Article

pubs.acs.org/jced

Solubility of N2O in and Density and Viscosity of Aqueous Solutions

of 1,4-Butanediamine, 2(Diethylamino)-ethanol, and Their Mixtures
from (298.15 to 333.15) K
Zhicheng Xu, Shujuan Wang,* and Changhe Chen
Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Beijing Key Laboratory for CO2 Utilization
and Reduction Technology, Department of Thermal Engineering, Tsinghua University, Beijing 100084, China
ABSTRACT: Densities of and N2O solubilities in aqueous
solutions of 1,4-butanediamine (BDA), 2-(diethylamino)ethanol (DEEA), and their aqueous mixtures were measured
at (298.15, 313.15, and 333.15) K, and viscosities were measured at
(298.15, 303.15, 313.15, 323.15, and 333.15) K. The experiments
cover the mole fraction ranges (1.9514.3 mol %) BDA,
(2.0119.3 mol %) DEEA, and (3.6316.7 mol %) BDA +
(2.6222.2 mol %) DEEA in the blended solutions. The
results were compared with available data in the literature. The
experimental density and viscosity data were correlated using two semi empirical correlations in the literature as functions of
temperature and concentration of BDA and DEEA.

INTRODUCTION
Absorption of CO2 with amine-based absorbents is an
established and proven technology.1 Many solvents, such as
monoethanolamine (MEA), methyldiethanolamine (MDEA),
diethanolamine (DEA), and piperazine (PZ), have been applied
to capture CO2.24 However, this process always requires lots of
energy during solvent regeneration. Recent years, the novel
process of biphasic system DMX and lipophilic solvents were
proposed with the energy consumption of DMX system being
estimated to be 2.3 GJ/t CO2.5,6 Dimethylcyclohexylamine (DMCA),
dipropylamine (DPA), and DPA and DMCA blend, 3(methylamino)propylamine (MAPA) and DEEA blend and some
other unspecied amines in the literatures were studied for the
biphasic system.711
The previous researches have investigated CO2 absorption by
some potential biphasic solvents. The mixture of 8.75 mol %
BDA and 17.5 mol % DEEA (2 M BDA+4 M DEEA) was found
to be a potential biphasic solvent and has 46 % higher cyclic
loading, 48 % higher cyclic capacity, and 11 % higher cyclic
eciency than 30 mass % MEA. The phase separation of the
solution after CO2 absorption was due to the fast reaction rate of
CO2 with BDA and the limited solubility of DEEA in the reaction
products of BDA and CO2.1214
As one of the most important issues in evaluating a solvent,
kinetics parameters are typically derived from the experiments
based on mass transfer process, and the data of physical
diusivity and solubility of CO2 in aqueous solvents solutions are
required. However, due to the chemical reactions between CO2
and amine, these properties are not possible to be measured
directly.15 It is suggested that using N2O analogy to estimate
the aforementioned physicochemical properties, since N2O
resembles CO2 in molecular volume, conguration and electronic
structure, and it is a nonreactive gas in amine conditions,1618 as
2013 American Chemical Society

shown in eq 1. Moreover, density and viscosity of aqueous solvents

are also essential for the calculation of other physicochemical
properties such as diusivity, gas solubility, and reaction rate
constants.
HCO H O
2
2
HN O Am
HCO2 Am =
2
HN2O H2O

(1)

BDA has been widely investigated by evaluating the eect of

chain length on the absorption and desorption capacity of
biamine and by measuring the vapor liquid equilibrium of pure
BDA.1922 However, so far as we know, there is still no literature
reporting the solubility of N2O in and density and viscosity of
BDA aqueous solution.
DEEA is usually blended with other activators (for example,
piperazine) to absorb CO2 because of its low reaction rate. The
densities of aqueous DEEA solutions were presented by
Barbas et al. and Lebrette et al.,23,24 which did not include the
concentrations needed in our kinetics study. The viscosities of
aqueous DEEA solutions were measured by Maham et al. and
Littel et al.25,26 The N2O or CO2 physical solubility in aqueous
DEEA solution was obtained by Littel et al., Vaidya, and Li
et al.,2629 which just covered limited concentrations around
4.54 mol %. The solubility of N2O in and density and viscosity of
BDA/DEEA mixtures have not been presented until now.
In the present work, N2O solubilities in and densities of aqueous
solutions of (1.9514.3 mol %) BDA, (2.0119.3 mol %) DEEA,
and their aqueous mixtures were measured at (298.15, 313.15, and
333.15) K, with viscosities measured at (298.15, 303.15, 313.15,
Received: December 27, 2012
Accepted: May 15, 2013
Published: May 24, 2013
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323.15, and 333.15) K. The results were compared with available

data in the literatures. The experimental data on density and
viscosity were correlated using two semi empirical correlations in the
literature as functions of temperature and concentrations of BDA
and DEEA.

EXPERIMENTAL SECTION
BDA ( 98 wt % pure) and DEEA ( 99 wt % pure) were from
Aladdin Reagent Company. The BDA and DEEA structures are
shown below.

Distilled water was used for preparing experimental solutions.

The BDA and DEEA concentrations were determined by
titration against 2 N H2SO4 using a Metrohm 809 Titrando auto
titrator. The N2O gas (99 vol % pure) was supplied by Beijing
Huayuan Gas Company.
Density and Viscosity. In this work, the densities of aqueous
solutions were measured by National Institute of Metrology
(NIM) of China, strictly following the JJG 1058-2010 verication
regulation of laboratory oscillation-type liquid density meters
issued by General Administration of Quality Supervision,
Inspection and Quarantine of China (AQSIQ), using a
DMA5000 density meter. NIM is Chinas highest research
center of metrology and the national technical center of legal
metrology. The result of every point was the average value of six
repeated trials.
The viscosities of aqueous solutions were measured by a A&D
SV-10 viscometer, with a measurement range of 0.31000
mPas. The total accuracy of viscosity given by the manufacturer
is 1 %. Calibration of viscometer was done by measuring the
viscosity of Standard Liquid GBW13601 (1203) and GBW13603
(1203) produced by NIM and approved by AQSIQ. The data for
the calibration are given in Table 1.

Figure 1. Experimental setup of N2O solubility.

The amount of solvent added (around half of reactor) into the

reactor was calculated by measuring the weight of solvent before
and after the transference. After the solution reached vapor
liquid equilibrium at set temperature, the pressure inside of the
reactor, P1,N2O, was recorded. The temperature of the reactor was
controlled by the circulating oil bath with an uncertainty of
0.1 K. Then N2O gas was added to the reactor by shortly
opening valve No. 5 linking the reactor and the vessel. Considering
that the open period for the reactor after the solution added was
very short and the good airtightness of the reactor, the vapored
amount of the solvent should be very small and can be neglected.
Equilibrium was then established after 615 h (depending on
temperature) with an agitation speed of 450 r/min. The reactor
and vessel pressure were recorded by two pressure transducers
(Druck PTX 7515 with uncertainty 0.2 % of full scale (200 kPa)).
Two K-type thermocouples recorded temperatures in the reactor
and in the vessel, respectively, with an uncertainty of 0.1 K.
The amount added of N2O, nNadded
, mol, was calculated from the
2O
pressure dierence of the gas supply vessel before and after
feeding N2O as

Table 1. Viscosities of Standard Solutions for Calibration,

293.15 K, 1 atm (1.01325105 Pa)

n Nadded
=
2O

viscosity (mPas)
standard

measurement

ref

deviation

GBW13601(1203)
GBW13603(1203)

1.84
8.80

1.8388
8.793

0.07 %
0.03 %

VV PV1 PV2

R TV1z1 TV2z 2

(2)

where PV1 and PV2 are the pressure of the vessel before and after
feeding, Pa; TV1 and TV2 are the temperature of the vessel before
and after feeding, K; z1, z2 represent the compressibility factor of
gas before and after the feeding; R is universal gas constant,
8.3145 J(molK)1. The compressibility factor was calculated
using the PengRobinson equation of state.
The amount of N2O in the gas phase of the reactor ngN2O can be
calculated by

It can be seen that viscosities from the measurements agree

very well with the reference values for the standard liquid.
Solubility of N2O. The N2O solubility apparatus consists of a
jacketed stirred glass reactor and a stainless steel gas holding
vessel, as shown in Figure 1. Before experiment, the volume of
the gas holding vessel was measured by lling it up with water and
calculating the water volume. Then the total volume of the
reactor and the auxiliary pipe linking the reactor and valves no.
36 were measured by adding into it a known amount of N2O
from the holding vessel. The added N2O amount was calculated
by the amount dierence in the gas holding vessel before and
after adding N2O into reactor. The results show that the volume
of vessel, VV, was 2.186103 m3, while that of the reactor and the
auxiliary, VR, was 5.628104 m3.
The reactor was rst vacuumed until the pressure was less than
1 kPa, and then the solution was sucked into it through valve no. 3.

n Ng 2O =

PN2O(VR VS)
z N2ORTR

(3)

where TR is the reactor temperature after reaching equilibrium,

K, and z is the compressibility factor of N2O after reaching
equilibrium. VS is the volume of added solvent, which is the
quotient of added solution amount and density, m3. PN2O is the
N2O partial pressure and calculated by eq 4, Pa.
PN2O = P1,N2O P2,N2O
(4)
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Table 2. Measured N2O Solubilities (Mass Fraction w, kg/kg) in Water and 30 Mass % MEA, 293.15 to 333.15 K in This Work
T (K)

293.15

water

PN2O (kPa)

MEA

w (%)
PN2O (kPa)

111.0
0.1338

w (%)
a

298.15

303.15

150.9

123.6

0.1677
141.7

0.1219

0.1402

313.15
150.3
0.1180
155.5
0.1195

323.15
142.7
0.0952

333.15
181.7
0.0829
142.0
0.0736

The standard uncertainty of w measurement is 2 %.

where P2,N2O is the total pressure of reactor after reaching

equilibrium, Pa. The N2O amount in the liquid phase, nNlN2O, can
then be expressed as the amount dierence between added N2O
and N2O in the gas phase by
n Nl 2O = n Nadded
n Ng 2O
2O

(5)

The N2O concentration in the liquid phase, CN2O, can be

calculated by
C N2O =

n Nl 2O
VS

(6)

The solubility of N2O at dierent pressures and temperatures

have been expressed as mass fraction w (kg/kg) in this paper.
Then the N2O solubility was expressed by a Henrys law constant
HN2O according to eq 7 in this paper.
PN2O = HN2OC Nl 2O

Figure 3. N2O solubility HN2O in 30 mass % MEA: this work comparing

with literature data.3537

(7)

The units of CN2O and HN2O are molm3 and kPam3kmol1.

All operating conditions, including temperature and pressure,
were recorded using Kingview (6.5.2 version) software.
Calibrations were done by measuring the solubility of N2O in
water and in 30 mass % MEA at dierent temperatures from
(293.15 to 333.15) K and comparing the data with the literature.
The data of N2O pressure in gas phase and concentration in
liquid phase are shown in Table 2, whereas the comparisons of
Henrys law constant HN2O with several literature references are
shown in Figures 2 and 3.15,30,3337

It can be seen that the solubility of N2O in water and in

30 mass % MEA measured by this work agree very well with
the literature data. The uncertainty is within 3 % when less
than 313.15 K, whereas the dierences were about 7 % at
(323.15 and 333.15) K when compared with the data of
Versteeg and van Swaaij.30

RESULTS AND DISCUSSION

Density. The measured densities for the aqueous solutions of
BDA, DEEA, and BDA/DEEA blends are presented in Table 3
and Figures 4 and 5.

Figure 2. N2O solubility HN2O in water: this work comparing with

literature data.15,30,33,34

Figure 4. Densities of aqueous BDA solutions measured and calculated

by this work.
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Table 3. Densities of Aqueous BDA (x1), DEEA (x2), and BDA/DEEA Blended Solutions at (298.15, 313.15, and 333.15) K and
1 atm (1.01325105 Pa)
density, a103 (kg/m3)
10x1 (mol/mol)

T/K

032

0.1952

0.4244

298.15
313.15
333.15

0.99704
0.99222
0.98320

0.992346
0.986497
0.976433

0.988532
0.981237
0.969713

T/K

032

0.2012

0.4547

298.15
313.15
333.15

0.99704
0.99222
0.98320

0.993744
0.987552
0.976860

0.6965
0.985772
0.976817
0.963518
10x2 (mol/mol)
0.7875

0.990151
0.983322
0.981577
0.972648
0.968366
0.957191
10x1/10x2(mol/mol)

1.0253

1.4336

0.982813
0.972197
0.957323

0.978544
0.966791
0.950667

1.2520

1.9329

0.971858
0.959656
0.942334

0.961569
0.948632
0.930379

T/K

0.3629/1.4516

0.8749/1.7499

1.6703/2.2270

0.6799/1.0198

0.5618/0.5618

0.8712/0.9376

298.15
313.15
333.15

0.962903
0.950135
0.932259

0.948513
0.935423
0.917224

0.930513
0.917399
0.899304

0.967362
0.954889
0.937515

0.979531
0.968135
0.952165

0.973321
0.961226
0.944402

The standard uncertainty of measurement is 0.01 %.

Figure 5. Densities of aqueous DEEA solutions measured and calculated by this work and compared with literature data.23,24

Table 4. Correlation Parameters, AADs, SSE, and R2 for Densities of BDA, DEEA, and BDA/DEEA Blended Solutions
k1
BDA
DEEA
BDA+DEEA
a

0.5635
0.5260
0.9686

k2
64.004
2920.0
142.11

k3

k4

k5

0.8865
0.01838
4.9035

1.495810
1.5151104
1.9634105
4

273.87
307.54
346.75

AADa

k6
0.65421
37.2233
0.11514

1.4610
1.56103
1.77103

SSEb

R2c
5

4.5910
6.76105
6.58105

0.9829
0.9889
0.9917

AAD = (1/N)i N= 1((|cal,i exp,i|)/exp,i). bSSE = i N= 1(cal,i exp,i)2. cThe squared correlation coecients.

Optimization method in the 1STOPT software produced by

7D-Soft High Technology Inc.

For DEEA solutions, the deviations are less than 0.3 % when
compared with Barbas et al. and Lebrette et al. under the same
conditions,23,24 as shown in Figure 5.
The densities of the binary and ternary mixtures decrease
with increasing mole fractions of BDA and DEEA and
temperature in the mixture. The experimental density data for
the binary and ternary mixtures were tted as a function of
temperature and concentration of amine using the equation
proposed by Liu et al.,31 as shown in eq 8. The correlation
parameters were tted for lowest average absolute deviation
(AAD) using LevenbergMarquardt and Universal Global

BDA + DEEA ( 103(kgm3)

k
k
= k1 + 2 (x BDA + k 3x DEEA ) + 42

T
T
k5

exp + k6(x BDA + k 3x DEEA )

T

(8)

where is the density of the mixture, T is the temperature, and x

is the mole fraction of BDA or DEEA. k1 to k6 are the correlation
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Table 5. Viscosities of Aqueous BDA (x1), DEEA (x2), and BDA/DEEA Blended Solutions from (298.15 to 333.15) K and 1 atm
(1.01325105 Pa)
viscosity a (mPas)
10x1 (mol/mol)
T/K

032

0.1952

0.4244

0.6965

1.0253

1.4336

298.15
303.15
313.15
323.15
333.15

0.89
0.80
0.65
0.55
0.48

1.86
1.23
0.98
0.80
0.63

2.64
1.83
1.39
1.10
0.90

3.50
2.51
1.85
1.40
1.06

5.53
3.65
2.57
1.86
1.37

7.92
4.87
3.29
2.29
1.62

T/K

32

0.7875

1.2520

1.9329

5.57
3.61
2.42
1.72
1.24

8.00
5.75
3.76
2.60
1.87

11.61
8.05
5.27
3.69
2.53

10x2 (mol/mol)
0

298.15
303.15
313.15
323.15
333.15

0.2012

0.4547

0.89
0.80
0.65
0.55
0.48

2.16
1.40
1.12
0.94
0.75

3.62
2.34
1.66
1.32
1.03
10x1/10x2(mol/mol)

T/K

0.3629/1.4516

0.8749/1.7499

1.6703/2.2270

0.6799/1.0198

0.5618/0.5618

0.8712/0.9376

298.15
303.15
313.15
323.15
333.15

13.50
8.42
5.42
3.67
2.47

16.48
9.86
6.13
3.99
2.61

15.28
9.10
6.00
3.93
2.54

11.97
7.97
5.18
3.53
2.43

9.12
5.26
3.70
2.64
1.89

10.05
6.76
4.54
3.21
2.30

The standard uncertainty of measurement is 6 %

Figure 6. Viscosities of aqueous DEEA solutions measured and calculated by this work and compared with literature data.25

Table 6. Correlation Parameters, AADs, SSE, and R2 for Viscosities of BDA, DEEA, and BDA/DEEA Blended Solutions
BDA
DEEA
BDA+DEEA
a

k1

k2

k3

k4

k5

k6

AADa

SSEb

R2c

1290
4486
975.1

0.7115
2.4061
0.9854

2.0806107
1.6338106
3.3713107

4011.71
4324.48
4032.22

1.238106
1.31106
1.40106

17.178
1.1926
119.26

0.1091
0.08617
0.09759

1.8350
1.4616
13.424

0.9748
0.9919
0.9726

AAD = (1/N)i N= 1((|cal,i exp,i|)/exp,i). bSSE = i N= 1(cal,i exp,i)2. cThe squared correlation coecients.

parameters. k3 is especially used to describe the interaction

between the BDA and DEEA in the mixed solution. The
calculated parameters k, the average absolute deviations
(AADs), the residual sum of squares (SSEs) and the squared
correlation coecients (R2) are listed in Table 4.

As shown in Figures 4 and 5, the calculated densities from the

correlation eq 8 are in good agreement with the experimental
data of this work and the data in literature. The R2 of the
correlation for BDA, DEEA, and BDA/DEEA blended solutions
are 0.9829, 0.9889, and 0.9917, respectively.
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where is the mixture viscosity, T is the temperature, x is the mole

fraction of BDA or DEEA, and k1 to k6 are the correlation parameters.
k2 is especially used to describe the interaction between BDA and
DEEA. The calculated parameters and the average absolute
deviations (AADs), the residual sum of squares (SSEs) and the
squared correlation coecients (R2) are listed in Table 6.
As shown in Figures 6 and 7, the calculated viscosities from
correlation eq 9 agree well with the experimental data in this
paper and in the literature. The R2 of the correlation for BDA,
DEEA, and BDA/DEEA blended solutions are 0.9748, 0.9919,
and 0.9726, respectively.
Solubility of N2O. The solubility of N2O dened by eq 7,
HN2O, in BDA, DEEA, and BDA/DEEA solutions were presented in
Figures 8 and 9, and the N2O solubility (mass fraction w, kg/kg)
were listed in Table 7.
Figure 10 compares the CO2 solubility data of DEEA
calculated by N2O solubility data using eq 1 in this work and
the data in the literatures2629 under the same conditions. Also,

Viscosity. The measurements of viscosities in this work also

comprise the aqueous solutions of BDA, DEEA, and the BDA/
DEEA blends. The experimental data are presented in Table 5 and
Figures 6 and 7.
For the DEEA solutions, the experimental data of this work are
compared with literature data25 in Figure 6 for the same conditions.
The viscosities of the binary and ternary mixtures increase with
increasing mole fraction of BDA or DEEA and decreasing
temperature. The experimental viscosity data for the binary and
ternary mixtures were also tted by Lius equation as a function of
temperature and concentrations of BDA and DEEA,31 shown as eq 9.
The correlation method was the same as for the density data.
BDA + DEEA (mPa s)

(x
(x
+ k 2x DEEA )
+ k 2x DEEA)2

= 1 + k1 BDA
+ k 3 BDA
T
T2

k
exp 4 + 52 + k6(x BDA + k 2x DEEA )2
T

(9)

Figure 7. Viscosities of aqueous BDA solutions measured and calculated

by this work.
Figure 9. N2O solubility HN2O in aqueous BDA/DEEA blended
solutions at (298.15, 313.15, and 333.15) K.

Figure 10. CO2 physical solubility HCO2 in aqueous DEEA solutions at

(298.15, 313.15, and 333.15) K in this work and compared with
literature.2729

Figure 8. N2O solubility HN2O in aqueous BDA and DEEA solutions at

(298.15, 313.15, and 333.15) K.
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Table 7. Solubility of N2O (Mass Fraction w, kg/kg) in Aqueous BDA (x1), DEEA (x2), and BDA/DEEA Blended Solutions at
(298.15, 313.15, and 333.15) K
10x1 (mol/mol)
0

0.1952

T/K

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

298.15
313.15
333.15

150.90
150.30
181.70

0.1677
0.1180
0.0829

129.80
152.98
146.43

0.1468
0.1111
0.0882

133.50
145.50
146.50

0.2012

0.6965
w/%

PN2O/kPa

0.1358
143.20
0.1009
166.02
0.0868
145.00
10x2 (mol/mol)

0.4547

T/K

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

298.15
313.15
333.15

150.90
150.30
181.70

0.1677
0.1180
0.0829

133.10
156.60
170.19

0.1281
0.1130
0.1104

158.10
154.39
142.15

0.3629/1.4516

0.4244

0.8749/1.7499

1.0253
w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

0.1143
0.1001
0.0863

143.20
166.02
145.00

0.1030
0.1053
0.0791

155.40
138.81
158.00

0.1039
0.0831
0.0827

0.7875
w/%

PN2O/kPa

0.1566
131.70
0.1196
140.97
0.1025
141.63
10x1/10x2(mol/mol)

1.6703/2.2270

1.4336

1.2520

1.9329

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

0.1385
0.1273
0.1141

128.80
130.94
139.49

0.1638
0.1513
0.1501

125.40
124.68
114.77

0.1962
0.1797
0.1457

0.6799/1.0198

0.5618/0.5618

0.8712/0.9376

T/K

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

PN2O/kPa

w/%

298.15
313.15
333.15

126.30
107.40
135.00

0.1798
0.1343
0.1513

122.10
117.50
127.80

0.2022
0.1748
0.1765

115.90
107.40
119.70

0.2628
0.2077
0.1993

140.40
151.10
132.40

0.1548
0.1572
0.1282

141.20
150.30
135.20

0.1281
0.1255
0.1065

152.40
145.90
142.00

0.1788
0.1530
0.1360

The standard uncertainty of w measurement is 2 %.

Notes

the solubility data of 2.01 mol % DEEA at (313.15 and 333.15) K

were repeated in Figure 10, to further veries the good accuracy
and repeatability of the experiment system.
Figures 8 and 9 indicate that the N2O solubility of BDA is higher
than DEEA at all of the measured concentrations. The N2O
solubility in BDA solution increases with the increasing BDA
concentration, while that in DEEA solution decreases with the
increasing DEEA concentration. The N2O solubility in BDA/DEEA
mixture decreases with the increasing DEEA concentration in the
mixtures.

The authors declare no competing nancial interest.

(1) Rochelle, G. T. Amine Scrubbing for CO2 Capture. Science 2009,

325, 16521654.
(2) Bishnoi, S.; Rochelle, G. T. Absorption of carbon dioxide in
aqueous piperazine/ methyldiethanolamine. AIChE J. 2002, 48, 2788
2799.
(3) Derks, P. W. J.; Dijkstra, H. B. S.; Hogendoorn, J. A.; Versteeg, G. F.
Solubility of carbon dioxide in aqueous piperazine solutions. AIChE J.
2005, 51, 23112327.
(4) Rinker, E. B.; Ashour, S. S.; Sandall, O. C. Absorption of carbon
dioxide into aqueous blends of diethanolamine and methyldiethanolamine. Ind. Eng. Chem. Res. 2000, 39, 43464356.
(5) Raynal, L.; Alix, P.; Bouillon, P. A.; Gomez, A.; de Nailly, M. F.;
Jacquin, M.; Kittel, J.; di Lella, A.; Mougin, P.; Trapy, J. The DMX
process: An original solution for lowering the cost of post-combustion
carbon capture. Energy Procedia 2011, 4, 779786.
(6) Zhang, X. Studies on multiphase CO2 capture system [D]; University
of Dortmund: Dortmund, 2007.
(7) Zhang, J.; Agar, D. W.; Zhang, X.; Geuzebroek, F. CO2 absorption
in biphasic solvents with enhanced low temperature solvent
regeneration. Energy Procedia 2011, 4, 6774.
(8) Tan, Y. H. Study of CO2-absorption into thermomorphic lipophilic
amine solvents [D]; University of Dortmund: Dortmund, 2010.
(9) Rojey, A.; Cadours, R.; Carrette, P. L.; Boucot, P. Method of
deacidizing a gas by means of an absorbent solution with fractionated
regeneration through heating. United States Patent, US 2009/0199709
A1, 2009.
(10) Hu, L. Phase transitional absorption method. United States
Patent, 7541001, 2009.
(11) Bruder, P.; Svendsen, H. F. Solvent comparison for post
combustion CO2 capture. Paper presented at 1st Post Combustion
Capture Conference, Abu Dhabi, Kingdom of Saudi Arabia, May 1719,
2011.
(12) Xu, Z. C.; Wang, S. J.; Chen, C. H. CO2 Absorption by BDA/
DEEA Biphasic Solvents. J. Eng. Thermophys. 2012, accepted.
(13) Xu, Z. C.; Wang, S. J.; Chen, C. H. Experimental Study of CO2
absorption by MAPA, DEEA, BDA and BDA/DEEA mixtures. J.
Combust. Sci. Technol. 2013, 19, 103118.

CONCLUSION
Densities, viscosities, and solubilities of N2O in BDA, DEEA, and
BDA/DEEA aqueous solutions were measured with the amine
concentration of (1.9514.3 mol %) BDA, (2.0119.3 mol %)
DEEA, and (3.6316.7 mol %) BDA + (2.6222.2 mol %)
DEEA. The densities and N2O solubilities were measured at
(298.15, 313.15, and 333.15) K, whereas the viscosities were
obtained at (298.15, 303.15, 313.15, 323.15, and 333.15) K. The
measurement results agreed well with the literature data.
The densities and viscosities of the binary and ternary mixtures
were correlated by two semiempirical correlations in the literature.
The correlated results are in good agreement with the experimental
and literature data within the range of temperature and amine
concentration in this work. The N2O solubility in BDA solution
increases with the increasing BDA concentration, whereas that in
DEEA solution decreases with the increasing DEEA concentration.
The N2O solubility in BDA/DEEA mixture decreases with the
increasing DEEA concentration in the mixture.

REFERENCES

AUTHOR INFORMATION

Corresponding Author

*E-mail: wangshuj@tsinghua.edu.cn.
Funding

Financial support from Chinese MOST project Key Technology Research and Development on Advanced Coal Conversion
and Power Generation (2010DFA72730) is greatly appreciated.
1639

dx.doi.org/10.1021/je301371p | J. Chem. Eng. Data 2013, 58, 16331640

Journal of Chemical & Engineering Data

Article

Methyldiethanolamine + Piperazine). J. Chem. Eng. Data 2007, 52,

13811385.
(35) Li, M. H.; Lai, M. D. Solubility and Diffusivity of N2O and CO2 in
(Monoethanolamine + N-Methyldiethanolamine + Water) and in
(Monoethanolamine +2-Amino-2-methyl-1-propanol + Water). J.
Chem. Eng. Data 1995, 40, 486492.
(36) Tsai, T. C.; Ko, J. J.; Wang, H. M.; Lin, C. Y.; Li, M. H. Solubility of
Nitrous Oxide in Alkanolamine Aqueous Solutions. J. Chem. Eng. Data
2000, 45, 341347.
(37) Ying, J.; Dag, A. E.; Yi, W. Measurements and Correlation of
Physical Solubility of Carbon Dioxide in (Monoethanolamine + Water)
by a Modified Technique. Ind. Eng. Chem. Res. 2012, 51, 69586966.

(14) Xu, Z. C.; Wang, S. J.; Chen, C. H. CO2 absorption by biphasic

solvents: mixtures of 1,4-Butanediamine and 2-(Diethylamino)-ethanol.
Int. J. Greenhouse Gas Control 2013, 16, 107115.
(15) Derks, P. W.; Hogendoorn, K. J.; Versteeg, G. F. Solubility of N2O
in and Density, Viscosity, and Surface Tension of Aqueous Piperazine
Solutions. J. Chem. Eng. Data 2005, 50, 19471950.
(16) Versteeg, G. F.; Van Dijck, L. A. J.; van Swaaij, W. P. M. On the
kinetics between CO2 and alkanolamines both in aqueous and nonaqueous solutions. An overview. Chem. Eng. Commun. 1996, 144, 113
158.
(17) Laddha, S. S.; Diaz, J. M.; Danckwerts, P. V. The N2O analogy; the
solubilities of CO2 and N2O in aqueous solutions of organic compounds.
Chem. Eng. Sci. 1981, 36, 229230.
(18) Sada, E.; Kumazawa, H.; Butt, M. A. Solubility and diffusivity of
gases in aqueous solutions of amines. J. Chem. Eng. Data 1978, 23, 161
163.
(19) Singh, P.; Niederer, J. P. M.; Versteeg, G. F. Structure and activity
relationships for amine based CO2 absorbents-I. Int. J. Greenhouse Gas
Control 2007, 1, 510.
(20) Singh, P.; Versteeg, G. F. Structure and activity relationships for
CO2 regeneration from aqueous amine-based absorbents. Process Safty
Environ. Protect. 2008, 86, 347359.
(21) Singh, P.; Niederer, J. P. M.; Versteeg, G. F. Structure and activity
relationships for amine based CO2 absorbents-II. Chem. Eng. Res. Des.
2009, 87, 135144.
(22) Ahmed, N. C.; Negadi, L.; Mokbel, I.; Jose, J. Phase equilibrium
properties of binary aqueous solutions containing ehtanediamine, 1,2diaminopropane, 1,3-diaminopropane, or 1,4-diaminobutane at several
temperatures. J. Chem. Thermodyn. 2011, 43, 719724.
(23) Barbas, M. J. A.; Dias, F. A.; Mendonca, A. F. S. S.; Lampreia, I. M.
S. Volumetric properties of aqueous binary mixtures of 2-diethyaminethanol from 298.15 to 303.15 K. Phys. Chem. Chem. Phys. 2000, 2, 4858
4863.
(24) Lebrette, L.; Maham, Y.; Teng, T. T.; Hepler, L. G.; Mather, A. G.
Volumetric properties of aqueous solutions of mono, and diethylethanolamines at temperatures from 5 to 80 C. Thermochim. Acta 2002,
386, 119126.
(25) Maham, Y.; Lebrette, L.; Mather, A. E. Viscosities and Excess
Properties of Aqueous Solutions of Mono and Diethylethanolamines at
Temperatures between 298.15 and 353.15 K. J. Chem. Eng. Data 2002,
47, 550553.
(26) Little, R. J.; Van Swaaij, P. M.; Versteeg, G. F. Kinetics of carbon
dioxide with tertiary amines in aqueous solution. AIChE J. 1990, 36,
16331640.
(27) Vaidya, P. D.; Kenig, E. Y. Acceleration of CO2 reaction with N,NDiethylethanolamine in aqueous solutions by Piperazine. Ind. Eng.
Chem. Res. 2008, 47, 3438.
(28) Vaidya, P. D.; Kenig, E. Y. A Study on CO2 absorption Kinetics by
aqueous Solutions of N,N-Diethylethanolamine and N-Ethylethanolamine. Chem. Eng. Technol. 2009, 32, 556563.
(29) Li, W.; Dong, L.; Chen, J. Absorption kinetics of CO2 in aqueous
solutions of secondary and tertiary alkanolamines. Chin. J. Process Eng.
2011, 11, 422428.
(30) Versteeg, G. F.; van Swaiij, W. P. M. Solubility and Diffusivity of
Acid Gases (Carbon Dioxide and Nitrous Oxide) in Aqueous
Alkanolamine Solutions. J. Chem. Eng. Data 1988, 33, 2934.
(31) Liu, J. Z.; Wang, S. J.; Hartono, A.; Svendsen, H. F.; Chen, C. H.
Solubility of N2O in and Density and Viscosity of Aqueous Solutions of
Piperazine, Ammonia, and Their Mixtures from (283.15 to 323.15) K. J.
Chem. Eng. Data 2012, 57, 23872393.
(32) Watson, J. T. R.; Basu, R. S.; Sengers, J. V. An Improved
Representative Equation for the Dynamic Viscosity of Water Substance.
J. Phys. Chem. Ref. Data 1980, 9, 12551290.
(33) Sun, W. C.; Yong, C. B.; Li, M. H. Kinetics of the absorption of
carbon dioxide into mixed aqueous solutions of 2-amino-2-methyl-lpropanol and piperazine. Chem. Eng. Sci. 2005, 60, 503516.
(34) Samanta, A.; Roy, S.; Bandyopadhyay, S. S. Physical Solubility and
Diffusivity of N2O and CO2 in Aqueous Solutions of Piperazine and (N1640

dx.doi.org/10.1021/je301371p | J. Chem. Eng. Data 2013, 58, 16331640