J. Chem. Eng.

Data 2007, 52, 1381-1385

1381

Physical Solubility and Diffusivity of N2O and CO2 in Aqueous Solutions of

Piperazine and (N-Methyldiethanolamine + Piperazine)
Arunkumar Samanta, Sushanta Roy, and Syamalendu S. Bandyopadhyay*
Separation Science Laboratory, Cryogenic Engineering Centre, Indian Institute of Technology, Kharagpur 721 302, India

In this work, the physical solubility and diffusivity of N2O in aqueous solutions of piperazine (PZ) and an aqueous
blend of N-methyldiethanolamine (MDEA) and piperazine have been measured over a range of temperatures and
at atmospheric pressure. For the binary mixtures, the mass percents of PZ used are (1.74 to 12) %. For the ternary
mixtures, the total amine strength in the solution has been kept at 30 mass %. The N2O analogy is then used
to estimate the physical solubility and diffusivity of CO2 in aqueous PZ and PZ-blended aqueous MDEA solutions.
The experimental physical solubility and diffusivity data have been correlated as a function of temperature and
concentration of amine and compared with the available data in the literature.

Introduction
Aqueous solutions of alkanolamines are widely used for the
removal of acid gas impurities, such as CO2 and H2S, from
natural gas and industrial gas streams by a regenerative chemical
absorption process. Industrially important alkanolamines for
such absorption processes are monoethanolamine (MEA), diethanolamine (DEA), di-isopropanolamine (DIPA), and Nmethyldiethanolamine (MDEA).1 Although MEA and DEA are
widely used today for total CO2 and H2S removal from sour
natural gas and industrial gas streams, aqueous MDEA is used
very often for selective removal of H2S from gas streams
containing both CO2 and H2S. Recently, blended amine solvents,
which consist of a mixture of a primary or secondary amine
with a tertiary amine to combine the higher equilibrium capacity
of the tertiary amine with the higher reaction rate of the primary
or secondary amine, have been suggested for industrial gastreating processes. The use of blended amines brings about a
significant improvement in absorption capacity and absorption
rate and consequently offers great savings in solvent regeneration
energy requirements. More recently, there is a growing interest
in the use of piperazine (PZ) activated aqueous MDEA for gastreating processes. Being a cyclic symmetric diamine, each mole
of piperazine can theoretically absorb two moles of CO2, and it
may favor rapid formation of the carbamates. The apparent
second-order rate constant of PZ has been found to be an order
higher than that of conventional alkanolamines such as MEA.2
Because PZ is effective in enhancing the rate of CO2 absorption
at a much lower concentration in its blend with MDEA than
the concentration of the primary and secondary amines in the
conventional blended amines (MEA/MDEA or DEA/MDEA),
PZ is better known as an activator or promoter in gas-treating
processes.
For the analysis of the experimental absorption rate and for
the rational design of the gas absorption units and equipment
using alkanolamines, knowledge of the physical properties, for
example, the solubility and diffusivity data of CO2 in aqueous
amine solvents and their blends at various amine concentrations
* To whom correspondence should be addressed. Telephone: 91-322223580(O)/283581(R). Fax: 91-3222-282258. E-mail: ssbandyo@
hijli.iitkgp.ernet.in.

and temperatures, is essential. However, because CO2 undergoes

chemical reaction with these solvents, the physical solubility
and diffusivity of CO2 in amine solutions cannot be measured
directly. As a result, one must use a nonreacting gas such as
N2O as a surrogate to CO2 in estimating the physical solubility
and diffusivity of CO2 in these solvents. The N2O analogy3
for estimating the physical solubility and diffusivity of CO2 in
amine solutions is given by eqs 1 and 2, respectively, as follows.

(
(

HCO2-amine ) HN2O-amine

DCO2-amine ) DN2O-amine

HCO2,water

)
)

HN2O,water
DCO2,water

DN2O,water

(1)

(2)

where HN2O-amine and DN2O-amine are the physical solubility and

diffusivity of N2O in the amine solution. This analogy has been
frequently used to estimate the physical solubility of CO2 in
amine solvents.4-9 Several properties of aqueous solutions of
MDEA and its blends with primary and secondary alkanolamines have been reported previously in the literature.5,7,10-12
However, in spite of the immense importance of these data,
the PZ activated aqueous MDEA solvent system has not been
thoroughly investigated so far.
Therefore, in the present work, the physical solubility and
diffusivity of N2O in aqueous PZ and PZ activated MDEA
solutions at various temperatures and various relative compositions of amine blends are measured, and the N2O analogy is
then applied to estimate the solubilities of CO2 in (PZ + water)
and in (MDEA + PZ + water) solutions. The experimental
results are correlated as a function of the temperature and
concentration of amine.

Experimental
Reagent grade piperazine (>99 % pure) and MDEA (>98
% pure) were obtained from E. Merck, FRG, and were used
without further purification. Distilled water degassed by boiling
was used for preparing the amine solutions. The total amine
contents of the solutions were determined by titration against
standard 0.5 molL-1 HCl using a methyl orange indicator. The

10.1021/je700083b CCC: $37.00 2007 American Chemical Society

Published on Web 05/19/2007

1382

Journal of Chemical and Engineering Data, Vol. 52, No. 4, 2007

Table 1. Measured Solubility of N2O and CO2 in Water

T

HN2O-water

HCO2-water

kPam3kmol-1

kPam3kmol-1

293
298
303
308
313

3530
3932
4497
5120
5535

2619
2949
3358
3850
4264

nitrous oxide (>99.99 % pure) and carbon dioxide (>99.9 %

pure) used for the physical solubility and diffusivity study were
obtained from BOC, India, and Chemtron Science Pvt. Ltd.,
India, respectively.
Physical Solubility. The physical solubility measurements
were carried out in a corning glass equilibrium cell, similar to
one used by Saha et al.8 The temperature of the cell and jacketed
eudiometer was controlled within ( 0.1 K of the desired level
with a circulator temperature controller (JULABO FP 55, FRG).
Also, the experimental setup was housed inside an enclosure
in which the environmental temperature could be controlled
within ( 1 K of the desired level. A precise manometric device
was used to maintain the atmospheric pressure in the cell
throughout the experiment. All solubility measurements were
carried out at atmospheric pressure.
For each run, the cell was purged with saturated N2O or CO2
gas when the system reached thermal equilibrium with respect
to the desired temperature for solubility measurement. The gasphase stirrer was put on at 65-70 rpm during purging to ensure
proper purging and a uniform gas-phase temperature throughout
the cell. When it was purged properly, the gas phase stirrer was
stopped for the time being. A measured volume of 10 mL of
freshly prepared aqueous amine solution of desired concentration
was quickly transferred into the cell, and the cell was fully
sealed. The liquid was agitated with a magnetic stirrer until there
was no further change in the gas volume at least for 1 h. The
measured volume change is equal to the volume of gas absorbed.
The partial pressure of N2O in the experiments was corrected
for the vapor pressure of the solution. The experimental
uncertainty in the measured physical solubility was estimated
to be ( 2 %. The reproducibility among the various experiments
was within ( 2 %.
DiffusiWity. A 2.8110-2 m o.d. stainless steel wetted wall
absorber was used to measure the diffusivity of CO2 in water
and of N2O in water and aqueous amine solutions. The apparatus
and procedure are the same as those described by Saha et al.8
The gas-liquid contact time could be varied from 0.3 to 0.85
s by varying the absorption length but keeping the liquid flow
rate constant. The rate of absorption of the gas was measured
by the volume uptake method using a soap film meter. The flow
rate of the solvent was measured with a rotameter that was
calibrated at various experimental temperatures and concentra-

Figure 1. Henrys constant of CO2 in water as a function of temperature:

1, Versteeg et al.;6 , Al-Ghawas et al.;10 9, this study; s, calculated by
eq 3.

Figure 2. Henrys constant of N2O in water as a function of temperature:

1, Versteeg et al.;6 , Al-Ghawas et al.;10 O, Mandal et al.;12 9, this study;
s, calculated by eq 4.

tions of the solutions. The temperature of absorption was

controlled within ( 0.1 K of the desired level with the circulator
temperature controllers (FP 55 and F 32 Julabo, FRG). The
pressure in the absorption chamber was about 100 kPa. The
experimental uncertainty was estimated to be ( 4 %. The
reproducibility among the various experiments was always
within ( 2 %.

Table 2. Estimated Solubility of CO2, HCO2, in PZ (2) + Water (3) Using the N2O Analogy
HN2O/kPam3kmol-1

HCO2/kPam3kmol-1

100 w2 T ) 293.0 K T ) 298.0 K T ) 303.0 K T ) 308.0 K T ) 313.0 K T ) 293.0 K T ) 298.0 K T ) 303.0 K T ) 308.0 K T ) 313.0 K
1.74
5.16
12.0

3581
3690
3866

4094
4198
4423

4664
4843
5037

5278
5565
5753

5981
6194
6345

2657
2737
2868

3044
3149
3318

3483
3616
3761

4047
4267
4411

4607
4772
4888

Table 3. Estimated Solubility of CO2, HCO2, in MDEA (1) + PZ (2) + Water (3) Using the N2O Analogy
HN2O/kPam3kmol-1

HCO2/kPam3kmol-1

w1/w2 T ) 293.0 K T ) 298.0 K T ) 303.0 K T ) 308.0 K T ) 313.0 K T ) 293.0 K T ) 298.0 K T ) 303.0 K T ) 308.0 K T ) 313.0 K
28/2
22/8
18/12

3992
3866
4199

4587
4346
4673

5140
4890
5302

5565
5333
5753

6050
5781
6269

2961
2867
3115

3441
3259
3505

3838
3651
3959

4267
4090
4411

4661
4454
4829

Journal of Chemical and Engineering Data, Vol. 52, No. 4, 2007 1383

Figure 3. Henrys constant of N2O in the PZ (2) + water (3) system at

various temperatures: 9, w2 ) 1.74; 2, w2 ) 5.16; b, w2 ) 12.0; s,
calculated by eq 5.

Figure 4. Henrys constant of N2O in the MDEA (1) + PZ (2) + water

(3) system at various temperatures: 9, w1/w2 ) 28/2; 2, w1/w2 ) 22/8; b,
w1/w2 ) 18/12; s, calculated by eq 5.
Table 4. Parameters and AADs for N2O Solubility Correlations for
the Binary and Ternary Solvent Systems
ai

bi
-2.3910-5

ci

AAD )

1
N

i)1

|Hcalcd,i - Hexptl,i|

Figure 6. Diffusivity of N2O in water as a function of temperature: 1,

Versteeg et al.;6 , Al-Ghawas et al.;10 0, Li and Lee;11 O, Mandal et al.;12
9, this study; s, calculated by eq 8.
Table 5. Measured Diffusivity of N2O and CO2 in Water
T

DN2O-water109

DCO2-water109

1.32

m2s-1

m2s-1

1.47

298
303
308
313

1.68
1.92
2.26
2.53

1.95
2.20
2.48
2.90

2.4210-4

i ) 1 4.69
i ) 2 1.0510-5 1.8910-4
7.3810-5
i ) 3 4.0510-5 1.6810-5 -5.9610-5
i ) 1 8.05
-3.85
-16.58
(MDEA + PZ + i ) 2 17.52
4.08
-10.38
i ) 3 0.026
-0.175
0.294
H2O)
R
0.969
(PZ + H2O)

AADa/%

Figure 5. Diffusivity of CO2 in water as a function of temperature: 1,

Versteeg et al.;6 , Al-Ghawas et al.;10 0, Li and Lee;11 O, Mandal et al.;12
9, this study; s, calculated by eq 7.

100

Hexptl,i

Results and Discussion

Solubility. To confirm the validity of the experimental method
and the apparatus used for the present study, the solubilities of
CO2 and N2O in water were measured at (293, 298, 303, 308,
and 313) K. The results are presented in Table 1 and compared
with the literature data6,10 in Figures 1 and 2. There is a good
agreement between the literature results and the results of the
present study, thus supporting the applicability of the present
experimental method. The results of the solubility of N2O and

CO2 in water have been correlated as a function of temperature

by eqs 3 and 4, respectively, as follows.
HCO2-water/kPam3kmol-1 ) 6.17106 exp(-2276/(T/K))

(3)

HN2O-water/kPam3kmol-1 ) 4.86106 exp(-2117/(T/K))

(4)

The data for the solubility of N2O and the estimated solubility
of CO2 using the N2O analogy in aqueous solutions of PZ and
PZ activated MDEA blends for the temperatures (293, 298, 303,
308, and 313) K are presented in Tables 2 and 3 and shown in
Figures 3 and 4. The experimental solubility data of N2O in

1384

Journal of Chemical and Engineering Data, Vol. 52, No. 4, 2007

Table 6. Estimated Diffusivity of CO2, DCO2, in PZ (2) + Water (3) Using the N2O Analogy
DN2O109/m2s-1

DCO2109/m2s-1

100 w2

T ) 298.0 K

T ) 303.0 K

T ) 308.0 K

T ) 313.0 K

T ) 298.0 K

T ) 303.0 K

T ) 308.0 K

T ) 313.0 K

1.74
3.45
6.88

1.69
1.58
1.53

1.89
1.80
1.67

2.12
2.03
1.94

2.28
2.18
2.14

1.94
1.81
1.75

2.15
2.05
1.90

2.40
2.30
2.20

2.57
2.46
2.41

Table 7. Estimated Diffusivity of CO2, DCO2, in MDEA (1) + PZ (2) + Water (3) Using the N2O Analogy
DN2O109/m2s-1

DCO2109/m2s-1

w1/w2

T ) 298.0 K

T ) 303.0 K

T ) 308.0 K

T ) 313.0 K

T ) 298.0 K

T ) 303.0 K

T ) 308.0 K

T ) 313.0 K

28/2
25/5
22/8

0.73
0.61
0.54

0.91
0.77
0.65

1.02
0.83
0.75

1.15
0.97
0.84

0.84
0.70
0.62

1.04
0.88
0.74

1.16
0.94
0.85

1.30
1.09
0.95

Table 8. Test of Validity of the Modified Stokes-Einstein Equation

(eq 9) for the Diffusivity of N2O, DN2O, in PZ (2) + Water (3)
T

DN2O109

103

D0.79/T1014

100 w2

m2s-1

mPas

m3PaK-1

298

1.74
3.68
6.88
1.74
3.68
6.88

1.69
1.58
1.53
2.28
2.18
2.14

0.96
1.02
1.17
0.68
0.72
0.82

2.35
2.31
2.49
2.31
2.30
2.51

313

DN2O109

103/

D0.79/T1014

w1/w2

m2s-1

mPas

m3PaK-1

298

28/2
25/5
22/8
28/2
25/5
22/8

0.73
0.61
0.54
1.15
0.97
0.84

3.18
3.34
3.48
1.93
1.97
2.03

2.61
2.28
2.08
2.64
2.27
2.02

313

binary and ternary mixtures are correlated as a function of

temperature and concentration of amine according to eq 5.
ln HN2O ) K1 +

K2
+ K3T
T

(5)

where the parameters, Kis, are expressed as

Ki ) ai + bi(w1 + Rw2) + ci(w1 + Rw2)

ai

bi

ci

AAD/%

i ) 1 -23.48
-0.122
-0.054
(PZ + H2O)
i)2
0.21
-7.7210-4 0.109
i)3
3.7810-5 -5.8910-5 4.7710-4
i ) 1 -26.41
-11.10
52.83
i ) 2 -29.81
-15.71
-2.86
(MDEA + PZ +
i)3
2.70
-19.14
33.85
H2O)
R
0.0999

Table 9. Test of Validity of the Modified Stokes-Einstein Equation

(eq 9) for the Diffusivity of N2O, DN2O, in MDEA (1) + PZ (2) +
Water (3)
T

Table 10. Parameters and AADs for N2O Diffusivity Correlations

for the Binary and Ternary Solvent Systems

1.34
3.27

DiffusiWity. To validate the diffusivity apparatus and the

experimental method of the measurement, the diffusivities of
CO2 and N2O in water were measured at (298, 303, 308, and
313) K. The results are presented in Table 5. The comparisons
between the literature results6,10-12 and results obtained in this
study for the diffusivities of CO2 and N2O in water are shown
in Figures 5 and 6. As shown in Figures 5 and 6, the diffusivities
of CO2 and N2O in water obtained in this study are in good
agreement with the literature values. However, the diffusivity
data of N2O in water reported by Al-Ghawas et al.10 are
somewhat different than those of this study. On the basis of
the results, the diffusivities of N2O and CO2 in water can be
correlated as a function of temperature by eqs 7 and 8,
respectively.
DCO2-water/m2s-1 ) 8.1310-6 exp(-2488/(T/K))

(7)

DN2O-water/m2s-1 ) 9.7210-6 exp(-2582/(T/K))

(8)

(6)

where ai, bi, ci, and R are the correlation parameters and w1
and w2 are the mass percent of individual amine.
The calculated parameters and average absolute deviations
(AADs) are listed in Table 4 for the (PZ + H2O) and (MDEA
+ PZ + H2O) systems. The calculated solubilities from eq 5
are in good agreement with the experimental results of this study.
The AAD values between the correlated and experimental data
for (PZ + H2O) and (MDEA + PZ + H2O) systems are about
1.32 % and 1.47 %, respectively. The measured and calculated
solubilities from the correlation (eq 5) are compared in Figures
3 and 4. The solubility data of Sun et al.13 and Derks et al.14
for N2O in aqueous PZ solutions for the temperature range (298
to 313) K show good agreement with the values found using
eq 5, and the average absolute deviations are 3.3 % and 1.0 %,
respectively. As shown in Figures 3 and 4, Henrys constant of
N2O in aqueous PZ increases with an increase in temperature
and increases with the mass percent of PZ in the mixture,
although the effect of PZ mass fraction on N2O solubility in
amines is less pronounced.

The measured diffusivities of N2O as well as the estimated

diffusivity of CO2 in (PZ + H2O) and (MDEA + PZ + H2O)
for the temperatures (298, 303, 308, and 313) K are presented
in Tables 6 and 7 and shown in Figures 7 and 8. The
experimental diffusivities of N2O in (PZ + H2O) and (MDEA
+ PZ + H2O) as presented in Tables 8 and 9 are correlated by
a modified Stokes-Einstein equation (eq 9). The viscosity of
(PZ + H2O) has been taken from Samanta and Bandyopadhyay,15 and the viscosity of (MDEA + PZ + H2O) has been
measured using the standard procedure described elsewhere.15
Equation 9 predicts the experimental diffusivities of N2O in (PZ
+ H2O) and (MDEA + PZ + H2O) with an average absolute
deviation of 6.4 %.
DN2O0.79
T

) constant

(9)

The prediction of diffusivity of N2O from eq 9 also requires

the knowledge of the solution viscosity. For convenience,
however, the same data are correlated by a simpler equation

Journal of Chemical and Engineering Data, Vol. 52, No. 4, 2007 1385

(PZ+ H2O) appear to be smaller than the measured diffusivities

of N2O, which is contradictory to the N2O analogy. As shown
in Figures 7 and 8, diffusivities of N2O in aqueous PZ and blends
of (MDEA + PZ) increase with an increase in temperature and
increase with the decrease in mass fraction of PZ in the mixture,
though the effect of PZ mass fraction in solution is less
pronounced on the N2O diffusivity in amines.

Conclusion

Figure 7. Diffusivity of N2O in the PZ (2) + water (3) system at various

temperatures: 9, w2 ) 1.74; b, w2 ) 3.45; 2, w2 ) 6.88; s, calculated by
eq 10.

The physical solubility and diffusivity of N2O in aqueous

piperazine and piperazine activated aqueous MDEA solvents
have been measured and correlated. The solubility measurements
were done using a corning glass equilibrium cell over the temperature range (293 to 313) K, and the diffusivity measurements
were done using a laboratory wetted wall contactor over the
temperature range (298 to 313) K. The N2O analogy was used
to estimate the solubility as well as the diffusivity of CO2 in
(PZ + water) and in (MDEA + PZ + water). Calculated results
using the correlations (eqs 5 and 10) for solubility and diffusivity
of N2O in binary and ternary mixtures are in good agreement
with the experimental data of this study and literature results
over the temperature and amine concentration ranges studied.

Literature Cited

Figure 8. Diffusivity of N2O in the MDEA (1) + PZ (2) + water (3)

system at various temperatures: 9, w1/w2 ) 28/2; b, w1/w2 ) 25/5; 2,
w1/w2 ) 22/8; s, calculated by eq 10.

that takes into account the effect of solution viscosity implicitly.

This equation has the following form
ln DN2O ) K1 +

K2
+ K3T
T

(10)

where the parameters, Kis, are expressed as

Ki ) ai + bi(w1 + Rw2) + ci(w1 + Rw2)2

(11)

Table 10 includes the determined parameters and AADs between the measured and calculated values for both (PZ + H2O)
and (MDEA + PZ + H2O) solutions. The AAD values for (PZ
+ H2O) and (MDEA + PZ + H2O) solutions are 1.34 % and
3.27 %, respectively. The small AADs indicate that the calculated diffusivities from eq 10 are in good agreement with the
experimental results of this study. The measured and calculated
diffusivities from the correlation (eq 10) are also compared in
Figures 7 and 8. The diffusivity data of Sun et al.13 for N2O in
aqueous PZ solutions for the temperature range (303 to 313) K
and for the PZ concentration range between 0.23 and 0.92
kmolm-3 show good agreement with the values calculated using
eq 10, the average absolute deviation being 4.41 %. The data
reported by Sun et al.13 for the estimated CO2 diffusivities in

(1) Kohl, A. L.; Nielsen, R. B. Gas Purification, 5th ed.; Gulf Publishing
Company: Houston, 1997.
(2) Bishnoi, S.; Rochelle, G. T. Absorption of carbon dioxide into aqueous
piperazine: reaction kinetics, mass transfer and solubility. Chem. Eng.
Sci. 2000, 55, 5531-5543.
(3) Clarke, J. K. A. Kinetics of Absorption of carbon dioxide in
monoethanolamine solution at short contact times. Ind. Eng. Chem.
Fundam. 1964, 3, 239-245.
(4) Laddha, S. S.; Diaz, J. M.; Danckwerts, P. V. The nitrous oxide analogy: the solubilities of carbon dioxide and nitrous oxide in aqueous
solutions of organic compounds. Chem. Eng. Sci. 1981, 36, 228-229.
(5) Haimour, N.; Sandall, O. C. Absorption of carbon dioxide into aqueous
methyldiethanolamine. Chem. Eng. Sci. 1984, 39, 1791-1796.
(6) Versteeg, G. F.; van Swaaij, W. P. M. Solubility and diffusivity of
acid gases (CO2, N2O) in aqueous alkanolamine solutions. J. Chem.
Eng. Data 1988, 33, 29-34.
(7) Littel, R. J.; Versteeg, G. F.; van Swaaij, W. P. M. Solubility and
diffusivity data for the absorption of COS, CO2, and N2O in amine
solutions. J. Chem. Eng. Data 1992, 37, 49-55.
(8) Saha, A. K.; Bandyopadhyay, S. S.; Biswas, A. K. Solubility and
diffusivity of N2O and CO2 in aqueous solutions of 2-amino-2-methyl1-propanol. J. Chem. Eng. Data 1993, 38, 78-82.
(9) Browning, G. J.; Weiland, R. H. Physical solubility of carbon dioxide
in aqueous alkanolamines via nitrous oxide analogy. J. Chem. Eng.
Data 1994, 39, 817-822.
(10) Al-Ghawas, H. A.; Hagewiesche, D. P.; Ruiz-Ibanez, G.; Sandall, O. C.
Physicochemical properties important for carbon dioxide absorption in
aqueous methyldiethanolamine. J. Chem. Eng. Data 1989, 34, 385-391.
(11) Li, M.-H.; Lee, W.-C. Solubility and diffusivity of N2O and CO2 in
(diethanolamine + N-methyldiethanolamine + water) and in (diethanolamine + 2-amino-2-methyl-1-propanol + water). J. Chem. Eng.
Data 1996, 41, 551-556.
(12) Mandal, B. P.; Kundu, M.; Padhiyar, N. U.; Bandyopadhyay, S. S.
Physical Solubility and diffusivity of N2O and CO2 into aqueous
solutions of (2-amino-2-methyl-1-propanol + diethanolamine) and (Nmethyldiethanolamine + diethanolamine). J. Chem. Eng. Data 2004,
49, 264-270.
(13) Sun, W.-C.; Yong, C.-B.; Li, M.-H. Kinetics of the absorption of
carbon dioxide into mixed aqueous solutions of 2-amino-2-methyl1-propanol and piperazine. Chem. Eng. Sci. 2005, 60, 503-516.
(14) Derks, P. W.; Hogendoorn, K. J.; Versteeg, G. F. Solubility of N2O
in and density, viscosity, and surface tension of aqueous piperazine
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(15) Samanta, A.; Bandyopadhyay, S. S. Density and viscosity of aqueous
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Received for review February 11, 2007. Accepted April 11, 2007.

JE700083B