
Fig. 10. Testing CFC block at the Dalat NRR.

13
DESIGN AND CONSTRUCTION OF A PREAMPLIFIER FOR …

3. Main specifications of the CFC block Table II. Main specifications of the power supply block.

- Range of input current: 3 nA  1 mA; High voltage power Low voltage power
supply supply
- Range of output frequency: 0 Hz  350 kHz;
Input voltage: 10.8 Input voltage: 18  36
- Linearity in full range: 99%; VDC to 13.2 VDC VDC
- Pulse amplitude: +12V; Positive high voltage Output voltage ±
adjustment range from 12VDC and output
- Power supply: ±12 VDC/200mA and +5 0 to +500 VDC current max: 1250 mA
VDC/300mA. Negative high voltage Output voltage +5
adjustment range from VDC and output
D. Power Supply block [1] 0 to -500 VDC current max: 1000mA
The Power Supply block is intended Max Current: 6mA Ripple and noise: <
±30mVpk
for the organization of electric supply for
Ripple and noise: 30
neutron detectors, CFC and Pulse mVPk-Pk
Preamplifier blocks. It consists of a high Short circuit and over
voltage power supply unit and a low voltage voltage protection
power supply unit. The high voltage power The power supply block was tested in
supply unit used THV 12-500P/N different conditions of temperature and
components and the low power supply unit humidity with all its main specifications as
used TEN15-2412 components of TRACO shown in Fig. 11. The testing results were
POWER Company. Its main specifications presented in the final report of the research
are shown in the Table II. project [1].

Fig. 11. Testing of the power supply block.

III. CONCLUSION order to fully test the Pulse Preamplifier block


at the operation condition of the reactor, a
A new preamplifier device (Fig. 12)
special permit and significant time resources
which intended for research reactor I&C
were required. In this regard, a device that
system, has been designed and constructed. The
simulates the FC signals in different modes is
testing results have shown that almost its
necessary to design and fabricate [6]. FC signal
design specifications are equivalent or better in
simulator allows us to generate a model signal
comparison with the same function blocks of
of FC in a wide range of pulse rates, i.e. allows
the DNRR’s control system which was made
modeling different modes of FC.
by the former Soviet Union and can be used for
the experimental and training purposes. In

14
TRINH DINH HAI, VO VAN TAI, LE VAN DIEP, NGUYEN NHI DIEN

Fig. 12. The designed preamplifier device.

REFERENCES [4] И. Я. Емельянов, А.И. Ефанов, Л. В.


Констатинов, Научно –технические основы
[1] Trinh Dinh Hai, Final report of the MOST’s управления ядерными реакторами, Москва
research project: Study on design and Энергоиздат 1981.
fabrication of a preamplifier device using for
[5] Dien Nguyen Nhi and Hai Trinh Dinh, Dalat
nuclear research reactor control system, Dalat
research reactor and its control and
2015.
instrumentation system renovation, IAEA-
[2] Комплекс Аппаратуры Контроля TECDOC-1625, August 2009.
Нейтронного Потока -5.
[6] A. V. Batyunin, V. A. Vorobyev, S. Yu.
Техническое Описание и Инструкция по
Obudovsky, S. A. Shvikin, Yu. A. Kaschuck,
эксплутации, 1981.
Fission chamber simulator for data acquisition
[3] С. В Волков, Н. С Кирилин, Детекторы performance tests, DOI:
нейтронов для программно-управляемых 10.1109/ANIMMA.2013.6728083.
каналов контроля нейтронного потока,
Приборы и системы. Упраправление,
контроль, диагностика. No. 10, 2006.

15
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 16-30

Development of an MCNP5-ORIGEN2 coupling scheme for


burnup calculation of VVER-1000 fuel assemblies
Nguyen Huy Hiep*, Nguyen Huu Tiep, Tran Viet Phu, Nguyen Tuan Khai

Nuclear Power Center, Institute for Nuclear Science and Technology


179 Hoang Quoc Viet, Nghia Do, Cau Giay, Hanoi, Vietnam
*email: huyhiep.sneep@gmail.com
(Received 15 July 2016, accepted 15 September 2016)

Abstract: The paper aims to develop an MCNP5-ORIGEN2 coupling scheme for burnup calculation.
Specifically, the Monte Carlo neutron transport code (MCNP5) and the nuclides depletion and decay
calculation code (ORIGEN2) are combined by data processing and linking files written in the PERL
programming language. The validity and applicability of the developed coupling scheme are tested
through predicting the neutronic and isotopic behavior of the “VVER-1000 LEU Assembly
Computational Benchmark”. The MCNP5-ORIGEN2 coupling results showed a good agreement with
the k-inf benchmark values within 600 pcm during the entire burnup history. In addition, the
differences of isotopes concentration at the end of the burnup (40 MWd/kgHM) when compared with
benchmark values were reasonable and generally within 6.5%. The developed coupling scheme also
considered the shielding effect due to gadolinium isotopes and simulated well the depletion of isotopes
as a function of the radial position in gadolinium bearing fuel rods.
Keywords: MCNP5, ORIGEN2, burnup, coupling, VVER-1000 LEU.

I. INTRODUCTION weeks. Such weakness is no longer a too difficult


problem because nowadays, computers are able
In the field of reactor core management, to perform simulations much more efficiently
which consists of nuclear fuel burnup calculation, and quickly than before. For this reason, the
deterministic and Monte Carlo methods are Monte Carlo based codes are being widely used
widely used to solve the neutron transport in nuclear reactors calculation.
equation. Each method has advantages and
weaknesses. Deterministic method (e.g., In recent decades, a number of Monte
collision probability method) has major Carlo burnup calculation code systems have
advantage of the short computer time needed to been developed worldwide thanks to the
find solutions while the disadvantages are related advancement of computer science. Some Monte
to the energy groups collapsing or the ability Carlo codes were added with an auxiliary
dealing with complicated reactor core geometries, module which has the function of depletion
which may lead to significant errors in the calculation such as MVP-BURN [1] and
results. Whereas, the Monte Carlo based codes BURNCAL [2] while several ones were
such as MCNP can model an arbitrary geometry coupled with a special depletion and decay
and use continuous energy libraries. For that calculation code such as the MCNP-ORIGEN
reason, they will provide high accurate solution coupling strategy based codes, which are
to the neutron transport equation. However, the regularly used. In detail, MCNP [3]
Monte Carlo method requests to use a large performance provides some parameters such as
number of neutron histories and consequently multiplication factor, neutron flux distribution,
this can be time consuming. For example, a and neutron cross sections for a given
simulation with multiple runs may be of little compositional model while ORIGEN [4]
practical value if each run requires days or calculates time-dependent fuel material

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

compositions via irradiation, transmutation, these MCNP-ORIGEN burnup calculation code


activation, fission, and decay in the nuclear systems, which are mentioned above, have a
reactor environment. The first MCNP-ORIGEN special attention in ORIGEN depletion
coupling program was created in 1995 by the calculation. The fact is that the cross sections
Idaho National Engineering and Environmental and neutron flux values vary continuously
Laboratory (INEEL) with the name MOCUP throughout reactor operation time, thus
(MCNP-ORIGEN Coupling Utility Program) beginning-of-time-step values are not fully
[5]. MOCUP was written in ANSI C representative of the entire time step, unless the
programming language and had a friendly time step is extremely small. For instance, in
interactive interface which was based on the MOCUP, cross sections and flux values at
portable X11 window environment and the beginning-of-time-step are assumed constant
Motif tool kit. MOCUP, however, only over the entire time step. With such simple
accounted for 17 actinides (ACT) and 41 fission method, the user needs small enough time steps
products (FP). Four years later (1999), the Los to obtain high accurate results. After the
Alamos National Laboratory (LANL) released development of MOCUP, other MCNP-
their version of an MCNP-ORIGEN coupler, ORIGEN coupling codes used a predictor-
MONTEBURNS [6], written in FORTRAN and corrector algorithm for the depletion calculation
PERL. MONTEBURNS used a simple in ORIGEN. This integrated algorithm allows
predictor-corrector method to improve the the user to create larger time steps.
accuracy of the ORIGEN depletion calculation.
In Vietnam, combining a Monte Carlo
In 2001, the Massachusetts Institute of
based code with a depletion and decay code to
Technology (MIT) distributed another MCNP-
realize burnup calculations, has received much
ORIGEN combined program, MCODE
attention in recent years. Typically, a REBUS-
(MCNP-ORIGEN DEpletion program) [7],
MCNP linkage system was used for core and
written in ANSI C. In MCODE, there are 39
fuel management of the Dalat Nuclear Research
actinides and 100 fission products considered in
Reactor (DNRR) [11][12]. Moreover, a
the burnup calculations, which account for
depletion calculation code using Radau IIA
more than 99% of neutron absorptions. In 2007,
Implicit Runge Kutta method was developed in
a burnup simulation system was developed at
combination with MCNP5 and named MCDL
CIEMAT (Centro de Investigaciones
(Monte Carlo Depletion for Light Water
Energéticas, Medioambientales y Tecnológicas),
Reactor) to investigate burnup of DNRR [13].
Spain with the name EVOLCODE (Burn-up
However, the study on the combination of
EVOLution Simulation CODE) [8]. In
Monte Carlo code and depletion code for
EVOLCODE, MCNPX was coupled with two
burnup calculation of commercial reactors such
point-depletion codes, ORIGEN and ACAB [9],
as VVER-1000 has not yet been done. For this
to enlarge the number of nuclear reactions taken
reason, the aim of this study is to develop a
into account by the irradiation calculations. In
coupling scheme between MCNP5 and
2013, another MCNP-ORIGEN burnup
ORIGEN2 codes to perform burnup calculation
calculation code system, named MCORE
of VVER-1000 fuel assemblies, in which we
(MCNP and ORIGEN burn-up Evaluation
used the simple approach adopted in MOCUP,
code) [10], was developed at Xi‟an Jiaotong
for the sake of simplicity. To validate the
University, China. In MCORE, besides the
MCNP5-ORIGEN2 coupling program, a
investigation of the reactivity effects and
VVER-1000 LEU benchmark assembly [14]
isotopic inventory as a function of burnup, it is
was calculated and analyzed. The obtained
also capable of simulating the fuel shuffling
calculation results showed a good agreement
process after burnup calculation. In general,
with the benchmark.

17
DEVELOPMENT OF AN MCNP5-ORIGEN2 COUPLING SCHEME FOR …

II. METHODOLOGY removal rate per unit volume of isotope i by


neutron absorption, and i Ni the removal rate
A. Depletion and decay calculation
per unit volume of isotope i by decay.
In a nuclear reactor environment,
formation of new isotopes comes primarily To solve the equation (1) one need to
from fission, neutron capture, and decay. gather information of important parameters such
Likewise, destruction of isotopes also comes as neutron fluxes and cross sections. Such
from these processes. An equation for modeling parameters are in fact not constant over the entire
isotopic depletion is expressed as follows: cycle. That is why the cycle needs to be divided
into a number of small time steps, during which
dN i
   ji f , j N j     c ,k i N k  ... the coefficients such as cross-sections and
dt j k neutron fluxes are assumed to be constant. These
  l i Nl  ( f ,i N i    a ,i N i   i N i )
constant coefficients can be calculated by the
l MCNP5 program for a specified geometry at a
(1) certain time step, and then used in ORIGEN2
calculations to provide the material compositions
where dN i is the rate of change in for the next time step. The calculations are
dt
repeated till the final time step. The coupling
concentration of isotope i, 
j
 f , j N j  the
ji
procedure between the MCNP5 and ORIGEN2
production rate per unit volume of isotope i codes is presented in the next section.
from fission of all fissionable isotopes, B. Description of MCNP5-ORIGEN2 coupler
 c,k i Nk  the production rate per unit
k
The developed MCNP5-ORIGEN2
volume of isotope from neutron transmutation coupler was written in the PERL programming
of all isotopes,  l i Nl the production rate language. The coupler consists of PERL files,
l which can generate the MCNP5 and ORIGEN2
per unit volume of isotope i from decay of all input files, modify and update the cross-section
isotopes,  f ,i Ni  the removal rate per unit library of ORIGEN2 during burnup, and
process the data in the MCNP5 and ORIGEN2
volume of isotope i by fission,  a ,i Ni  the
output files automatically.

Fig. 1. MCNP5-ORIGEN coupling flow diagram

18
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

This coupler provides full capabilities of equation (2) [15] should be used to normalize
the Monte Carlo code MCNP5 and the the F4 flux tally (ΦF4):
versatile nuclides depletion and decay code  neutron 
P W   
ORIGEN2. It makes use of the tally  neutron   fission  1  1 
   F 4  2 
information of MCNP5 to get neutron fluxes  cm s  
2
13 J   MeV  keff  cm 
1.6022 10  wf
and nuclides cross-sections, which are  MeV   fission 

processed to obtain input information of (2)


ORIGEN2 for every active cell. After running where Φ denotes the actual total neutron flux in
ORIGEN2, the coupler exploits the depletion the system.
and decay information from ORIGEN2 output
D. Cross-section calculation
files and provides the material compositions of
all active cells for the next time step. The ORIGEN2, unlike MCNP5, uses one-
coupling procedure is illustrated in Fig. 1. The group cross sections which are averaged for all
normalization of the neutron flux values energies, whereas in MCNP5, cross sections are
obtained by MCNP5 and the generation of the available for all energy points. Therefore one
one-group cross sections for performing can use MCNP5 to generate a mean cross
ORIGEN2 calculations are presented in section for all energies, which can be used in
sections 2.3 and 2.4, respectively. the ORIGEN2 code to update the one-group
cross-section library. Such MCNP5 calculation
C. Neutron flux normalization
can be done by using the F4 and FM4 tallies.
Since all tallies in MCNP5 are The F4 tally gives neutron flux in a cell while
normalized as per fission source neutron, the the FM4 tally can multiply flux by cross
flux values are in units of (number-of- sections in all energy points for each isotope
neutrons)/(fission-source-neutron)/cm2, which and each reaction. Finally, the dividing FM4
needs to be multiplied by a constant factor to value by F4 value can give a one-group cross
convert into (number-of-neutrons)/(cm2.second) section for that isotope and for all important
for using in ORIGEN2. The constant factor can reactions. The Eq. (3) shows how the above
be calculated based on the power of the system. approach will be done.
The system producing power P needs P
  ( E )( E )dE FM 4 (3)
wf
 E

fissions per second, where wf denotes effective  ( E )dE
E
F4
energy released per fission event. Although the
value of wf will vary somewhat with the type of For fission products, only neutron
reactor and the detailed core composition, it is capture cross sections are calculated since their
typically taken by 198 MeV for steady state principal effect is due to neutron absorption.
condition. This fission rate produces P For actinides, four type of cross sections are
wf considered including (n,γ), (n,f), (n,2n), and
(n,3n) reactions because actinides are important
neutrons per second, where  denotes the
in terms of generating fission source neutrons
average number of neutrons released per fission.
and transforming into higher-mass actinides
For subcritical and supercritical systems, one
1
(see Eq.(1)).
should multiply the above result by to
keff Because of the excessive computer time
maintain the critical i.e. steady-state power and the unavailability of many MCNP5 cross-
level system (k = 1). Accordingly, the following sections, only a limited set of libraries of

19
DEVELOPMENT OF AN MCNP5-ORIGEN2 COUPLING SCHEME FOR …

important nuclides, 24 actinides and 61 fission others, data from libraries evaluated at different
products, were updated by using MCNP5 as laboratories are used. Because the MCNP5
shown in Table I. In ORIGEN2 depletion cross section libraries are only available at
calculations, the cross sections, which are not certain temperatures (293, 600, 900, 1200K),
provided by MCNP5, are taken from the libraries of U-235, U-238, Pu-239 were created
ORIGEN2 one-group cross section library from JEFF3.2 at 1027K (the required
PWRU.LIB (PWR library, thermal spectrum) benchmark temperature) by the NJOY99 code
which includes 129 actinides and 879 fission [16] in order to consider the Doppler
products. The cross sections for most of the broadening of resonance cross sections of these
isotopes are obtained from ENDF/B-IV, three important isotopes.
ENDF/B-V, and ENDF/B-VI, while for the
Table I. List of nuclides were updated the one-group cross sections library using MCNP5

U-234, U-235, U-236, U-237, U-238, U-239, Np-236, Np-237,


Np-238, Np-239, Pu-238, Pu-239, Pu-240, Pu-241, Pu-242,
24 Actinides
Pu-243, Am-241, Am-242, Am-243, Cm-242, Cm-243,
Cm-244, Cm-245, Cm-246

Kr-83, Y-89, Zr-91, Zr-92, Zr-93, Zr-94, Zr-96, Mo-95,


Tc-99, Ru-101, Ru-103, Rh-103, Rh-105, Pd-104, Pd-105,
Pd-106, Pd-108, Ag-109, Cd-110, Cd-111, Cd-112, Cd-113,
I-127, I-129, I-135, Xe-130, Xe-131, Xe-132, Xe-134, Xe-135,
61 Fission
Xe-136, Cs-133, Cs-134, Cs-135, Cs-137, Ba-138, Pr-141,
products*
Nd-143, Nd-145, Nd-147, Nd-148, Pm-147, Pm-148, Pm-149,
Sm-147, Sm-149, Sm-150, Sm-151, Sm-152, Eu-151, Eu-152,
Eu-153, Eu-154, Eu-155, Gd-152, Gd-154, Gd-155,
Gd-156, Gd-157, Gd-158, Gd-160

Library in
JEFF3.2 (U-235, U238, Pu-239) (Created by NJOY99)
MCNP5
ENDL92 (Np-236, Np-238)
LANL (U-239)
ENDF/B-IV, ENDF/B-V, ENDF/B-VI (other nuclides)

1027K (U-235, U-238, Pu-239) (Created by NJOY99)


Library's
880.8K (Xe-135)
temperature
293.6K, 300K (other nuclides)

*34 FPs shown in bold characters are important in reactivity prediction [17]. These 34 FPs were used
for criticality calculation in MCNP5.

III. BENCHMARK ANALYSIS and to the Benchmark Mean (BM) values. Each
MCNP5 run was done with 50 millions neutron
The MCNP5-ORIGEN2 coupling histories that lead to a statistical error of about
scheme was validated through predicting the ±10 pcm (±1σ) for k-inf. This section presents
neutronic and isotopic behavior of a VVER- the specification of the VVER-1000 LEU
1000 LEU benchmark assembly [14]. The assembly (section 3.1) and the analysis and
results of coupling calculations were compared discussion about the calculated results (sections
with those of several burnup codes including 3.2-3.4).
MCU, TVS-M, WIMS8A, HELIOS, Multicell

20
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

A. VVER-1000 LEU assembly benchmark composition of fuel pins, cladding and


specification moderator are given in Table II.
The VVER-1000 LEU hexagonal The calculations are performed under hot
assembly consists of one central tube, 18 guide operating poisoned condition, i.e. at Tfuel =
tubes, and 312 fuel pin locations (12 of which 1027K, Tmoderator = 575K with equilibrium 135Xe
are gadolinium rods - UGD). The hexagonal and 149Sm concentrations, a power density of
lattice pitch of the assembly is 23.6 cm. The 108 MWt/m3 up to a burnup of 40 MWd/kgHM.
fuel pins, which are cylindrical and cladded The burnup calculation is realized with 30 steps
with Zirconium alloy have a pitch of 1.275 cm. of 0.5 MWd/kgHM and 10 step of 2.5
The benchmark assembly is shown in Fig. 2 and MWd/kgHM. The Gd rods are divided into 10
consists of fuel rods with 3.7 wt.% enrichment. annuli of equal area in order to account for the
Cell numeration in the 1/6 of the fuel assembly shielding effect due to gadolinium isotopes.
for simulating different isotopic composition is This permits us to easily calculate the nuclides
as shown in Fig. 3.The 12 UGD pins have a concentrations as a function of the radial
235
U enrichment of 3.6 wt.% and a Gd2O3 position (5 regions required in benchmark
content of 4.0 wt.%. Descriptions of material document [14]).

Fig. 2. MCNP5 model of the VVER-1000 LEU benchmark assembly

21
DEVELOPMENT OF AN MCNP5-ORIGEN2 COUPLING SCHEME FOR …

Fig. 3. Cell numeration in the 1/6 of the benchmark assembly

Table II. Material composition of the VVER-1000 LEU benchmark assembly


Material name Comment Isotopic content (atoms/barn-cm)
235 16
UO2 LEU fuel 3.7 w/o enrichment U 8.6264E-4 O 4.6063E-2
238
U 2.2169E-2
UGD LEU fuel of 3.6 w/o of 235U 235
U 7.2875E-4 155
Gd 1.8541E-4
238 156
containing 4 w/o of Gd2O3 U 1.9268E-2 Gd 2.5602E-4
16 157
O 4.1854E-2 Gd 1.9480E-4
152 158
Gd 2.5159E-6 Gd 3.0715E-4
154 160
Gd 2.7303E-5 Gd 2.6706E-4
Cladding Zirconium alloy Zr 4.259E-2 Hf 6.597E-6
Nb 4.225E-4
10
Moderator Light water with 0.6 g/kg of H 4.483E-2 B 4.794E-6
16 11
boron, Tm = 575K, d = 0.7235 O 2.422E-2 B 1.942E-5
g/cm3

B. K-inf versus burnup in beginning burnup steps and then the


difference increases in later ones. The
The infinite multiplication factor (k-inf)
maximum of the deviation with BM values are
of the VVER-1000 LEU Benchmark Assembly
440, 400, 460, 260, 360, 585 pcm for MCU,
was calculated with respect to burnup using
TVS-M, WIMS8A, HELIOS, MULTICELL,
MCNP5-ORIGEN2 coupling scheme and
and MCNP5-ORIGEN2, respectively. As can
compared with those obtained by the
be seen in Figure 4, at the beginning, the
aforementioned burnup codes as shown in Fig.4
reactivity slightly increases with burnup due to
The differences in the k-inf values of these
the use of Gd2O3 in UO2 for core reactivity
codes from benchmark mean values are also
control. As the gadolinium isotopes burn out,
shown separately in Table III.
the reactivity starts to decrease with burnup in a
Table III shows that, the k-inf results roughly linear manner due to the effect of
obtained using MCNP5-ORIGEN2 are in fissile material depletion and neutron-absorber
satisfactory agreement with the results accumulation. It is obviously seen that the
estimated by the rest of burnup codes. The k-inf effect on reactivity of the gadolinium absorber
values between MCNP5-ORIGEN2 coupling is well simulated by the MCNP5-ORIGEN2
scheme and the BM values are slighly different coupling scheme.

22
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

Fig. 4. Variation of k-inf with burnup for VVER-1000 LEU


Benchmark Assembly

Table III. Deviation of k-inf values from benchmark mean values

Deviation from BM Values, pcm


Burnup
(MWd/kgHM) MCNP5-
MCU TVS-M WIMS8A HELIOS MULTICELL
ORIGEN2
0 30 30 -220 50 130 14
1 150 -40 -460 120 210 117
2 -30 -20 -390 200 250 167
3 180 -110 -400 170 160 84
4 40 -80 -320 220 160 111
5 50 -100 -270 220 90 44
6 70 -110 -210 200 30 12
7 140 -100 -210 170 10 -24
8 210 -100 -290 140 40 51
9 -30 -10 -290 180 160 228
10 70 -40 -370 140 180 315
11 -70 0 -350 180 240 432
12 30 -40 -380 160 210 413
13 -60 -20 -360 180 230 485
14 80 -50 -380 160 200 471
15 20 -40 -350 180 210 489
20 -80 -60 -280 240 160 585
25 30 -140 -190 250 50 556
30 140 -240 -80 250 -80 546
35 440 -390 10 200 -280 466
40 260 -400 230 260 -360 493

23
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

C. Isotopic composition versus burnup atoms/barn-cm at the end of cycle) is negligible


in the burnup calculation. The results from
Figs. 5-15 display the MCNP5-
MCORE, an MCNP4C-ORIGEN2.1 coupling
ORIGEN2 calculations for the isotopic
code, developed by Meiyin Zheng et. al. in
composition variation as a function of burnup
2013 [10] showed a better agreement with the
of nuclides 235U, 236U, 238U, 239Pu, 240Pu, 241Pu,
242 BM values. In MCORE‟s results, the deviation
Pu, 135Xe, 149Sm, 155Gd and 157Gd,
from BM value at 40 MWD/kgHM is only -
respectively in cell-1 and cell-24 of the VVER-
2.0% for 157Gd when compare with -15.07% in
1000 LEU benchmark assembly in comparison
this research. One of the reason is MCORE
with the benchmark mean values [14], where
considered 37 actinides and 101 fission
we can see a good agreement. It should be
products in burnup calculations when compare
noted that the deviations obtained from the
with 24 actinides and 61 fission products in this
comparison mentioned above at the end of the
work. In MCORE, the NJOY system code was
burnup (40 MWd/kgHM) are generally within
also used to process the source evaluated
6.5% as shown in Table IV.
nuclear data files into libraries useable for
As can be seen in Figs. 14-15, the MCNP code. Another reason for the more
depletion of the burnable absorbers 155Gd and accurate results in MCORE is that the code
157
Gd is well simulated in the MCNP5- considered (n,γ), (n,2n), (n,α) and (n,p)
ORIGEN2 coupling scheme. The figures show reactions for updating fission product‟s libraries
that 157Gd depletes faster than 155Gd due to its while this study only considered (n,γ). Besides,
higher absorption cross section (155σa = 60,801 MCORE obtained more reliable results due to
barns and 157σa = 253,929 barns at thermal the burnup calculation was realized with 60
neutron 0.0253 eV). Despite the deviation from steps of 0.25 MWD/kgHM and 50 steps of 0.5
BM values of 157Gd isotope in gadolinium MWD/kgHM when compare with only 30 steps
bearing fuel rod exceeds 15%, this percentage of 0.5 MWD/kgHM and 10 steps of 2.5
of the small concentration of 157Gd (1.469E-7 MWD/kgHM in this work.

Fig. 5. 235U isotopic composition as a function of Fig. 6. 236U isotopic composition as a function of
burnup burnup

24
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

Fig. 7. 238U isotopic composition as a function of Fig. 8. 239Pu isotopic composition as a function of
burnup burnup

Fig. 9. 240Pu isotopic composition as a function of Fig. 10. 241Pu isotopic composition as a function of
burnup burnup

Fig. 11. 242Pu isotopic composition as a function of Fig. 12. 135Xe isotopic composition as a function of
burnup burnup

25
DEVELOPMENT OF AN MCNP5-ORIGEN2 COUPLING SCHEME FOR …

Fig. 13. 149Sm isotopic composition as a function of Fig. 14. 155Gd isotopic composition as a function of
burnup burnup

Fig. 15. 157Gd isotopic composition as a function of burnup

Table IV. Isotopic composition error (%) compared to BM values at 40 MWd/kgHM


235 236 238 239 240 241 242 135 149 155 157
Isotope U U U Pu Pu Pu Pu Xe Sm Gd Gd
Cell 1 -4.82 4.99 0.07 -4.69 6.29 3.78 6.20 -1.07 3.52
Cell 24 -3.30 4.89 -0.09 -6.14 3.81 3.18 5.50 -1.45 4.16 -1.42 -15.07

D. Isotopic composition versus fuel volume gadolinium pin radial zones for burnup point 40
radius MWd/kgHM (235U and 239Pu) and for burnup
point 2 MWd/kgHM (155Gd and 157Gd) are
As mentioned in section 3.1, every UGD
presented in Figs. 16-19. The radial
rod has radial sub-divisions (10 rings) in order
distributions of the 235U, 239Pu and 155Gd
to take into account the shielding effect due to
calculated by MCNP5-ORIGEN2 coupling
gadolinium. In this section, the concentration of
scheme showed good agreement with the
some isotopes in 5 zones (each zone consists of
benchmark results. In detail, the deviation
2 rings) of cell 24 (see Fig. 3) were calculated
between MCNP5-ORIGEN2 coupling scheme
and compared with benchmark mean values.
and BM composition for 235U, 239Pu and 155Gd
The isotopic compositions in five fuel-

26
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

in outer zone are only -3.6%, -5.28% and surface of the fuel pellet. Such 239Pu-formation
6.69% as shown in Table V, respectively. The by the neutron resonance absorption is well
157
Gd concentration, however, had a huge known via the so-called “rim effect”. As the
deviation of nearly 50% in the outer zone as burnup increases, the local burnup in the fuel
compared to the BM value. This is due to the close to the surface is largely increased due to
fact that 157Gd has neutron absorption cross- 239
Pu-formation and therefore the “rim effect”
section larger than 155Gd and therefore it burns becomes more predominant at high burnup as
most in the outer zone. Consequently, the can be seen in Fig. 20.
concentration of 157Gd at outer zone is small
Figs. 18-19 show that gadolinium mostly
and leads to a large statistical error.
burns in the outer rings due to the high
One can see from Fig. 17 that the absorption cross section of 155Gd and 157Gd.
gradient in 239Pu concentration falls off nearly Gadolinium burning shifts toward the inner
exponentially within the fuel volume. This is rings with fuel burnup until all gadolinium
due to the spatial resonance self-shielding, there isotopes burn out such as the depletion of 157Gd
are more 238U absorptions in the outer ring. as shown in Fig. 21.
More 239Pu, therefore, is produced towards the

Fig. 16. 235U isotopic composition versus radius Fig. 17. 239Pu isotopic composition versus radius

Fig. 18. 155Gd isotopic composition versus radius Fig. 19. 157Gd isotopic composition versus radius

27
DEVELOPMENT OF AN MCNP5-ORIGEN2 COUPLING SCHEME FOR …

Fig. 20. Depletion of 239Pu as a function of the radial Fig. 21. Depletion of 157Gd as a function of the
position with burnup change radial position with burnup change

Table V. Error (%) of isotopic composition in cell-24 vs radius compared to BM values; Burnup=40
MWd/kgHM for 235U, 239Pu; Burnup=2 MWd/kgHM for 155Gd, 157Gd

Radius, cm 0.173 0.244 0.299 0.345 0.386


Zone 1 2 3 4 5 average
235
U -2.98 -3.20 -3.37 -3.48 -3.60 -3.30
239
Error Pu -6.41 -6.33 -6.57 -7.03 -5.28 -6.21
(%) 155
Gd 0.14 0.32 1.21 4.00 6.69 1.96
157
Gd 0.03 1.11 5.01 18.72 47.79 4.73

Table V shows the relative deviation The calculation results of MCNP5-


from BM values of the isotopic composition in ORIGEN2 coupling scheme were compared
each zone of five annulars of equal area. The with several other burnup codes and benchmark
„average‟ values are the comparison with BM mean values from the benchmark document.
values of the isotopic compositions of the entire The infinite multiplication factor (k∞) and
fuel volume. isotopic compositions of the important isotopes
were compared and analyzed. The deviations
IV. CONCLUSIONS between the obtained results and the BM values
for the k∞ were found within 600 pcm. At the
In this paper, a burnup calculation for the
end of burnup (40 MWd/kgHM) the differences
VVER-1000 LEU benchmark assembly [14]
of isotope compositions were generally within
through an MCNP5-ORIGEN2 coupling code
6.5%. Moreover, the coupling scheme also
has been performed. The coupling code was
reproduced well the isotopic composition
built based on the Monte Carlo neutron
behavior along the radius in the gadolinium
transport code MCNP5 and the versatile point
bearing rods. This allowed us to conclude that
depletion code ORIGEN2. The MCNP5-
the MCNP5-ORIGEN2 coupling scheme
ORIGEN2 coupler can process the output files
developed in this study can be applied for the
of MCNP5 and ORIGEN2 and then construct
burnup calculations of the VVER-1000 reactors.
the input files automatically.

28
NGUYEN HUY HIEP, NGUYEN HUU TIEP, TRAN VIET PHU, NGUYEN TUAN KHAI

However, potential errors can occur [3] X-5 Monte Carlo Team, “MCNP – A General
during the burnup calculation because of N-Particle Transport Code, Version 5”, Los
presence of the improper isotopic composition Alamos National Laboratory, April 2003.
from strong absorbers like 157Gd. Such errors [4] A. G. Croff, “A User‟s Manual for the
ORIGEN2 Computer Code”, Oak Ridge
can be reduced by using smaller time steps or
National Laboratory, July 1980.
integrate a predictor-corrector algorithm into
[5] R.L. Moore, B. G. Schnitzler, C. A. Wemple, R.
the depletion calculation. Furthermore, all cross S. Babcock, D. E. Wessol, “MOCUP: MCNP-
sections of the 1008 isotopes consisting of 129 ORIGEN2 Coupled Utility Program,” INEL-
actinides and 879 fission products should be 95/0523, Idaho National Engineering
updated through burnup time steps in order to Laboratory, September 1995.
avoid error accumulation. To do this, the cross [6] David I. Poston, Holly R. Trellue, “User‟s
section libraries, which are unavailable in Manual, Version 2.0, for Monteburns, Version
MCNP5, should be created by using NJOY 1.0”, LA-UR-99-4999, Los Alamos National
code [16]. Therefore, the future tasks needed Laboratory, September 1999.
[7] Zhiwen Xu, Pavel Hejzlar, Michael J. Driscoll,
are to (1) study the “modified predictor-
and Mujid S. Kazimi, “An improved MCNP-
corrector” method and integrate to the depletion
ORIGEN Depletion Program (MCODE) and its
calculation; (2) update one-group cross section Verification for High-burnup Applications”,
libraries for more actinides and fission PHYSOR, Seoul, Korea, October 2002.
products; and (3) build up an MCNP5- [8] F. Alvarez-Velarde, E. M. Gonzalez-Romero, I.
ORIGEN2 coupling scheme for burnup Merino Rodriguez, “Validation of the Burn-up
calculation of VVER-1000 cores. code EVOLCODE 2.0 with PWR Experimental
Data and with a Sensitivity/Uncertainty
ACKNOWLEDGMENTS Analysis”, Annals of Nuclear Energy, June
2014.
We would like to thank MSc. Tran Quoc [9] Javier Sanz, Oscar Cabellos, Nuria García-
Duong, Dalat Nuclear Research Institute, for Herranz, “ACAB Inventory Code for Nuclear
sharing his experience of using MCNP5 and Application: User‟s Manual version 2008”,
ORIGEN2 codes, and PhD. Pham Nhu Viet Ha December 2008.
for useful comments in improving the quality of [10] Meiyin Zheng, Wenxi Tian, Hongyang Wei,
Dalin Zhang, Yingwi Wu, Suizheng Qiu,
the manuscript. We acknowledge the support
Guanghui Su, “Development of an MCNP-
from Ministry of Science and Technology of
ORIGEN Burn-up Calculation Code System
Vietnam under grant number and its Accuracy Assessment”, Annals of
DTCB.13/15/VKHKTHN. Nuclear Energy, August 2013.
[11] Luong Ba Vien, Le Vinh Vinh, Huynh Ton
REFERENCES Nghiem, Nguyen Kien Cuong, “Design
Analyses for Full Core Conversion of The
[1] Keisuke Okumura, Yasunobu Nagaya,
Dalat Nuclear Research Reactor”, Nuclear
Takamasa Mori, “MVP-BURN: Burn-up
Science and Technology, Vol. 4, No. 1, p. 10-
Calculation Code Using a Continuos-energy
25, March 2014.
Monte Carlo Code MVP”, Japan Atomic
[12] Nguyen Nhi Dien, Luong Ba Vien, Le Vinh
Energy Agency (JAEA), January 2005.
Vinh, Huynh Ton Nghiem, Nguyen Kien
[2] Edward J. Parma, “BURNCAL: A Nuclear
Cuong, “Full Core Conversion and Operational
Reactor Burnup Code Using MCNP Tallies”,
Experience with LEU Fuel of the DALAT
Sandia National Laboratories, November 2002.
Nuclear Research Reactor”, RERTR 2014 –
35th International Meeting on Reduced
Enrichment for Research and Test Reactors,

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IAEA Vienna Interational Center, Vienna, [15] Luka Snoj, Matiaz Ravnik, “Calculation of
Austria, October 2014. Power Density with MCNP in TRIGA reactor”,
[13] Nguyen Kien Cuong, Huynh Ton Nghiem, International Conference, Nuclear Energy for
Vuong Huu Tan, “The Development of New Europe 2006, September 2006.
Depletion Program Coupled with Monte Carlo [16] R. E. MacFarlane, A. C. Kahler, “Methods
Computer Code”, The 11th National Conference for Processing ENDF/B-VII with NJOY”,
on Nuclear Science and Technology, Da Nang, Nuclear Data Sheets, October 2010.
Vietnam, August 2015. [17] Go Chiba, Masashi Tsuji, Tadashi
[14] NEA/NSC/DOC 10, “A VVER-1000 LEU Narabayashi, Yasunori Ohoka & Tadashi Ushio,
and MOX Assembly Computational “Important Fission Product Nuclides
Benchmark”, Nuclear Energy Agency, Identification Method for Simplified Burnup
Organization for Economic Co-operation and Chain Construction”, Journal of Nuclear
Development, 2002. Science and Technology, 2015.

30
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 31-39

Research and design of the moving system


for the cobalt-60 industrial irradiator
Le Minh Tuan, Tran Khac An, Cao Van Chung, Phan Phuoc Thang

Research and Development Center for Radiation Technology


(Received 04 November 2016, accepted 25 November 2016)

Abstract: On the way of localization of Cobalt-60 industrial irradiators, Research and Development
Center for Radiation Technology (VINAGAMMA) has successfully designed and manufactured the
first version of Co-60 industrial irradiator, VINAGA1. The second version of Co-60 industrial
irradiator has been studied and designed by VINAGAMMA in the frame of the scientific project No.
ĐTCB.02/15/TTNCTK. The nucleus of a Co-60 industrial irradiator is a mechanical system inside an
irradiation room namely a tote box moving system. This report presents the tote box moving system
designed by VINAGAMMA. The tote box moving system contains 52 tote boxes with the dimensions
of 50 cm (w) × 70 cm (l) × 150 cm (h) that are moving around the source racks in the manner of 4
passes and 2 levels. The irradiator with this tote box moving system has good specifications: The
minimum time of an irradiation cycle is 1h 20 min. and the dose uniformity ratio (DUR) at the product
densities of 0.1 g/cm3 and 0.5 g/cm3 is 1.4 and 1.8, respectively. Radiation energy utilization efficiency
at the product densities of 0.1 g/cm3 and 0.5 g/cm3 is 19.7% and 48.8%, respectively. These
specifications meet the requirements for a multi-purpose Co-60 industrial irradiator and the present
irradiation requirements in Vietnam.
Keywords: Tote box moving system, irradiator, cobalt-60, density, dose uniformity ratio (DUR).

I. INTRODUCTION the first version of multi-purpose Co-60


industrial irradiator, VINAGA1. This irradiator
The first Cobalt-60 semi-industrial has some advanced features over imported Co-
irradiator in Vietnam has been put into 60 industrial irradiators. VINAGA1 will be
operation in 1991. Nowadays, Vietnam has 9 installed at Da Nang irradiation center of
industrial irradiators: 2 accelerators and 7 Co- Vietnam Atomic Energy Institute (VINATOM).
60 irradiators. These Co-60 industrial
irradiators are supplied by Hungary (5), by the This paper presents the results of
Russia (1) and by China (1) [1]. With the research and design work to manufacture the
development of the national economics, the tote box moving system for the Co-60 industrial
demand of sterilization of medical products and irradiator in the frame of the scientific project
food processing is increased. The localization No. DTCB.02/15/TTNCTK.
of Co-60 industrial irradiator is a market
II. OBJECTIVES AND RESEARCH
requirement for the development of irradiation
METHODOLOGY
processing technology in the country.
In order to develop the applications of A. Objectives
radiation technology in the national economics, The objectives of the research and design
VINAGAMMA has the orientation of design of the tote box moving system for the multi-
and manufacture of multi-purpose cobalt-60 purpose Co-60 industrial irradiator are:
industrial irradiators. In this development way,
VINAGAMMA has designed and constructed

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
RESEARCH AND DESIGN OF THE MOVING SYSTEM FOR …

- The moving system should be able to one could made design drawings, part modeling
work with high source activity, namely more and assembly modeling as well.
than 800 kCi in the aspect of food irradiation.
This activity is required for meeting irradiation III. RESULTS AND DISCUSSION
demands at present and in future as well as
A. Preliminary design
economical ones.
Upon the knowledge and results gained
- The system should have high radiation
from the design and construction of the tote box
energy utilization efficiency, good dose
moving system VINAGA1 and IAEA
uniformity in products. For multi-purpose Co-
documents for the Co-60 industrial irradiator [1,
60 industrial irradiators, values of DUR for
4, 5, 6], the tote box moving system for the Co-
medical products with low density and for food
60 industrial irradiator could have the following
with high density should be in the acceptable
features of preliminary design:
ranges.
- Tote boxes of the system will have the
- The system is safe, easy operation and
width less than 60 cm. In order to get more
maintenance and can be upgraded if needed.
processing rate than the VINAGA1, the height
B. Research methodology of a tote box is selected about 3 times of the
For research and design of the tote box source rod length and the box length should be
moving system the following methods have increased. For that height of a tote box, the
been applied: source rack will be about 1.5 m.

- By using MCNP code version 4C [2], - The system will have four passes, two
the dose distributions inside a tote box have levels.
been determined for various product densities - The system contains 52 boxes with the
namely from 0.1 to 0.6 g/cm3. Based on the disposition of 4 boxes at temporary places (at the
calculation results such as DUR, irradiation border of the system) and 48 boxes in 8 rows.
efficiency the selection of the tote box sizes has
- The system is suitable for the densities
been made. The selected dimensions of a tote
of medical products with the density range of
box could give the irradiator high efficiency
0.1 g/cm3 ÷ 0.2 g/cm3 and food with the density
and accepted DUR value.
range of 0.5 ÷ 0.6 g/cm3.
- By using some calculation tools in the
- The system can be operated in three
mechanical design the structure of the tote box
main irradiation modes: Continuous irradiation,
moving system, the structure of a tote box has
batch irradiation and stationary irradiation.
been designed. The following mechanical data
for the system should be calculated: Maximum The continuous mode is often used for
load capacity of a tote box is 220 kg, the irradiation of a big volume of product with the
maximum load capacity of the moving system same density and used for irradiation of
is 13,000 kg and static load of bearing 6004zz required low doses like foods. The batch mode
is 500kg, etc. The Autodesk Inventor 2014, the is often used for irradiation of product with the
3D CAD software [3] has been used as the main same density and often used for irradiation of
tool for calculation of some main data in high doses like medical products. The
mechanical design such as deformation, stress, stationary irradiation is only used when an
displacement, safety factor of the frame of the irradiation with long dwell time is interrupted
tote box moving system. By using the software by some technical reasons.

32
LE MINH TUAN, TRAN KHAC AN, CAO VAN CHUNG, PHAN PHUOC THANG

In the continuous mode, the system the last dwell time was not completed due to
receives one new tote box brought by the irradiation interruption.
transport system from the loading-unloading
Tote boxes are brought in or out of the
area and delivers one irradiated tote box which
tote box moving system by a car of the
has been went through 52 positions in the
transport system.
system. In the batch mode, 52 tote boxes in the
system move defined steps and no tote box The principle diagram of the tote box
either goes in or goes out; in the stationary moving system is illustrated in Fig. 1.
mode, 52 boxes stay for compensating time that

Fig. 1: Principle diagram of the tote box moving system

The moving manner of tote boxes can be to prevent a box moving over right in the lift
explained by the lines with arrow in the above C10 when C1 pushes boxes in the first row one
pictures. Cylinder C1, C3, C11, C13 are used step right [7].
for pushing tote boxes in the row 1, row 3 of
In order to increase the processing rate of
the lower level and the row 2, the row 4 of the
the irradiator using the tote box moving system,
upper level one step right; Cylinder C2, C4,
it is predetermined that the height of a tote box
C12, C14 are used for pushing tote boxes in the
is 150 cm with the useful height of 140 cm, the
row 2, row 4 of the lower level and the row 1,
length of a tote box is 70 cm with the useful
the row 3 of the upper level one step left; Two
length of 66 cm and the width of a tote box
lift mechanisms with C10 and C17 are used
should be chosen among three assuming values,
change a box between two levels; C5, C15, C6,
namely 45, 50 and 55 cm with the useful widths
C16 are used to change a box between rows; C8
of 41, 46 and 51 cm, respectively.
is used for unlock a box on the car; C9 is used

33
RESEARCH AND DESIGN OF THE MOVING SYSTEM FOR …

B. Calculation of physical parameters of the point. Fig. 2 presents the dose calculation points
tote box moving system inside a tote box.
For a multi-purpose Co-60 industrial
irradiator two main physical parameters should
be determined, namely dose uniformity ratio
(DUR) and radiation energy utilization
efficiency (hereinafter called efficiency) for
various densities of product.
These parameters can be calculated if
dose mapping data for various densities of
product are known. The dose mapping data
inside a tote box can be known by experimental
measurement or by theoretical calculation. In
our case the calculation is carried out by using
MCNP code version 4C [2].
Absorbed doses of 63 cells of MCNP
code inside a tote box with different dimensions
and different densities of product have been
calculated. There are three cases of tote box Fig. 2: Dose calculation points inside a tote box
dimensions, namely (45 cm × 70 cm × 150 cm)
(Case 1), (50 cm × 70 cm × 150 cm) (Case 2), The calculated minimum and maximum
(55 cm × 70 cm × 150 cm) (Case 3). The absorbed doses for 6 different densities of
densities of product loaded in tote boxes are products with calculation error about 2% and
0.1, 0.2, 0.3, 0.4, 0.5 and 0.6 g/cm3. for 3 cases of the tote box dimensions are given
in Table I.
Dose calculations are carried out for the
source activity of 800 kCi. It takes 1 hour of
computer running time for dose calculation of a

Table I. Calculation results of minimum and maximum absorbed doses with different densities of product
Density
0.1 0.2 0.3 0.4 0.5 0.6
(g/cm3)
Unit: kGy Dmax Dmin Dmax Dmin Dmax Dmin Dmax Dmin Dmax Dmin Dmax Dmin

Case 1 5.53 3.99 4.88 3.38 4.34 2.86 3.90 2.41 3.58 2.09 3.32 1.83
Case 2 5.33 3.82 4.67 3.14 4.15 2.66 3.73 2.23 3.42 1.89 3.16 1.64
Case 3 5.15 3.58 4.49 2.94 3.98 2.42 3.56 2.02 3.27 1.70 3.03 1.45

Table II. The calculation results of DUR values with different densities of product

Density (g/cm3) 0.1 0.2 0.3 0.4 0.5 0.6


Case 1 1.38 1.44 1.52 1.62 1.72 1.81
Case 2 1.40 1.49 1.56 1.67 1.81 1.93
Case 3 1.44 1.52 1.64 1.76 1.92 2.09

34
LE MINH TUAN, TRAN KHAC AN, CAO VAN CHUNG, PHAN PHUOC THANG

Table III. The calculation results of efficiency values with different densities of product

Density (g/cm3) 0.1 0.2 0.3 0.4 0.5 0.6


Case 1 18.4% 31.1% 39.5% 44.5% 48.1% 50.5%
Case 2 19.7% 32.4% 41.2% 46.1% 48.8% 50.8%
Case 3 20.5% 33.7% 41.6% 46.2% 48.7% 49.9%

The calculation results of DUR and C. Mechanical design


efficiencies (E) are presented in Table II and
The tote box moving system consists of the
Table III.
following parts: structural frame, guiding structure
Based on the calculation results the for box move, lift mechanisms for changing boxes
following conclusions can be drawn: between levels, row-row changing mechanisms for
changing boxes between rows.
- In the central lines of two box sides
faced to the source there are two locations of The tote box and the system are
maximum dose value. Two locations are illustrated in Fig. 3 and Fig. 4.
about at the distance one fourth of the box
height from the top and the bottom and
symmetrical through the central point in
height of the box.
- The positions of minimum dose value
are often located at two ends of the central
lines of two box sides perpendicular to the
source.
- For a multi-purpose Co-60 industrial
irradiator, the tote box dimensions of 50 cm ×
70 cm × 150 cm is selected upon the
compromise between the DUR and efficiency
values [4].
Fig. 3. A tote box of the moving system

Fig. 4. The tote box moving system

35
RESEARCH AND DESIGN OF THE MOVING SYSTEM FOR …

A tote box consists of a base, a 12,000 kg (48 × 250 kg) and the total weight of
rectangular frame, box covers and 4 bearings. 4 temporary positions is 1,000 kg (4 × 250 kg).
The box base is made of 304 stainless steel, Therefore, the total load of the tote box moving
rectangular frame is made of box stainless steel system is 13,000 kg.
with the sizes of 50 cm (w) × 70 cm (l) × 150
By using the Stress Analysis function in
cm (h), the box covers are made of aluminum
environment of Inventor software [3] three
plate with the thickness of 2 mm, 4 couples of
main parameters of the tote box moving system
bearing 6004ZZ. The tote box has been
namely stress, displacement and safety factor
designed to carry products with the maximum
have been calculated. The forces applied on the
weight of 220 kg.
frame are F1, F2 and F3 with the values of
The tote box moving system is made of 120,000 N (12,000 kg × 10 m/s2), 5,000 N and
CT3 steel. The structural frame is also made of 5,000 N (2 × 250 kg × 10 m/s2), respectively.
CT3 (σbk = 345 MPa) [8], box steel with a Illustrations of stress and displacement
length of 6 m, a width of 2.692 m and a height calculations are given in Fig. 5 and Fig. 6 and
of 3.510 m. The lift mechanisms consist of a the calculation results are given in Table IV.
box container, guiding part for a box and 12 Table IV. Result of stress calculation
bearings 6004ZZ. The row-row changing
Name Steel
mechanisms are located at two outside parts of
the system. Mass density 7.85 g/cm3
General Yield strength 207 MPa
The system contains 48 boxes in 8 rows
Ultimate tensile strength 345 MPa
and 4 boxes at temporary places. The tote box
Young’s modulus 210 GPa
carries products with the maximum weight of
Stress Poisson’s ratio 0.3 ul
220 kg (net weight of a box is 30 kg). The total
weight of 48 boxes with the maximum load is Shear modulus 80.7692 GPa

Fig. 5. Von Mises Stress of the frame

36
LE MINH TUAN, TRAN KHAC AN, CAO VAN CHUNG, PHAN PHUOC THANG

Fig. 6. Displacement of the frame

Based on the above calculated results, the The specifications of the cylinders used
safety factor can be calculated by the equation in the system are given in Table V and the main
as This result mechanical data of the system are given in
Table VI.
comfirms the designed tote box moving system
meets the required safety factor according to
standard safety factor of 1.5 [8].
Table V. Specifications of cylinders used in the tote box moving system
No. Cylinder name Quantity Specifications
167/Ø100/715
1 C1 1
Cylinder with magnetic piston
C2, C3, C4 167/Ø100/810
2 7
C11, C12, C13, C14 Cylinder with magnetic piston
167/Ø100/110
3 C9 1
Cylinder with magnetic piston
167/Ø50/600
4 C5, C15 2
Cylinder with magnetic piston
167/ Ø50/680
5 C6, C16 2
Cylinder with magnetic piston
167/Ø125/1510
6 C10, C17 2
Cylinder with magnetic piston

37
RESEARCH AND DESIGN OF THE MOVING SYSTEM FOR …

167/Ø50/100
7 C7 2
Cylinder with magnetic piston
2700-5 Ø40/25
8 C8 2
Cylinder with magnetic piston

Table VI. Main mechanical data of the tote box moving system

Specifications Weight /unit Total weight


No. Unit Qty.
(mm) (kg) (kg)

Box steel 5 mm
1 piece 28 79.1 2,215
60 (w) × 120 (h) × 6,000 (l)
Box steel 3 mm
2 piece 8 26.2 210
50 (w) × 50 (h) × 6,000 (l)
Box steel 3 mm
3 piece 4 20.6 82
40 (w) × 40 (h) × 6,000 (l)
Box steel 2 mm
4 piece 8 8.5 68
25 (w) × 25 (h) × 6,000 (l)
Box steel 2 mm
5 piece 4 21.7 87
40 (w) × 80 (h) × 6,000 (l)
U steel 3 mm
6 piece 26 14.13 367
25 (h) × 50 (w) × 25 (h) × 6,000 (l)
U steel 3 mm
7 piece 8 7.07 57
25 (h) × 50 (w) x 25 (h) × 3,000 (l)
U steel 3 mm
8 piece 4 14.13 57
40 (h) × 80 (w) × 40 (h) × 3,000 (l)
9 Accessories part set 1 200
Total 3,342

The tote box moving system with 52 tote products and food irradiation. This tote box
boxes having dimensions of 50 cm × 70 cm × moving system version is timely for the present
150 cm has been designed for the multi-purpose irradiation demands. Table VII presents the
Co-60 industrial irradiator. Its specifications are parameters of the tote box moving system.
suitable for both sterilization of medical
Table VII. Parameters of the tote box moving system
No. Parameters Value
1 Tote box quantity 52
2 Tote box sizes 50 cm × 70 cm × 150 cm
3 Useful box sizes 46 cm × 66 cm × 140 cm
4 DUR at the densities of
- 0.1 g/cm3 1.4
- 0.5 g/cm3 1.8
5 Radiation energy utilization efficiency at the density of
- 0.1 g/cm3 19.7%
- 0.5 g/cm3 48.8%

38
LE MINH TUAN, TRAN KHAC AN, CAO VAN CHUNG, PHAN PHUOC THANG

6 Minimum time of an irradiation cycle, min. 80


7 Maximum Co-60 activity could be used for food 1,000
irradiation with the minimum absorbed dose of 3.2kGy,
kCi
8 Maximum throughput of food irradiation with the density 0.83
of 0.5 g/cm3 and the required minimum absorbed dose of
3.2 kGy, tons.(h.100 kCi)-1

IV. CONCLUSIONS [2] J.F. Briesmeister, MCNP- A General Monte


Carlo N-Particle Transport Code, LA 1265-M,
The second version of tote box moving
Version 4C Los Alamos National Laboratory,
system for the Co-60 industrial irradiator has been
Los Alamos, 2000.
designed. The tote box moving systems has high
performances for multi-purpose utilization [3] Nguyen Huu Loc, Manual of Autodesk
Inventor, Ho Chi Minh City Publisher, 2008.
namely for food irradiation and radiation
sterilization of medical products in comparison [4] Radiation safety of Gamma and Electron
with VINAGA1. In addition, the second version Irradiation facilities, IAEA, Safety series No.
of tote box moving systems favorably meets the 107, 1992.
requirements for a multi-purpose Co-60 industrial [5] Safe design and use of Panoramic, wet source
irradiator and the present irradiation requirements storage gamma irradiators (Category IV),
in Vietnam. Based on pre-estimated price, the American National Standard N43.10, July
designed tote box moving system was lower price 1984.
compared to imported one with the equivalent [6] Gamma Irradiators for Radiation Processing,
irradiation capacity. IAEA, Vienna, Austria, 2005.
[7] Operation and Maintenance Manual for SVST-
REFERENCES
Co60/B type irradiator, Institute of Isotopes Co.
[1] Le Minh Tuan, et al, Summary report of the Ltd., 2nd Edition, Vol. 1, 2, 3, May 1999.
scientific project of Ministry of Industry and [8] Nguyen Thi Yen, Lectures on mechanical
Trade, “Research, design and pilot manufacture materials, Hanoi Publisher, 2005.
of the moving system for a Co-60 industrial
irradiator”, Code 04/HĐ-ĐT 2010, 2013.

39
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 40-47

UV light induced DNA damages and the radiation protection


effects of Lingzi mushrom extract
Vo Thi Thuong Lan1, Dinh Ba Tuan1, Ta Bich Thuan1, Tran Bang Diep2, Tran Minh Quynh2*
1
Hanoi University of Sciences, Vietnam Natural University, 334 Nguyen Trai, Thanh Xuan, Ha Noi
2
Hanoi Irradiation Center, Vietnam Atomic Energy Institute, km12, Road 32, Minh Khai, Tu Liem, Hanoi
*Email: tmqthuquynh@yahoo.com
(Received 26 July 2016, accepted 20 September 2016)

Abstract: UV light has strongly influenced on the growth of E. coli as well as caused DNA damages.
Configurations of both genomic DNA and pUC 19 plasmids extracted from E. coli were significantly
changed by the exposure to UV light of 254 nm and DLT, an extract of Ganoderma lucidum Lingzi
mushroom. The results also revealed the radio-protective effects of DLT to UV radiation. By adding
2% DLT to its culturing suspension, the growth of E. coli was significantly decreased, whereas a low
DLT amount of about 0.5% slightly improved its growth, indicated that the DLT extract can be used
as a promising protective substance against UV radiation. At the molecular level, the radio-protective
effects of DLT were observed for both UV treated DNA and protein. Thus, DLT can protect DNA in
vivo, but not in vitro. This effect was also observed for Taq polymerase, suggested that the radio-
protection effect of DLT may due to it accelerated the degradation of radicals or species that produced
in the suspensions during UV exposure.
Keywords: UV radiation, DNA damage, plant extract, radio-protection.

I. INTRODUCTION mutations can also lead to serious diseases, and


even cause cancers [3].
UV radiation (UVR) can attack various
targets in the cell. It produces unexpected
photochemical reactions that are severely
damaging for the DNA, proteins and other bio-
macromolecules, resulting in cellular
dysfunction or even death [1]. It can also
produce free radicals, which act as mutagen or
carcinogenic agents. Fortunately, various living
organisms and even the cells possess their own
Fig. 1. Spatial configuration of pUC19 DNA
defense systems against radiation that can fix
plasmids: supercoil (SX), circular (V) and linear (T)
those lesions. In addition, there are many natural DNA produced by UV radiation as mentioned in the
products with protective properties that can be previous study [4]
used as the radio-protectors.
Analysis of UVR induced DNA
Within a DNA molecule, the pyrimidine damages at the molecular level has been
nucleotides (thymine and cytosine) can link proved as an important method to determine
together in order to form nucleotide complexes the relationship between UV radiation doses
(dimers) by the exposure to UVR. These and lesions including the changes in the DNA
changes prevent the normal transcription and spatial configuration (Figure 1), as well as the
replication of the DNA. The UVR induced damages (single strand, double strand breaks

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
VO THI THUONG LAN et al.

and dimerization) [5]. Investigation of the hot water followed by precipitation with
radiation damages at the molecular level for ethanol was kindly supplied by Hanoi
specific cells and tissues at various University of Pharmacy. Its influences on the
development and differentiation stages is growth of E. coli, as well as radiation
essensial to determine the proper radiation dose protective effects against UV radiation on the
in mutation breeding. Recently, this method DNA and protein were investigated.
has been applied to create and select new
plants (cereals, legumes, fruits and flowers) II. EXPERIMENTAL
with the desired traits in Vietnam [6-8].
Materials
It has been found that many natural
E. coli carrying pUC19 recombinant
products and compounds reveal their potential
vectors, as well as DLT extract from
protective effects not only to radiation induced
Ganoderma lucidum mushroom was prepared
diseases, but also to several types of cancers by
by the Laboratory for Medical Biology,
shielding genetic materials, activating cellular
Faculty of Biology, VNU University of
repair mechanisms or scavenging free radicals
Sciences, Hanoi.
that are strong oxidants for the DNA, proteins
and other biological molecules [9, 10]. E. coli was cultured in Luria - Bertani
(LB) liquid medium, supplemented with or
In our previous study, the protective
without DLT as described in the previous
effect of the extract from Ganoderma lucidum
study, until the optical density at 600 nm
mushroom against UVR has been proved by
reached 0.4
the reduction of the damages for the DNA
exposure to UV [4]. The study on the Vietnam Plasmid and genomic DNAs were
ginseng, Tran et al. found that saponin isolated by using QIA prep Spin Miniprep and
extracted from the Vietnamese ginseng can WizardSV Genomic DNA Purification,
protect the liver cells against damages [11]. respectively. EcoRI was purchased from New
England BioLab (NEB).
The extracts of red ginseng can also
improve the anti-tumor activity of 5- Cell density and DNA concentration
fluorouracil, a popular anti-cancer drug [12]. measurements
Recently, the radio-protective effects of the The same volume of E. coli was
extract of Crinium latifolium leave have been transferred and cultured in the LB liquid medium
confirmed, this extract inhibited proliferation with or without supplement of DLT extract to
of tumor cells [13]. It is obviously that many determine the effect of DLT on bacteria growth.
plant extracts have anti-oxidant properties, The cell density of E. coli suspension was
which are able to scavenge several free radicals determined by the interval measurement of its
and species that may be associated to UV- optical density at 600 nm (OD600). One ml of cell
oxidative stress [9]. The understanding of their suspension was taken and its OD600 was
protection mechanisms is very useful for measured by a UV-vis spectrophotometer (UV-
formulating new safety and effective radio- 2450, Shimadzu, Japan).
protective drugs.
The optical density of DNA solution was
In this study, the extract (abbreviated as measured at 260 nm (OD260), and the
DLT) obtained from Ganoderma lucidum concentrations of both genomic and plasmid
Lingzhi mushroom by normal extraction with DNAs were calculated as follows:

41
UV LIGHT INDUCED DNA DAMAGES AND THE RADIATION PROTECTION EFFECTS OF …

[DNA] = OD260 × n × 50 (g/ml) (1) Aqueous solutions of the DNA in distilled water
and DLT were also exposed to UV for
where OD260 = 1 corresponding to the DNA
analyzing its UV induced damages and the
amount of 50 g/ml in a test sample, and n is
protective effects of DLT for the DNA.
dilution factor.
Estimation of DNA damage
UV radiation treatment
The electrophoresis results have been
The genomic DNA is very sensitive to
used to analyze the size of the DNA fragments
UV light in replication during the logarithmic
and the DNA damages as mentioned in our
phase in the bacteria growth, where the OD600 is
previous study [4]. Briefly, the agarose gel
about 0.3 to 0.6 [14]. E. coli cultured in the LB
electrophoresis was prepared; then, the DNA
with or without the supplement of DLT (0.5%)
samples were loaded in the agarose wells. The
were transferred to a petri dish and then the dish
DNA fragments are visualized by staining with
was exposed to UV radiation at 254 nm using
ethidium bromide, and they are taken by a
BIO-LINK crosslinker (BLX 254, USA) within
specific camera. Be aware that the DNA will
different periods to receive the corresponding
diffuse within the gel over time, and that the
doses of 0.5; 2.5; and 5 J/cm2. The study on the
photography should be taken just after the
UV effect to the DNA in vitro, pUC19 plasmids
cessation of electrophoresis [15].
were isolated, purified and used as targets.
Table I. Primer sequences used for RAPD-PCR

Primer Sequences (5’ - 3’) Primer Sequence (5’ - 3’)


OPL1 AAGAGCCCGT AD2 GCAAGTAGCT
OPL12 GGGCGGTACT AD3 TCACGATGCA
OPK19 CACAGGCGGA B1 CCCAGCTGTG
OLG2 GGACCACTAC B21 AAGCCTCGTC
S216 TTAGCAATTG OPA10 GTGATCGCAG
S256 ATCCGCGTGT OP15 CCTGGGTTCC
S285 TGGACACTGA OPK8 GCCAACGAGA

Unlike the traditional PCR, the RAPD- Enzyme activity measurement


PCR requires random primers, but not any
The protease activity is its capacity to
specific DNA sequences [5]. By the RAPD-
break peptide bonds. In this experiment, the
PCR method, the genetic similarity of the
protease activity was determined as its
genome can be estimated from the patterns of
casein digestion and the liberation of amino
DNA segments, which were amplified with the
acids and soluble peptide fragments. This
short primers (10 nucleotides) using Taq
was measured by the size of the hydrolysis
polymerase. In the present experiment, the
zone produced by protease on the casein
primers amplified the DNA templates from
agar plate [16].
unirradiated and UV irradiated bacteria in the
RAPD-PCR to estimate DNA damages, are
listed in Table I.

42
VO THI THUONG LAN et al.

III. RESULTS AND DISCUSSION 2% DLT. This may be due to the effects of
different bioactive substances which are
Effect of DLT on the growth of E. coli present in DLT extract and their high
concentration may inhibit the bacteria growth.
Therefore, the DLT concentration of 0.5% was
selected to investigate its radio-protective
effects on UV exposed DNA.
Effect of DLT on growth and DNA demages
of the UV irradiated E. coli
It is clear that UVR has much influenced
the bacteria growth. Number of the irradiated
cells seems to be reduced and leveled off after
90 minutes of culturing, while this value
Fig. 2 Growth of E. coli in the media supplemented
rapidly increased for the unirradiated ones. By
with DLT was determined by the OD600
adding DLT, the irradiated cell density was
E. coli was cultured in the LB medium increased after 60 minutes and their OD600
supplemented with various concentrations of value was nearly doubled after 90 minutes. The
DLT and the optical density of cultural results also again indicated that DLT did not
solution was measured at the wavelength of affect to the growth of unirradiated bacteria,
600 nm (OD600) as a function of time intervals though the growth of the UV exposed bacteria
(see Fig. 2). At low DLT concentration of was recovered by adding this DLT (see Fig. 3).
0.5%, the bacteria growth rate was However, its adding points (initial and just
significantly increased with a higher value of before UV radiation) seem not to influence the
OD600, especially for culturing time more than growth of the irradiated bacteria, namely DLT
90 minutes. did not protect the bacteria with the absorption
However, its growth was inhibited by of UV energy, but the radio-protective effects
the presence of DLT at higher concentrations. may be obtained by its stimulation for the
The most obvious reduction was observed for repair mechanism in the cell or the degradation
E. coli culturing in the LB medium containing of radicals or species produced by UVR.

Fig. 3 The effect of 0.5% DLT on the recovery of the UV exposed E. coli. Bacteria at OD600 = 0.4 was
exposed to the UV of 0.5 J/cm2.
(): E. coli incubated in the LB media as the negative control; (): DLT was added in the medium before culturing as
the positive control; (): UV exposed bacteria without DLT; (): DLT was added immediately before and () at the
beginning of the incubation and exposed to UVR when the OD reached 0.4. Error bars show SD

43
UV LIGHT INDUCED DNA DAMAGES AND THE RADIATION PROTECTION EFFECTS OF …

Fig. 4 Electrophoresis results of pUC19 plasmid DNA extracted from E. coli just after exposure to UV (-):
culture and UV treated in LB. DLT: cultured and UV treated in LB supplemented with 0.5% DLT; M -
marker 1kb. (Red arrow: DNA band representative for supercoil forms)

The plasmid DNA isolated from bacteria or without 0.5 % DLT and reached OD600 of
is mainly in supercoil with small amount of 0.4. The same concentration of pUC19 that was
circular forms. By UV treatment, the number of diluted in either water (H2O) or 0.5% DLT was
the circular DNA increased due to increasing of irradiated by various doses of UVR. The
the single stranded breaks, and the double plasmid digested by the EcoRI restriction
stranded breaks leading to the formation of enzyme to obtain the linear form was used as
linear DNA fragments. These DNA the control. There are significant differences
configurations can be recognized and between the DNA irradiated in pure water and
discriminated by electrophoresis (see Fig. 4). DLT solution as shown in Fig. 5. The changes
Therefore, changes in the plasmid DNA from supercoil to circular forms were observed
configuration reveal the DNA damages induced in DLT diluted pUC19. Both of these forms of
by UV treatment. The plasmid DNAs could be pUC19 diluted in H2O were decreased,
extracted from UV exposed bacteria, or from the suggesting that the DNA was fragmented more
bacteria, and subsequently exposed to UV. than that diluted in DLT. Thus, DLT did protect
On the other hand, the alteration of the DNA in vitro against UV as it the shows radio-
genomic DNA caused by UV irradiation was protective effect on the DNA in vivo.
evaluated by the RAPD-PCR using random
primers. If there are differences in the genomic
DNA, namely chromosomal alteration has
occurred in the template DNA at the site that was
previously complementary to the primer, a PCR
product will not be produced, resulting in a
different pattern of the amplified DNA fragments
on the gel. Therefore, different sizes in the DNA
Fig. 5 Electrophoresis results of pUC 19 DNA
fragments yielded in RAPD-PCR reveal the plasmids dispensed in pure water (H2O) and 0.5%
changes in the bacterial DNA. DLT aqueous (DLT) treated by UV of dose from 1
to 4 J/cm2. P and Pcut: PUC19 uncut and cut by
The pUC19 plasmid was also isolated
EcoRI. M: DNA ladder 1 kb
from bacteria cultured in the LB medium with

44
VO THI THUONG LAN et al.

Effect of DLT on the activity of UV treated was exposed to UVR in the presence or
enzymes absence of DLT, and Taq polymerase
activity was investigated by amount of PCR
To study the UV protective effect of
products.
DLT on protein, commercial Taq polymerase

Fig. 6. Electrophoresis results of RAPD-PCR products obtained with random primers. DNA patterns
amplified from 20 ng of the genomic DNA that was isolated either from non-irradiated E. coli cultured
without (LB) and with 0.5 % DLT (DLT) or from 0.5 mJ/cm 2 of irradiated E. coli cultured with DLT
(DLT+UV) and without DLT (UV). M: DNA ladder 1kb

After UV treatment in 1XTaq buffer buffer solution become smaller and disappear
supplemented with or without 0.25 % DLT, by increasing of the UV dose, but the band still
Taq polymerase was amplified using 1 ng of observed for one irradiated in buffer solution
the DNA plasmid as the template. supplemented with DLT. These results proved
Electrophoresis image of the PCR products that DLT has a protective effect for Taq
was presented in Fig. 7. It can be seen that the polymerase and this property may be due to the
DNA band of the sample irradiated in the Taq degradation of free radicals and DLT.

Fig. 7 PCR products amplified from 1 ng DNA plasmid by using Taq polymerase that was dispensed in Taq
buffer without (B) or with 0.25 % DLT (B+DLT) and irradiated by UVR.
M: DNA ladder 1 kb

45
UV LIGHT INDUCED DNA DAMAGES AND THE RADIATION PROTECTION EFFECTS OF …

IV. CONCLUSIONS [5]. RP. Sinha, DP. Häder. UV-induced DNA


damage and repair: a review, Photochem.
The genomic DNA and pUC19 plasmid Photobiol. Sci, 1, 225-36, 2002.
of E. coli were injured by UV exposure at [6]. LD. Thao, NV. Dung, NT. Tham. Study on
some extent. The plant extract, DLT, does not chrysanthemum breeding by gamma (Co-60)
irradiation on callus of 4 exotic varieties,
affect to the growth of E. coli. In contrast, DLT
Journal of Agricultural Technology, 11(8),
shows positive effects against UV radiation. 1813-1822, 2015.
Bacterial growth was recovered by adding of [7]. VTM. Tuyen, NT. Hong, PQ. My, NT. Hue,
0.5% DLT to the cell suspension, and there are LH. Ham. Application of gamma rays
no differences in the recovery capacity among irradiation and marker assisted selection for
improving of bacterial leaf blight resistant rice
the bacteria that were cultured in the LB
variety BT62.1, Journal of Agricultural
medium containing DLT and in LB medium,
Technology, 11(8), 2441-2449, 2015.
which added DLT just before UV treatment. [8]. PTA. Duong, VTT. Lan. Evaluating genetic
These radio-protective effects of DLT were polymorphism of some plant species collected
also recognized for the DNA and protein. DLT from Ma Da area and Cat Tien National Park
revealed its protective effect to the DNA in by using RAPD markers, VNU Journal of
Science, Natural Sciences and Technology, 26
vivo and in vitro. The radio-protective effect of
(1S), 8-12, 2010.
DLT was also observed for Taq polymerase. [9]. CW. Choi, SC. Kim, SS. Hwang, BK. Choi,
Thus, the plant extract DLT can be used as the HJ. Ahn, MY. Lee, SH. Park, SK. Kim.
radio-protector for the DNA and protein, and Antioxidant activity and free radical
its protective effect may be due to its scavenging capacity between Korean
scavenging of radicals and species which are medicinal plants and flavonoids by assay-
guided comparison, Plant Science, 163, 1161-
produced during UV exposure.
1168, 2002.
[10]. AB. Fishbein et al. Asian ginseng enhances the
REFERENCES anti-proliferative effect of 5-fluorouracil on
human colorectal cancer: comparison between
[1]. RP. Rastogi, A. Kumar, MB. Tyagi, RP. Sinha.
white and red ginseng, Archives of Pharmacal
Molecular Mechanisms of Ultraviolet
Research, vol. 32, no. 4, pp. 505–513, 2009.
Radiation-Induced DNA damage and repair,
[11]. LQ. Tran, I. Adnyana, Y. Tezuka, T. Nagaoka,
Journal of Nucleic Acids, 10, 1-21, 2010.
Q. Tran, S. Kadota. Triterpene saponins from
[2]. PM. Girard, S. Francesconi, M. Pozzebon, D.
Vietnamese ginseng (Panax vietnamensis) and
Graindorge, P. Rochette, R. Drouin, E. Sage.
their hepatocytoprotective activity, J. Nat.
UVA-induced damage to DNA and proteins:
Prod., 64, 456–461, 2001.
direct versus indirect photochemical processes,
[12]. KC. Kim, IG. Kim. Ganoderma lucidum
Journal of Physics: Conference Series, 261,
extract protects DNA from strand breakage
2011.
caused by hydroxyl radical and UV irradiation,
[3]. GP. Pfeifer, YH. You, A. Besaratinia.
International Journal of Molecular Medicine,
Mutations induced by ultraviolet light, Mutant
4, 273-80, 1999.
Res, 571, 19-31, 2005.
[13]. M. Jenny, A. Wondrak, E. Zvetkova, NTN.
[4]. DH. Van, TM. Quynh, NT. Thom, DB. Tuan,
Tram, PT. Phi Phi, H. Schennach, Z. Culig, F.
TT. Anh, NT. Ngan, TB. Thuan, VTT. Lan.
Ueberall, D. Fuchs. Crinum Latifolium Leave
Study on DNA damages induced by UV
Extracts Suppress Immune Activation
radiation, Nuclear Science and Technology, 5,
Cascades in Peripheral Blood Mononuclear
16-22, 2015.

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VO THI THUONG LAN et al.

Cells and Proliferation of Prostate Tumor Laboratory Manual, Third Edition, 5.36-5.38,
Cells, Sci. Pharm., 79(2), 323–335, 2011. p. 1-3, 2006.
[14]. JL. Zimmer, RM. Slawson. Potential repair of [16]. NQ. Uyen, NX. Truong, PT. Ha, NHM.
Escherichia coli DNA following exposure to Quyen. Study some properties and the use of
UV radiation from both medium- and low- mutagen NTG to enhance the proteolytic
pressure UV sources used in drinking water activity of extracellular protease of Bacillus
treatment, Appl Environ Microbiol, 68, 3293– sp., Journal of Science, Vietnam National
99, 2002. University, Hanoi, 26 (2), 121-128, 2010.
[15]. J. Sambrook, DW. Russell, Alkaline Agarose
Gel Electrophoresis, Molecular Cloning: A

47
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 48-53

The effect of gamma-irradiation on graphene oxide in a


monoglyceride/ethanol solution
Luu Anh Tuyen1, Ha Thuc Huy2, Nguyen Thanh Duoc3,
Doan Binh3, Pham Thi Thu Hong3*

1
Center for Nuclear Techniques, 217 Nguyen Trai Street, HCM. City, Vietnam
2
University of Science – Ho Chi Minh City, 227 Nguyen Van Cu Street, HCM. City, Vietnam
3
Research and Development Center for Radiation Technology,
202A street 11, Linh Xuan ward, Thu Duc district, HCM. City, Vietnam
*Email: hongphamkado@gmail.com
(Received 20 May 2016, accepted 28 August 2016)

Abstract: Gamma-irradiation effects on graphene oxide (GO) in a monoglyceride/ethanol


(MG/EtOH) solution was investigated. GO was dispersed in MG/EtOH solution (GOM) with the GO:
MG ratio of 1:10 (w/w). The prepared GOM was irradiated by -ray under nitrogen atmosphere in a
range of absorbed dose from 0 to 50 kGy. The characteristics and morphology of reduced GOM were
analyzed by Ultraviolet-visible (UV-vis) spectroscopy, Fourier transform infrared (FT-IR)
spectroscopy, X-ray diffraction (XRD) and Transmission Electron Microscopy (TEM). The results
confirmed that the structure of reduced graphene oxide in monoglyceride solution was changed and
exfoliated completely after -ray irradiation at absorbed dose 50 kGy compared with non-irradiation
sample.

Keywords: reduction, monoglyceride, graphene oxide,  -ray.

I. INTRODUCTION methods have also been used to reduce


graphene oxide to graphene such as thermal
Graphene is a two-dimensional reaction, ultrasonic irradiation, gamma ray
crystalline material, discovered by two and/or electron beam irradiation because of
scientists Novoselov and Geim in 2004 [1]. their several advantages, including not using
The structure of graphene is a flat plate with a reducing agents, the product can be produced a
thickness of one atom of carbon atoms large amount, and being environmentally-
connected by the Sp2 bonds forming a friendly one [8-15]. Therefore, -ray and/or
hexagonal lattice, due to its interesting electron beam irradiation–induced reduction of
properties including excellent thermal GO in an ethanol/water and ethylenediamine
conductivity, large theoretical specific surface solution has been reported [11,12].
area, high electron mobility, good optical
transmittance, very thin, and harder than GO is synthesized from the oxidation of
diamonds [1,2]. Until now, graphene has been graphite so the GO structure contains
studied for applications in solar cells, polarizing function groups (hydroxyl, carboxyl,
electronic or optical devices, sensors, energy epoxide) [16].
storage and nanocomposite [3-6]. In recent In this paper, the effects of -ray
years, in addition to the chemical methods used irradiation on graphene oxide in a
to produce graphene from graphite through an monoglyceride/ethanol solution (GOM) were
intermediary graphene oxide [7], the physical studied. A monoglyceride (MG) is a fatty

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
PHAM THI THU HONG et al.

ester. Its chemical structure includes two an ice bath at 0oC. Then 38 g KMnO4 was
functional groups of hydroxyl and alkyl. So, added slowly. After 30 min, the temperature of
MG has self-asssembly ability when it the system was raised to 35 oC and the mixture
contacted with the polarized surface. When was continuously stirred in 2 hours for graphite
GO modified with monoglyceride, oxidation. Next step, the suspension was
monoglyceride could be self - assembly well diluted slowly by 460 ml of distilled water.
between the cavity of GO structure and The system was raised to 98 oC and stirred for
expanded the cavities or exfoliated single- 15 min. Then, the suspension continues to be
layer graphite oxide by the hydrogen bond diluted with 1,400 ml distilled water and to
formation with polarizing functional groups lower temperature of reaction system to 50 oC.
on the surface of GO. After creating To remove residual KMnO4 and other
monolayer modified GO, -ray irradiation – impurities, 500 ml H2O2 (30 wt.%) was added
induced reduction of method is used to restore to the mixture. After completion of the
the aromatic skeletons (Sp2 bonds) of mono- reaction, the suspension became bright yellow
layer graphite and/or the preeminent in color. The prepared suspension was
properties of the pristine Graphite. centrifuged, washed with HCl (5 wt. %)
solution to remove all residual ions of SO4-2.
II. EXPERIMENTAL After that, hydrochloride acid and other
impurities in GO suspension were removed by
Chemicals and materials
acetone solvent. Finally, the repaired
Graphite flake (purity 99.9%) was suspension of GO was dried at 60 oC in
purchased from SEC Carbon, Japan. vacuum and ground into fine powder.
Monoglyceride with Mw = 356.54 g/M (MG)
was supplied by Kamdhenu Foods Ltd., Delhi, Preparation of GOM and iGOM
India. Ethanol (99.5 wt.%) (EtOH) was GO suspension in a MG/EtOH blend
provided by Chemical and scientific solution (GOM) was prepared by adding an
technology JSC, Hochiminh City Branch, amount of 0.01 g GO, 0.1 g MG into 10 ml
Vietnam. Sulfuric acid (H2SO4), hydrogen ethanol/distilled water solution (25 v/v %)
peroxide (H2O2), potassium permanganate and dispersing under ultrasonic for 1 hour.
(KMnO4), sodium nitrate (NaNO3), After deoxygenated by nitrogen bubbling for
hydrochloric acid (HCl), acetone were obtained 10 min, the prepared suspension is sealed
from commercial sources. All chemicals were and irradiated at a room temperature by  -
of reagent grade and used without further ray. The total absorbed doses were ranged
purification. Distilled water was used in all from 0 to 50 kGy at a dose rate of 1.0 kGy/h.
experiments. A commercial alpha-cellulose Afterward, irradiated GOM (iGOM) was
membrane with 8-12 m pore-size was used obtained by filtration and washed with
for filtration. distilled water several times and dried an
Synthesis of Graphite oxide (GO) oven at 70 oC.

The Hummers method was used to Characterization methods


synthesize GO from a graphite powder [16]. UV-vis absorption spectra were recorded
Accordingly, 10 g graphite, 5 g NaNO3, and on a UV-vis spectrophotometer (JASCO V630,
240 ml H2SO4 (98 wt.%) were placed in 2,500 Japan) within the wavelength region of 200-
ml four-neck flask. The mixture was stirred in 800 nm. Distilled water was used as a solvent.

49
THE EFFECT OF GAMMA-IRRADIATION ON GRAPHENE OXIDE IN …

FT-IR spectra were colleted by a FTIR at 242 and 264 nm, and the absorption peak
spectrophotometer (8400S, Shimadzu, Japan) of iGOM-50 kGy was shifted toward a longer
using KBr pellets on the transmission module wavelength at 264 nm in comparison to that
at 4 cm-1 resolution and for 20 scans. the control GOM (0 kGy) at 240 nm (*
The X-ray diffraction (XRD) was carried transition of aromatic C–C bonds) and at 300
out using X Pert‟ Pro, Panalytical model at a nm (n* transition of C=O bonds)
scanning rate of 0.04o/s in a wide angle range [13,17,18]. The overall results were
(2 = 0-60o) with monochromatized Cu K demonstrated that GO was reduced in
radiation (= 1.5406Å). MG/EtOH solution by -ray and GO was
reduced completely at an absorbed dose of
The Transmission electron microscopy 50 kGy.
(TEM) measurements of all the samples were
carried out in the high resolution scanning FT-IR analysis
electron micro-scope JEM 1010, JEOL in a FT-IR spectroscopy was used to
transmission mode characterize the functional groups attached to
MG, non-irradiated GOM and irradiated GOM
III. RESULTS AND DISCUSSION as shown in Fig. 3, the oxygen containing
functionalities at 3315 (hydroxyl, -OH), 1731
Gamma irradiation of GOM
(carboxyl, C=O), 1392 and 1049 cm-1 (epoxide,
Fig. 1 shows the images of the GO C–O) were greatly reduced with an increase in
dispersion in MG/EtOH mixture solution and the absorbed dose. In comparison to the FT-IR
the irradiated dispersion at 50 kGy with a spectra of MG and GOM, the FT-IR spectrum
dose rate of 1.0 kGy/h. Evidently, the brown of iGOM-50 kGy was appeared a new peak at
color of initial GO dispersion changed in 1575 cm-1 attributed to the stretching vibration
black after gamma irradiation. bands C=C. It was suggested that the
restoration of aromatic skeletons (Sp2 bonds)
(a) (b) [12,15] on the mono-layer graphite was
occurred in the sample of iGOM-50 kGy,
which correspond to the results of the UV-Vis
spectra analysis.
XRD study
The XRD patterns for graphite, GO,
non-irradiated and irradiated GOM samples are
described in Fig. 4. In case of pristine graphite,
Fig.1. Photographs of non-irradiated GOM a sharp diffraction peak was observed at 2 =
dispersion (a), and GOM dispersion irradiated at 26.49o (d-spacing = 3.36 Å) corresponding to
50 kGy (b).
the (002) plane of graphite. GO has damaged
UV-Vis spectra crystalline structure with a broad diffraction
The -ray irradiation–induced peak was observed at 2 = 10.87o (d-spacing =
reduction of GO in MG/EtOH mixture 8.13 Å) indicating introduction of hydrophilic
solution was studied by UV-vis as presented functional groups (-OH, -COOH, epoxide) to
in Fig. 2, the UV-Vis spectra of iGOM- carbon layers.
23.5kGy was appeared two absorption peak

50
PHAM THI THU HONG et al.

Fig. 2. UV-Vis spectra of non-irradiated GOM (a), GOM irradiated at 23.5 kGy (b) and 50 kGy (c).

Fig. 3. FT-IR spectra of MG (a), non-irradiated GOM (b), GOM irradiated at 23.5 kGy (c) and 50 kGy (d).

For iGOM-50 kGy sample (Fig. 4d), a perfectly flat. Dark areas in Fig. 5a indicate the
new broaden diffraction peak was appeared at thick stacking nanostructure of several
2 = 21.52o (d-spacing = 4.12 Å) instead of the graphene oxide and/or graphene layers in
peak at around 10.87o of GO and GOM (0 MG/EtOH solution.
kGy) suggesting the efficient reduction and
After –ray irradiation, the image of
exfoliation [11,15] of GO by -gamma iGOM-50 kGy (Fig. 5b) is observed on highly
irradiation in a MG/EtOH solution. exfoliated graphite. The higher transparency
TEM analysis areas indicate much thinner sheets of a few
layers stacked attributed to reduced graphene
Fig. 5 presents TEM images of non-
oxide due to from stacking nanostructure
irradiated GOM and GOM irradiated at 50
exfoliation [15,18].
kGy. The non-irradiated GOM sheets are not

51
THE EFFECT OF GAMMA-IRRADIATION ON GRAPHENE OXIDE IN …

Fig. 4. XRD pattern of Graphite, GO (a), non-irradiated GOM (b), GOM irradiated at 23.5 kGy (c)
and 50 kGy (d).

a b

Fig. 5. TEM images of non-irradiated GOM (a) and iGOM-50 kGy (b)

III. CONCLUSIONS ACKNOWLEGEMENTS

GO was successfully reduced in a The authors thank University of


monoglyceride/ethanol solution by gamma Science – Ho Chi Minh City, Center for
irradiation under nitrogen gas. The UV-vis, Nuclear Techniques, HCM City for GO
FT-IR, XRD and TEM results confirmed that preparation and XRD measurement. We are
GOM can be simply and quickly reduced by  also thankful to Research and Development
–ray irradiation, and the resulting iGOM Center for Radiation Technology, HCM City
exhibited dose-dependent manner. This method for γ–irradiation and FT-IR, UV-Vis
is a promising way for the massive production measurement.
of graphene from GO with a support of the
self-assembly agent as MG.

52
PHAM THI THU HONG et al.

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Materials Letters, 126, 151–153, 2014.
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53
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 54-59

The Brandon mathematical model describing the effect of


calcination and reduction parameters on specific surface area of
ex-ADU UO2 powders
Nguyen Trong Hung, Le Ba Thuan, et.al.

Institute for Technology of Radioactive and Rare Elements (ITRRE),


48 Lang Ha, Dong Da, Ha Noi, Vietnam.
Email: nthungvaec@gmail.com
(Received 19 April 2016, accepted 14 June 2016)

Abstract: The report “Brandon mathematical model describing the effect of calcination and reduction
parameters on specific surface area of UO2 powders” [14] has built up a mathematical model describing
the effect of the fabrication parameters on SSA (Specific Surface Area) of ex-AUC (Ammonium
Uranyl Carbonate) UO2 powders. In the paper, the Brandon mathematical model that describe the
relationship between the essential fabrication parameters [reduction temperature (TR), calcination
temperature (TC), calcination time (tC) and reduction time (tR)] and SSA of the obtained ex-ADU
(Ammonium Di-Uranate) UO2 powder product has established. The proposed model was tested with
Wilcoxon’s rank sum test, showing a good agreement with the experimental parameters. The proposed
model can be used to predict and control the SSA of ex-ADU UO2 powders.
Keywords: UO2 powder, Ammonium Di-Uranate (ADU), Brandon mathematical model.

I. INTRODUCTION and granulation) might be omitted for UO2


ceramic pellet preperated from the ex-AUC
The manufacture of the UO2 nuclear fuel UO2 powder [1, 7-9].
pellets includes the conversion of UF6 into UO2
powder and the fabrication of UO2 pellets from Chemical reactions for ADU formation
such UO2 powder [1-3]. In regard to the from uranyl solution, in particular, are as below
conversion of UF6 into UO2 powder, many dry [6]:
and wet conversion methods have been 2UO2F2 + 6NH4OH = (NH4)2U2O7 + 4NH4F +
developed [4-9]. In a former wet conversion, 3H2O (1)
UF6 was hydrolyzed in water to form uranyl
2UO2F2 + 6NH3(gas) + 3H2O = (NH4)2U2O7 +
fluoride – fluoride acid (UO2F2-HF) solution.
4NH4F (2)
Subsequently, the solution was precipitated
through either an ammonium di-uranate (ADU) The ADU intermediate products are often
route or an ammonium uranyl carbonate (AUC) contaminated with fluoride (F) ions. So, the
route. These ADU and/or AUC powders are preparation of UO2 powder via ADU route
then calcinated and reduced into UO2 powders includes two sequential steps: the calcination of
[5-9]. The ex-ADU UO2 powder possesses ADU precipitate into U3O8 powder with
some characteristics different from the ex-AUC coincident F elimination and the reduction of
UO2 powder, such as particle size and the U3O8 into UO2 ceramic powder [10-11].
flowability [7-9]. The flowability and the These two steps are essential in the UO2 pellet
particle size of the ex-AUC UO2 powder are fabrication.
better than those of the ex-ADU UO2 powder, The parameters of the UO 2 preparation
so press feed preparation stage (pre-pressing strongly affect the final characteristics of UO 2

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
NGUYEN TRONG HUNG, LE BA THUAN, et.al.

powder and, therefore, have an effect on UO2 II. EXPERIMENTAL SECTION


pelletizing [6-9]. Specific surface area (SSA)
of the UO2 powder is one of the most The ADU powder was precipitated by the
important characteristics affecting the activity reaction of ammonium liquid with a solution
and the correspondence of the powder during containing uranyl fluoride (UO2F2) and fluoride
UO2 ceramic pellet fabrication. The SSA is a acid (HF) with U:F molar ratio of 1:6. The
function of grain size, aggregation and solution is composed of the same constituents
agglomeration, morphology and structure of (UO2F2 and HF) and their molar ratio as the
the powder [6-9]. Therefore, SSA is product of the UF6 hydrolyzing process.
considered as the most important feature to Analytical grade nitrogen and hydrogen were
assess sinterability of the UO 2 powder. In used as pure gases during calcination and
report [14], we built a mathematical model to reduction.
describe the relationship between its SSA and The calcination of ADU into U3O8 and
the process parameters for the calcination and the reduction of the U3O8 into UO2 powder were
reduction for the ex-AUC UO2 powder, the carried out in an apparatus consisting of a
equation was: rotary tube furnace 1300oC (Nabertherm,
( ) ( Germany) and hydrogen-nitrogen-steam supply
)( system. Figure 1 shows a sketch of our
)( apparatus. The calcination was carried out over
)( a range of time and temperatures in an
atmosphere of nitrogen and steam (1:1 in molar
) ( )
ratio). After the calcination finished, the
subsequent reduction was carried out in a
reducing atmosphere of hydrogen and nitrogen
In the paper, we would establish a
gases (3:1 in molar ratio). The final product was
mathematical model to describe the relationship
UO2 powder. The specific surface area (SSA)
between its SSA and the process parameters for
of the obtained UO2 powder was measured by
the calcination and reduction that were
the Brunauer–Emmett–Teller (BET) method
employed for UO2 powder fabrication via ADU
(Coulter SA 3100, USA).
route.

Fig. 1. Experimental setup, 1. N2 flow for reduction; 2. Valve of H2 and N2 mixture flow for reduction; 3. N2
flow for calcination; 4. Valve of N2 and H2O (stream) mixture flow for calcination; 5. H2 flow for reduction; 6.
Valve for gases out;

55
THE BRANDON MATHEMATICAL MODEL DESCRIBING THE EFFECT OF CALCINATION …

III. RESULTS AND DISCUSSION Brandon model by determining corresponding


parameters in that order.
Multiple regression analysis for the
establishment of Brandon equation By using the method of least squares and
Solver tool of Microsoft Excel, the function
In order to master preparing the UO2 f1(TR) is determined in the equation as follows:
powders whose properties are appropriate to the
UO2 ceramic pellet fabrication and on the basis ( ) (8)
of experimental data that describe the effects of ŷ1 was calculated as follows:
process conditions on SSA of UO2 powder, a
( )
statistical modeling method using Brandon ̂ ( )
( ) ( )
multiple regression model is used. The form of
Brandon mathematical equation is as follows: With the same calculation, the other
functions of TC, tC, and tR were obtained as
( ) ( ) ( ) ( ) ( ) bellows:
Where, y denotes the SSA of UO2 ( ) (10)
powder, fj(xj) are the functions presenting the
effect of process parameter xj on SSA (y), and a ( ) (11)
is a constant [12-14]. ( ) (12)
In Brandon equation, the series of The corresponding independent functions
functions fj(xj) are presented in a descending ŷ1 were:
order of the relevance of process factors.
̂
̂ ( )
In order to establish Brandon equation, ( )
an experimental data set y; x1, x2,…xk is used
̂
for determining the regression function y = ̂ ( )
( )
f1(x1). From f1(x1), a new data set is obtained by
evaluating: ̂
̂ ( )
( )
̂ ( )
( ) All of these values are reported in Table I.
As a result, ŷ1 is independent on x1 but is The constant a in Brandon equation was
affected by x2, x3, …xk: calculated from average of y4 to be 0.999813.
̂ ( ) ( ) ( ) ( ) ( ) Thus, Brandon function describing the
effect of the process parameters on the SSA of
The others fj(xj) are calculated in the
same way with f1(x1), we obtain: the UO2 powder is in the form:
( ) ( ) ( ) ( ) ( )( )
̂ ( )
( ) ( ) ( ) ( ) ( )
Our experimental data indicated that four ( )(
parameters (factors) affecting SSA of UO2 )( )(
powder are in a descending order as follows: ) ( )
reduction temperature T R, calcination
SSA(Cal.) values of the UO2 powder are
temperature TC, calcination time tC, and
shown in Table I.
reduction time tR. Thus, we established

56
NGUYEN TRONG HUNG, LE BA THUAN, et.al.

Table I. Experimental and calculated data of function f1(TR) and ŷ1; f2(TC) and ŷ2; f3(tC) and ŷ3; f4(tR)
and ŷ4; and SSA(Cal.) (ŷ) used to establish Brandon mathematical model

TR tR TC tC SSA(Ex.)(ÿ) SSA(Cal.)
Sample (m2/gr.)
f1(TR) ŷ1 f2(TC) ŷ2 f3(tC) ŷ3 f4(tR) ŷ4 (ŷ)
o
( C) (hr.) (oC) (hr.) (m2/gr.)

M1 550 5 650 4 4.430 3.991 1.110081 1.138 0.975467 0.984 0.991429 1.012 0.980 4.519
M2 600 5 650 4 4.333 3.871 1.119436 1.138 0.983687 0.984 0.999783 1.012 0.988 4.383
M3 650 5 650 4 5.521 3.751 1.471992 1.138 1.29349 0.984 1.314656 1.012 1.300 4.247
M4 700 5 650 4 3.478 3.631 0.957942 1.138 0.841777 0.984 0.855551 1.012 0.846 4.112
M5 600 2 700 3 4.070 3.871 1.051489 0.993 1.058902 0.951 1.113930 0.975 1.142 3.563
M6 600 3 700 3 3.340 3.871 0.862893 0.993 0.868976 0.951 0.914134 0.987 0.926 3.607
M7 600 4 700 3 3.514 3.871 0.907846 0.993 0.914246 0.951 0.961757 1.000 0.962 3.651
M8 600 5 700 3 3.538 3.871 0.914047 0.993 0.920490 0.951 0.968325 1.012 0.957 3.695
M9 700 3 600 5 4.199 3.631 1.156526 1.283 0.901423 1.017 0.886181 0.987 0.897 4.678
M10 700 5 700 4 3.626 3.631 0.998705 0.993 1.005746 0.984 1.022203 1.012 1.010 3.588
M11 700 3 700 5 3.549 3.631 0.977497 0.993 0.984388 1.017 0.967743 0.987 0.980 3.620
M12 650 4 750 2 2.917 3.751 0.777721 0.848 0.917124 0.917 0.999809 1.000 1.000 2.916
M13 650 4 750 3 2.868 3.751 0.764657 0.848 0.901718 0.951 0.948578 1.000 0.949 3.021
M14 650 4 750 5 3.424 3.751 0.912896 0.848 1.076529 1.017 1.058325 1.000 1.059 3.233

Test Brandon mathematical model by Group SSA(Cal.): Y1, Y2, Y3, …, Yn2;
Wilcoxon’s rank sum test distribution ŷ
The Wilcoxon rank-sum test is a Null Hypothesis: SSA(Ex.) = SSA(cal.)
nonparametric alternative to the two-sample
Herein, SSA(Ex.) is experimentally
(for example A and B) test that we wish that the
obtained SSA. The two groups are combined
data of measurements in population A is the
into one group (for example WT) WT of W(1),
same as that in B. We have two groups:
W(2), W(3), …, W(n1+n2); order data in the
Group SSA(Ex.): X1, X2, X3, …, Xn1; combined group W(1) ≤ W(2) ≤ . . . ≤ W(n1+n2);
distribution ÿ and then assign ranks (as in Table II).

Table II. Order of all observations in the combined sample and assign ranks
of the group WT (SSA(Cal.) data are underlined)

WT 2.868 2.916 2.917 3.021 3.233 3.34 3.424 3.478 3.514 3.538

Rank 1 2 3 4 5 6 7 8 9 10

WT 3.549 3.563 3.588 3.607 3.62 3.626 3.651 3.695 4.07 4.112

Rank 11 12 13 14 15 16 17 18 19 20

WT 4.199 4.247 4.333 4.383 4.43 4.519 4.678 5.521

Rank 21 22 23 24 25 26 27 28

57
THE BRANDON MATHEMATICAL MODEL DESCRIBING THE EFFECT OF CALCINATION …

Thus, sum of ranks S of group ŷ is 95% reliability of T is: T  1.96   T


calculated as follows:
T  1.96   T  203 1.96  21.76  160.35
S=2+4+5+12+13+14+15+17+18+20+22+24
T  1.96   T  203  1.96  21.76  245.65
+26+27=219
The sum of ranks S of group ŷ is 219, in
Mean rank (T) of distribution ŷ is:
reliability range from 160.35 to 245.65, so two
n2 (n1  n2  1) 14(14  14  1) group SSA(Ex.) and SSA(Cal.) are asserted to be
T    203
2 2 the same. Figure 2 is the plot comparing SSA(Ex.)
with SSA(Cal.) of the UO2 powder indicating the
And the variance is:
agreement of the proposed calculation with the
n1n2 (n1  n2  1) 14  14(14  14  1) experimental data. Thus, we suppose that the
 T2    473.66
12 12 Brandon mathematical model is capable to
describe the effect of the factors on the SSA of
σT = σT2 = 473.66=21.76 the UO2 powder that was obtained from the
calcination and reduction of ADU.

5.5

5
SSA(cal.), in m2/gr.

4.5

3.5

2.5

2
2 2.5 3 3.5 4 4.5 5 5.5 6
SSA(ex.), in m2/gr.

Fig. 2. Comparison of SSA(Ex.) and SSA(Cal.) of the ex-ADU UO2 powder.

IV. CONCLUSIONS calcination time (tC) and reduction time (tR)]


and SSA of the obtained ex-ADU UO2 powder
In this paper, we proposed a product. The proposed model was tested with
mathematical model describing the effect of the Wilcoxon’s rank sum test, showing a good
fabrication parameters on SSA of the ex-ADU agreement with the experimental parameters.
UO2 powders. To the best of our knowledge, The proposed model was well applied for
the Brandon model as presented in equation (17) roughly predicting SSA of the ex-ADU UO2
is used to describe the relationship between the powders that is fabricated by means of
essential fabrication parameters [(reduction calcination and reduction of ADU at our
temperature (TR), calcination temperature (TC), institution.

58
NGUYEN TRONG HUNG, LE BA THUAN, et.al.

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N.Y. Smirnov, and V. V. Zarutskii, “Study of
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59
Nuclear Science and Technology, Vol.6, No. 3 (2016), pp. 60-66

The efficient neutron-gamma pulse shape discrimination with


small active volume scintillation detector
Phan Van Chuan1, Nguyen Duc Hoa1, Nguyen Xuan Hai2, Nguyen Ngoc Anh2,
Tuong Thi Thu Huong2, Nguyen Nhi Dien2, Pham Dinh Khang3
1
Dalat University, 01 Phu Dong Thien Vuong, Dalat, Lam Dong, Vietnam
2
Nuclear Research Institute, 01 Nguyen Tu Luc, Dalat, Lam Dong, Vietnam
3
Hanoi University of Science and Technology, 01 Dai Co Viet, Hanoi, Vietnam
(Received 13 September 2016, accepted 07 December 2016)

Abstract: A small detector with EJ-301 liquid scintillation was manufactured for the study on the
neutron-gamma pulse shape discrimination. In this research, four algorithms, including Threshold
crossing time (TCT), Pulse gradient analysis (PGA), Charge comparison method (CCM), and
Correlation pattern recognition (CPR) were developed and compared in terms of their discrimination
effectiveness between neutrons and gamma rays. The figures of merits (FOMs) obtained for 100 ÷ 2000
keVee (keV energy electron equivalent) neutron energy range show the charge comparison method was
the most efficient of the four algorithms.
Keywords: EJ-301 liquid scintillation detector, threshold crossing time, pulse gradient analysis,
charge comparison, correlation pattern recognition.

I. INTRODUCTION convertor (ADC), field programmable gate


array (FPGA), and digital signal processing
The neutron - gamma (n-) pulse shape (DSP). That makes the PSD methods widely
discrimination (PSD) techniques are very applied. In modern PSD systems, pulses from
important in the fast neutron measurement detector are digitized by flash ADC and the
using the scintillation detectors. Among of data are stored in memory and analyzed by PSD
these detectors, the EJ-301 liquid scintillation method on computer[5-7], or on the board
detector has been widely employed because of FPGA/DSP [4]. Almost studies of neutron -
their excellent neutron-gamma discrimination, gamma PSD were performed on different
high efficiency for the fast neutron detection detectors; however, the evaluation of neutron-
and superior time resolution. It detects both gamma PSDs’ capacities has not been carried
neutron and gamma ray and the two particle out. In this work, a prototype of a small active
types can be distinguished by analyzing the volume scintillation detector was made for
shapes of measured pulses. studying neutron and gamma measurement.
Various n- PSD techniques have been Based on the digitized pulses from the detector,
developed, including both analog and digital the four algorithms of RTD, PGA, CCM and
approaches such as zero-crossing method, CPR have been used to evaluate the detector’s
constant fraction discriminator [1,2], charge efficiency for neutron-gamma discrimination.
comparison [2,3], frequency gradient analysis
II. EXPERIMENT
[4], threshold crossing time, correlation pattern
recognition methods [5], etc. A. Experiment setup
Fast electronics development has created The prototype detector’s intrinsic volume
new techniques such as flash analog digital has the dimensions of 34mm in diameter and

©2016 Vietnam Atomic Energy Society and Vietnam Atomic Energy Institute
NGUYEN XUAN HAI et al.

60mm in length. It was filled with EJ301 liquid characterized difference between neutron and
scintillator and encapsulated in an aluminum gamma would be located in the tail of the pulse.
cell whose walls were1mmthick and well-
The detector testing was done with
polished. The scheme of the detector is shown
radioactive sources and digital oscilloscope.
in Fig. 1. The scintillation cell was contacted
Fig. 2 shows the layout of experimental
with a Hamamatsu R9420 photomultiplier tube
arrangement; in which the high voltage power
(PMT) with operating negative voltage of
supply was a model 3002D and detector’s
1200V through a 2 mm thick ultra violet glass
output was connected to the input of
layer. The output pulses from the anode of the
oscilloscope model DPO7254C. The standard
PMT which had very short rise time (less than
gamma ray sources (22Na, 60Co and 137Cs) were
5ns) and small amplitude were not digitized
also used to initially characterize the energy
convenient. Because of that, a fast preamplifier
performance of the detector. The 252Cf neutron
was connected directly to the anode of the
source with the activity of approximately 3.0
PMT. The preamplifier would shape the pulses
mCi was used to evaluate the detector’s
which had the rise time of approximately 10ns
efficiency of neutron-gamma separation. The
and fall time of approximately 30ns. These
DPO7254C with 8-bit resolution was operated
shapes removed the causes of distortion in
on sampling rate of 1 Giga-sample per second.
cables, but retained the different characteristics
The sampling data were saved on a memory
of scintillator pulses induced by neutron or
stick for off-line analysis.
gamma particles. Because slower decay time-
constant of EJ301 is about 32ns, the

1
2 3 4 5

neutrons

Fig. 1. Scheme of neutron detector: (1) detector vessel; (2) liquid scintillator; (3) UV window glass; (4)
PMT; (5) Preamplifier (Preamp).

Neutron source Digital oscilloscope Computer


252Cf
100cm
H.V.

EJ301 PMT Preamp

Fig. 2. Diagram of the experimental setup.

B. Data analysis proportion of the slow scintillation component.


The PSD methods are based on the different
The typical pulse shapes of the EJ-301
characteristics in the pulse tails of neutrons and
liquid scintillation detector are shown in Fig. 3;
gamma-rays. In this work, TCT, PGA, CCM
the neutron pulses exhibit a larger decay time to
and CPR methods were applied for data
the base line, which is due to a greater
analysis.

61
THE EFFICIENT NEUTRON-GAMMA PULSE SHAPE DISCRIMINATION WITH …

Fig. 3. Typical sample of detector signals for neutron and gamma ray in one sampling frame.

a) TCT method is carried out by ∫ ( ) ∑ ( ) (2)


measuring the time interval (∆t) between the
time where the pulse amplitude begins to fall Where V(k) is the amplitude of the kth in
(t2) and the time where the amplitude cuts the sampling period T, t1 and t2 are timing of
threshold (t3) (see Fig. 3). The time where the beginning and ending of sampling period and t
amplitude is over the threshold of neutron = t2 – t1.
pulses is greater than that of the gamma pulses, d) For CPR method, a signal is
so it was used as a parameter to neutron - considered as an object vector X whose
gamma PSD. components are the digitized amplitude xn of
b) PGA method is gradient analysis of the signal at sampling time tn. CPR is
the integrated pulses to discriminate neutron performed by taking a scalar product of this
and gamma radiation. The value of gradient is vector with the reference vector Y which
based on the comparison of the relative heights describes a gamma ray or neutron signal [5].
of the samples at the pulse tail, and determined
by equation (1) [11]. X  ( x1, x2 ,..., xn ); Y  ( y1,y2 ,..., yn ) (3)

dV ( t ) V ( k  nT )  V ( k )
   X .Y
dt nT r (4)
(1) X .Y
Where V(k) is the amplitude of the kth in
sampling period T and n is the number of Where, r is the correlation coefficient
sampling periods. In approximation, if n is a
between vector X and vector Y , X .Y is
constant, then | ( ) ( )|.
scalar product, X and Y are the norm of the
c) CCM is based on area comparison of
vectors X and Y respectively.
the rising or the falling portions of a pulse.
n
Because the pulse gradient of neutrons is  xi . yi
different from that of gamma rays; therefore, i 1
  Acr cos (5)
the ratios of a pulse area are also changed. The n n
 xi 
2 2
area S of the pulse was calculated based on yi
i 1 i 1
equation (2) [5].

62
NGUYEN XUAN HAI et al.

Where,  ( rad ) is the angle between the III. RESULTS AND DISCUSSION
vectors; the  value indicates the similarity of A. Results
the object vector with the reference vector. Fig. 4 shows the amplitude spectra which
C. Evaluation of pulse shape discrimination were measured with radioisotope sources of
60
Co, 22Na and 137Cs. The upper inset plot shows
The FOM was used to evaluate the the results of amplitude calibration in which its
quantitative results of neutron-gamma points are the positions of Compton edges
discrimination, and defined by equation 6. coinciding with the gamma peaks induced from
radioisotope sources. These data points were
Chn  Ch
FOM  fitted with a linear model with first order
FWHM n  FWHM  function as E(Ch) = 0.188×Ch - 30.55; where E
(6)
and Ch are energy and channel, respectively.
Where, Chn , Ch are the positions of
The measured data with a neutron
neutron and gamma peaks respectively; source 252Cf were analyzed by the methods of
FWHMn and FWHM are the full-width-half- TCT, PGA, CCM and CPR. The scatter plots
maximums of neutron and gamma peaks of the n- separation with energy threshold of
respectively, in the histogram. 100keVee by four methods are shown in Fig.
5, 6, 7 and 8.

Fig. 4. Pulse height distribution from sources of 60Co, 22Na and 137Cs. The upper inset shows the calibration
data using the Compton edges of the gamma - ray spectra

Fig. 5. Threshold crossing time versus pulses Fig. 6. Pulses gradient versus pulse height

63
THE EFFICIENT NEUTRON-GAMMA PULSE SHAPE DISCRIMINATION WITH …

Fig. 5 shows the two-dimensional plot of angle ratios versus pulse heights for each
threshold crossing time versus pulse amplitude. waveform. Based on the analytical results, the
The data in Fig. 5 show that n- PSD of the discrimination between neutron-gamma pulses
pulse heights for each waveform in the energy in the RTD and CCM methods are better than
region greater than 500 keVee is good. Fig.6 is the PGA and CPR methods in the high energy
the scatter plot of gradients versus pulse heights region (> 200 keV).
for each waveform. Fig.7 shows the scatter plot Fig. 9, 10, 11 and 12 are the statistical
of area ratios of pulse tails versus pulse heights charts of four methods, the energy threshold
for each waveform. Fig.8 is the scatter plot of was set at 800keV.

Fig. 7.The integrated charge versus pulse heights Fig. 8. Angle ratios versus pulse heights

Fig. 9. Histogram of threshold crossing time Fig. 10. Histogram of pulse gradient analysis

Fig. 12 shows the distribution of FOM Fig. 12 shows the distribution of FOM
values of methods as threshold crossing time, values of methods as threshold crossing time,
pulse gradient analysis, charge comparison, and pulse gradient analysis, charge comparison, and
correlation pattern recognition in the range of correlation pattern recognition in the range of
energy from 100 to 2000keVee. energy from 100 to 2000keVee.

64
NGUYEN XUAN HAI et al.

Fig. 11. Histogram of charge comparison Fig. 12. Histogram of correlation pattern

Fig. 13.The FOM values as a function of energy threshold corresponding with four methods as threshold
crossing time, pulse gradient analysis, charge comparison, and correlation pattern recognition in the range of
energy from 100keV to 2000keV

Table I shows FOM values at 700 keV considered as specialist of the four surveyed
energy threshold and duty time for data methods.
processing. The values in the table can be
Table I. The FOM values and processing time of PSD methods
Method FOM (at 700keV) Processing time (ns)

Threshold crossing time 1.10 260 ± 6


Pulse gradient analysis 0.78 86±2
Charge comparison 1.20 170 ± 3
Correlation pattern recognition 0.98 228 ± 2

B. Discussion the active volume of the detector was small-


typed. In this detector, the FOM of CCM
The obtained FOM values were in the
method was the highest in the energy region of
average range from 0.2 to 1.4. This result is
100 keV to 2000 keV.
suitable for the simulation estimation because

65
THE EFFICIENT NEUTRON-GAMMA PULSE SHAPE DISCRIMINATION WITH …

The difference of FOMs between CCM Methods Phys. Res. Sect. A Accel.
and TCT is less than twenty percent, but the Spectrometers, Detect. Assoc. Equip., Vol. 527,
processing time of TCT is about thirteen No. 3, pp. 512–518, 2004.
percent larger than that of CCM. However the [4] G. Liu, M. J. Joyce, X. Ma, and M. D. Aspinall,
algorithm implementation for TCT method is “A digital method for the discrimination of
rather simple and can easily be done on the neutrons and rays with organic scintillation
neutron measuring system using an FPGA. The detectors using frequency gradient analysis,”
PGA method has the shortest processing time, Nucl. Sci. IEEE Trans., Vol. 57, No. 3, pp.
1682–1691, 2010.
but its’ FOM is small and not stable in the
surveyed energy region with the detector's [5] D. Takaku, T. Oishi, and M. Baba,
small active volume. “Development of neutron-gamma
discrimination technique using pattern-
IV. CONCLUSIONS recognition method with digital signal
processing,” Prog. Nucl. Sci. Technol., Vol. 1,
This study surveyed the efficiency of pp. 210–213, 2011.
distinguishing between neutron and gamma [6] S. Marrone, D. Cano-Ott, N. Colonna, C.
pulses from the small active volume Domingo, F. Gramegna, E. M. Gonzalez, F.
scintillation detector using the EJ-301 liquid Gunsing, M. Heil, F. Käppeler, P. F. Mastinu,
scintillation. The four neutron-gamma PSD and others, “Pulse shape analysis of liquid
algorithms were used to do the analysis and the scintillators for neutron studies,” Nucl.
results show that the FOM of CCM method is Instruments Methods Phys. Res. Sect. A Accel.
better than of the TCT, PGA, and CPR Spectrometers, Detect. Assoc. Equip., Vol. 490,
methods. These results are the basis for No. 1, pp. 299–307, 2002.
building the neutron detection systems using [7] S. D. Jastaniah and P. J. Sellin, “Digital pulse-
the EJ-301 liquid scintillation detectors with a shape algorithms for scintillation-based neutron
small active volume in combination with DSP detectors,” IEEE Trans. Nucl. Sci., Vol. 49 I,
and FPGA techniques. no. 4, pp. 1824–1828, 2002.
[8] G. F. Knoll, Radiation Detection and
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