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Design and analysis of internal 20K helium gas purification system

for the KW class Helium Refrigerator/Liquefier


A Report submitted in partial fulfillment of the requirements for the degree of Master of
Technology in Cryogenics and Vacuum Technology


By
Adarsh Kumar Behera
Roll: 212ME5403




Under the supervision of



Internal Supervisor: External Supervisor:
PROF. R.K Sahoo Mr. A. K. Sahu
Department of Mechanical Engineering, Engineer SF, Division Head,
NIT Rourkela Large Cryogenic Plant & Cryosystem,
Institute for Plasma Research,
Bhat, Gandhinagar.






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ACKNOWLEDGEMENTS

With respectable regards and immense pleasure I take it as a privilege to
express my profound sense of gratitude and indebtedness to my supervisor
Prof. R .K SAHOO, Assistant Professor, Department of Electrical Engineering,
NIT Rourkela, Rourkela, for his encouragement, guidance and great support during
the project work. He was always motivated and shares his expertise during the
whole course of project work.
I am extremely thankful to Mr A.K SAHU Scientist / Engineer SF
Division Head Large Cryogenic Plant and Cryosystem ,Institute for Plasma
Research, for his erudite suggestions, perceptive remarks, wondrous guidance and
affection.
In addition, none of this would have been possible without the support of my
parents who have guided me and nurtured me in an academic friendly
environment. I express my deep sense of gratitude towards them.
I shall be failing in my duty, if I dont express my thanks to NIT
ROURKELA for providing me the financial help in the form of stipend and also
encouragement to complete the study successfully.






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CONTENTS:
Acknowledgements..............................................................................2
Contents...3
Abstract........................................................................4
1. Introduction..5
2. Literature review..6
2.1Adsorption...8
2.2Pressure swing adsorption...8
2.3Temperature swing adsorption8
2.4Cryogenic adsorption mechanism...9
3. Adsorbents.......................................................................9
4. Calculation.12
5. Conclusion.16
6. References..16







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ABSTRACT: The Helium refrigerator/Liquefier (HRL) is normally operated with helium gas having
purity better than 99.999% by volume which is equivalent to having 10PPM (parts per million) impure
gas in helium gas. Although sufficient precautions and impurity removal procedures are used, still, in the
process of gas transfer or due to some other processes before reaching to liquefaction, impurity level
sometimes can go as high as 500 PPM averaging to about 100 PPM. These impurities mainly consists of
gases present in the air, like N
2
,O
2,
Ar,H
2
,H
2
O,CO,CO
2
and the traces of Ne. Hydrocarbons of the
lubricating oil can also be sources of H
2
.These gases condense at significantly higher temperature
compared to LHe (4.5K).If such high level of impurity enters the process equipment placed inside the
cold box of HRL, then it can condense and choke the pipelines and the valves leading to large pressure
drop and inefficient liquefaction process. Sometimes condensed and choked impurity can destroy the
blades of turbines of the HRL. Hence to be on safer side generally, internal purifiers are place at two
temperature levels inside the cold box to take care the operational problem due to impurities .One is at
80K to remove N
2
,O
2,
Ar. And another one is at 20k to remove H
2
.This project is about the design and
analysis of 20K purification system. The impurity level of H
2
in helium gas stream is expected to about
10 to 50 PPM. Activated charcoals are to be used to adsorb impure gases from cold helium gas at 20K
and 80K at 14v bar. The nominal flow rate of helium is 100gm/sec which will pass through thee purifier
bed. These single bed type purifier will be designed to condense the amount of impurities that are
expected to reach the cold box in the operation period of one week after which it can be purged and make
ready for next operation. The size of LHe dewar is 1500 Ltr storage capacity. The maximum quantity of
impurity to be removed from the helium gas will depend on the equivalent quantity of helium gas
required to to make 1500 Ltrs of LHe in operation. At the outlet of the 20K purifier, the total impurity
should be 1PPM. At the downstream of the adsorber bed, fine filters of 10 micron pore size should be
placed to trap the charcoal dust which can come sometime through the helium stream. This purifier will
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be a part of the indigenous helium development project. In this context, this work also involves the
manufacturing, assembly, test, repair aspect of these purifiers.
INTRODUCTION: Helium, the second most abundant element in the universe. Helium makes up about
0.0005% of the earth's atmosphere. This trace amount of helium is not gravitationally bound to the earth
and is constantly lost to space. The earth's atmospheric helium is replaced by the decay of radioactive
elements in the earth's crust. Alpha decay, one type of radioactive decay, produces particles called alpha
particles. An alpha particle can become a helium atom once it captures two electrons from its
surroundings. This newly formed helium can eventually work its way to the atmosphere through cracks in
the crust.Helium due to its unique properties like low boiling point, low density, low solubility, high
thermal conductivity and inertness is used in numerous applications like space research, cryogenics
industry,superconducting magnet, inert gas arc welding , leak detection, controlled atmosphere, quantum
mechanics.
LIQUID HELIUM: Kamerlingh Onnes worked for many years to liquefy the element which persisted as a
gas to the lowest temperature. Using liquid air to produce liquid hydrogen and then the hydrogen to jacket
the liquefaction apparatus, he produced about 60 cubic centimeters of liquid helium on July 10, 1908. Its
boiling point was found to be 4.2 K. Onnes received the Nobel Prize in 1913 for his low temperature
work leading to this achievement.
When helium is cooled to a critical temperature of 2.17 K (called its lambda point), a remarkable
discontinuity in heat capacity occurs, the liquid density drops, and a fraction of the liquid becomes a zero
viscosity "superfluid". Super-fluidity arises from the fraction of helium atoms which has condensed to the
lowest possible energy. A remarkable transition occurs in the properties of liquid helium at the
temperature2.17K, called the "lambda point" for helium. Part of the liquid becomes a "superfluid", a zero
viscosity fluid which will move rapidly through any pore in the apparatus. Another remarkable
characteristic of the superfluid is its very high heat conductivity, 30 times that of copper. These are the
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properties that make liquid helium very important in the study of superconductivity and for the
applications of superconducting magnets
HELIUM LIQUEFIER AT IPR: The process instrumentation diagram of the proposed indigenous
HRL is given below.

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LITERATURE REVIEW: The helium stream before entering into the cold box of the HRL passes
through an external purification unit. Though sufficient precaution is taken, still, in the process of gas
transfer and some other processes the helium stream gets contaminated and impurity level sometimes
goes up to 500 PPM. Though the impurity is in PPM range it can cause damage to cold box by
condensing or choking in the pipe lines,leading to damage the turbine blades and inefficient
liquefaction. These impurities mainly consists of gases present in the air, like
N
2
,O
2,
Ar,H
2
,H
2
O,CO,CO
2
and the traces of Ne. Hydrocarbons of the lubricating oil can also be
sources of H
2
.
These contaminants comes due to various reasons like when the isolated equipment bled down to
atmospheric pressure, the barometric pressure changes throughout the day which causes changes in
pressure in piping. The bed is not purged of contamination during installation. During maintenance oil in
the pipes exposed to air has an affinity to attract contamination. The make up
of lost helium also brings inbuilt impurity.

The cold box of the HRL contains two purification units placed at 80K and 20K respectively .The 80K
purification unit is to purify impurities like N
2
,O
2,
Ar as these impurities condense below the boiling point
temperature of liquid nitrogen. The 20K purifier unit is to purify H
2
and traces of Neon present. The
Hydrogen impurity mainly comes from the dissociation of hydrocarbons from the compressor oil.
Each time the cycle runs hydrogen in dissociates from the compressor oil and comes into the system
with helium stream. As the amount of neon present is very less and its boiling point temperature is
much less than 20K it is of less concern for purification. This 20K purifier mainly deals with removing
hydrogen impurity .The mechanism used in purification is adsorption.


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ADSORPTION: Adsorption has been defined as operation that uses surface forces on solid bodies called
adsorbents, to achieve the concentration of volatile materials. Adsorption differs from absorption that
in which a fluid (the adsorbate) permeates or is dissolved by a liquid or solid (the absorbent). Note that
adsorption is a surface-based process while absorption involves the whole volume of the material.

PRESSURE SWING ADSORPTION: Pressure swing adsorption (PSA) is a technology used to separate
some gas species from a mixture of gases under pressure according to the species' molecular
characteristics and affinity for an adsorbent material. It operates at near-ambient temperatures and differs
significantly from cryogenic distillation techniques of gas separation. Special absorptive materials
(e.g., zeolites) are used as a molecular sieve, preferentially adsorbing the target gas species at high
pressure. The process then swings to low pressure to desorb the adsorbed material.

TEMPERATURE SWING ADSORPTION: Temperature swing adsorption (TSA) is another technique
use for regenerating a bed of adsorbent that is loaded with the targeted impurity gas. Whereas pressure
swing adsorption (PSA) uses changes in pressure to release adsorbed gas, TSA modulates or swings
temperature to drive off the adsorbed gas.
TSA technology began commercially in the 1960's and continues today for drying compressed air and
natural gas as well as other purification applications such as carbon dioxide stripping from air. TSA
exploits the capacity of certain adsorbent materials, such as activated alumina, silica gel and zeolites, to
adsorb gases at moderate temperatures (40C, 100F) and later release them when the temperature rises
above 120C (250F). TSA can separate a single gas from a mixture of gases. A typical TSA system
employs a cyclic process where a number of connected vessels containing adsorbent undergo successive
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loading with the target gas followed by heating and cooling steps to produce a continuous stream of dried
or purified product gas.

CRYOGENIC ADSORPTION MECHANISM: Cryogenic adsorption is based on the physical adsorption,
using different adsorbents .Theses adsorbents have a porous and divided material, with a specific area as
high as 200 to 1200 m2/g. The physical adsorption is a reversible process (adsorption / desorption) and an
exothermic process, where the adsorption heat is similar to the latent heat. The adsorption often consists
of three processes, i.e. the outside diffusion, the inside diffusion and the intramural adhesion. These
physical processes occur quickly, and the phase balance among different components will be achieved
instantly. According to adsorption thermodynamics, if the absorbent and the adsorbate are both at uniform
temperature and pressure, the adsorbate's quantity is dominated by the adsorbed gas pressure and the
adsorption equilibrium temperature. Adsorbate gases flows through the absorbent bed, the adsorbent first
forms a mass transfer area. After this mass transfer area is formed, as long as the gas flow rate is uniform,
itslength also increases uniformly along the flow direction when more impurities areadsorbed. In the
dynamic adsorption process, the adsorbents bed is divided into three sections, the saturated adsorbent
zone, the adsorption mass transfer zone and the clean adsorbent zone. The adsorbent used here is
activated charcoal.
ADSORBENT MATERIALS: Adsorbents are used usually in the form of spherical pellets, rods,
moldings, or monoliths with hydrodynamic diameters between 0.5 and 10 mm. They must have
high abrasion resistance, high thermal stability and small pore diameters, which results in higher
exposed surface area and hence high surface capacity for adsorption. The adsorbents must also
have a distinct pore structure that enables fast transport of the gaseous vapors. Various
adsorbents are listed below.
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Activated carbon: Activated carbon is a highly porous, amorphous solid consisting of micro
crystallites with a graphite lattice, usually prepared in small pellets or a powder. It is non-polar
and cheap. One of its main drawbacks is that it reacts with oxygen at moderate temperatures
(over 300 C). Activated carbon can be manufactured from carbonaceous material, including
coal (bituminous, subbituminous, and lignite), peat, wood, or nutshells (e.g., coconut). The
manufacturing process consists of two phases, carbonization and activation. The carbonization
process includes drying and then heating to separate by-products, including tars and other
hydrocarbons from the raw material, as well as to drive off any gases generated. The process is
completed by heating the material over 400 C (750 F) in an oxygen-free atmosphere that
cannot support combustion. The carbonized particles are then "activated" by exposing them to an
oxidizing agent, usually steam or carbon dioxide at high temperature. This agent burns off the
pore blocking structures created during the carbonization phase and so, they develop a porous,
three-dimensional graphite lattice structure. The size of the pores developed during activation is
a function of the time that they spend in this stage. Longer exposure times result in larger pore
sizes. The most popular aqueous phase carbons are bituminous based because of their hardness,
abrasion resistance, pore size distribution, and low cost, but their effectiveness needs to be tested
in each application to determine the optimal product.Zeolites: Zeolites are natural or synthetic
crystalline aluminosilicates, which have a repeating pore network and release water at high
temperature. Zeolites are polar in nature.They are manufactured by hydrothermal synthesis of
sodium aluminosilicate or another silica source in an autoclave followed by ion exchange with
certain cations (Na
+
, Li
+
, Ca
2+
, K
+
, NH
4
+
). The channel diameter of zeolite cages usually ranges
from 2 to 9 (200 to 900 pm). The ion exchange process is followed by drying of the crystals,
which can be pelletized with a binder to form macro porous pellets. Zeolites are applied in
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drying of process air, CO
2
removal from natural gas, CO removal from reforming gas, air
separation, catalytic cracking, and catalytic synthesis and reforming.

SAMPLE CALCULATION:
The operating pressure=14 BAR
The operating temperature=20K
Amount of impurity=10PPM
Liquid Helium capacity=1500ltrs
Volume of effluent required=1500*0.7542
=1131.3m
3
/day
Amount of impurity=1131.3*10*10
-6

=0.011313m
3
/day
Calculating for 30days=30*0.01131
=0.33939m
3
P/Psat at 14 bars operating pressure =0.00014 bars
It is found that at this partial pressure of 0.00014 bars the volume of impurity adsorbed per m
2
of
adsorbent area is 0.31cm
3
/m
2

Then for a sample of 1100m
2
/gm surface area the amount adsorbed will be 341cm
3
/gm

Amount of mass required to adsorb the impurity(M)=IMPURITY/(Vad*Sarea)(in grams)
= 995.2785924gm
For 50PPM impurity and 30days operation the mass of adsorbent required will be=1.69695m
3

Amount of mass required to adsorb the impurity(M)=IMPURITY/(Vad*Sarea)(in grams)
= 4976.392962gm
Now taking a margin of 70% the amount of adsorbent required will be=1.7*4976.39gm
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=8.45Kg

Excel code calculation for Mass of adsorbent for 10ppm impurity.

SURFACEarea(
m2/gm) Vad(cm3/m2)
Vad*SURFACEarea(cm3/g
m)
M=IMPURITY/(Vad*Sa
rea)(in grams)
M(for 30
days)(in gm)
100 0.31 31 364.9354839 10948.06452
150 0.31 46.5 243.2903226 7298.709677
200 0.31 62 182.4677419 5474.032258
250 0.31 77.5 145.9741935 4379.225806
300 0.31 93 121.6451613 3649.354839
350 0.31 108.5 104.2672811 3128.018433
400 0.31 124 91.23387097 2737.016129
450 0.31 139.5 81.09677419 2432.903226
500 0.31 155 72.98709677 2189.612903
600 0.31 186 60.82258065 1824.677419
700 0.31 217 52.13364055 1564.009217
800 0.31 248 45.61693548 1368.508065
900 0.31 279 40.5483871 1216.451613
1000 0.31 310 36.49354839 1094.806452
1100 0.31 341 33.17595308 995.2785924
1200 0.31 372 30.41129032 912.3387097
1300 0.31 403 28.0719603 842.1588089









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For 50ppm and 30 days operation:
M=IMPURITY/(Vad*Sarea)(in
grams 50PPM)

1824.677419
1216.451613
912.3387097
729.8709677
608.2258065
521.3364055
456.1693548
405.483871
364.9354839
304.1129032
260.6682028
228.0846774
202.7419355
182.4677419
165.8797654
152.0564516
140.3598015
130.3341014
121.6451613
114.0423387
M(for 30 days)(in gm)

54740.32258
36493.54839
27370.16129
21896.12903
18246.77419
15640.09217
13685.08065
12164.51613
10948.06452
9123.387097
7820.046083
6842.540323
6082.258065
5474.032258
4976.392962
4561.693548
4210.794045
3910.023041
3649.354839
3421.270161

Calculation for the size of the container:
Mass of adsorbent=8.45kg
Density of charcoal=550Kg/m
3

Volume =8.45/550=0.01538m
3

Taking L=2.5d
d=0.198m
L=2.5*0.198
=0.49m
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The operating pressure =14bar=14*10^5N/m
2

Calculating the minimum thickness of the shell:
S
w
=o.25*ultimate strength of ss304l=121.25MPa
e
w
=welding efficiency=1
t
min=
P*d/(2(S
a
*e
W
*-o.6P))
=0.001m
Outside diameter =0.198+2*0.001
=0.002m
But due to safety reasons shell assuming thickness 0.025m
PRESSURE DROP CALCULATION:
The Ergun equation is commonly employed is given below:
F
p
= (P/L)*( D
p
/

U
2
)*(
3
/(1- ))
F
p
= friction factor
DENSITY ( 33.430Kg/m
2
at 14 bar and 20k
Viscosity ()=4.0845*10^-6 Pa-sec at 14 bar and 20K
Viscosity () =4.0845*10^-6 Pa-sec
Reynolds no (R
e
) = (D
p
U
Mass flow rat of the system=100gm/sec
=0.1kg/sec
Volume flow rate of the system=M
.
/
=0.1/33.430
=2.99*10^-3 m
3
/sec
Calculating the pressure drop keeping the length of bed and superficial velocity constant and varying the
properties of charcoal samples.
Calculating for sample1:
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Dp =equivalent spherical diameter of the carbon
=0.003m

Void porosity () =0.6
Superficial velocity (U) =V
.
/area of cross-section of the shell
=0.09723m/sec
Reynolds no (R
e
)=(D
p
U
=5968.4
From Ergun equation friction-factor ( F
p
)= 1.75+150/ R
e

=1.775

Pressure drop across the bed:
F
p
= (P/L)*( D
p
/

U
2
)*(
3
/(1- ))
P = 166.22Pa
= 1.662mbar
Calculating for sample 2:
Dp = equivalent spherical diameter of the carbon particle
=0.0007m

Void porosity () =0.4
Superficial velocity (U) =V
.
/area of cross-section of the shell
=0.09723m/sec
Reynolds no (R
e
) = (D
p
U
=927.724
From Ergun equation friction-factor ( F
p
) = 1.75+150/ R
e

=1.911
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Pressure drop across the bed:
F
p
= (P/L)*( D
p
/

U
2
)*(
3
/(1- ))
P = 3944.66pa
= 39.446mbar
The change in pressure drop in these two samples suggest that the pressure drop is a function of many
parameters such as( void porosity ,superficial velocity, length of the bed, equivalent spherical diameter of
charcoal beads), it still need some sort of optimization to get an optimum design.
Future Work Proposed:
Calculating details of the experimental set up with percentage level impurity. Designing of the
experimental set up for Helium purification .Predicting the mass transfer zone and break through Curve
for helium purification.

Conclusion:
Adsorbent mass required for Helium purification is Calculated , the container of the vessel is also
designed. Pressure drop is calculated for two samples. Since the pressure drop is a function of many
parameters it still needs some sort of optimization to get an optimum design.
REFERENCES:
[1] Barry Crittenden & W John Thomas, Adsorption Technology & Design, Elsevier Science &
Technology Books, April 1998.
[2] Douglas M. Ruthven, Principles Of Adsorption and Adsorption Processes, John Wiley & Sons,
1984.
[3] Roopchand Bansal & Meenakshi Goyal, Activated Carbon Adsorption, CRC Press, 2005.
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[4] Robert E. Treybal, Mass-Transfer Operations, third edition, McGraw-Hill publ[ications, 1981.
[5] Ralph T. Yang, Adsorbents: Fundamentals and Applications, John Wiley & Sons Publication, 2003.
[6] M. Douglas Levan, Giorgio Carta, Perrys Chemical Engineers Handbook, 8
th
edition, McGraw-
Hill Publication, 2008.
[7] Mccabe, Smith, Harriot, Unit Operations of Chemical Engineering, 6
th
edition, Mc-Graw Hill
Publication, 2001.
[8] Randall F. Barron, Cryogenic Systems, second edition, Clarendon Press, Oxford, 1985.
[10]High pressure adsorption isotherms of Neon, Hydrogen and Helium at 76k,A.J Kidnay, M.J Hiza
[11] Hydrogen adsorption on graphite and in carbon slit pores from path integral simulations By QINYU
WANG and J. KARL JOHNSON ,Department of Chemical and Petroleum Engineering, University of
Pittsburgh , Pittsburgh, PA 15261, USA, MOLECULAR PHYSICS, 1998, VOL. 95, NO. 2, 299 309