Aspen Plus

Rate-Based Model of the CO2 Capture Process by

DEA using Aspen Plus
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Revision History
Version Description

V7.0 First version

V7.1 Update H2S Solubility model parameters
V7.1 CP1 Add O2, CO and H2 to the model as Henry Components
V7.2 Update results for V7.2
V7.3 Update databank to PURE25.
Add the definition of acid gas loading and amine weight fraction
convention.
V7.3.2 Update databank to PURE26.
Modify convergence specifications for the absorber.
Revise the simulation results.
V8.0 Update databank to PURE27.
V8.2 Update databank to PURE28.
V8.6 Update databank to PURE32.

Revision History 3
Contents
Introduction ............................................................................................................5

1 Components .........................................................................................................6

2 Process Description..............................................................................................7

3 Physical Properties...............................................................................................8

4 Reactions ...........................................................................................................14

5 Simulation Approach ..........................................................................................17

6 Simulation Results .............................................................................................21

7 Conclusions ........................................................................................................23

References ............................................................................................................24

4 Contents
Introduction

This document describes an Aspen Plus rate-based model of the CO2 capture
process by DEA (Diethanolamine) from a gas mixture of CH4, C2H6, C3H8, N2,
CO2 and H2S. The model consists of an absorber and a stripper. The
operation data from a natural gas treating unit at Pyote, Texas (1975)[1] were
used to specify feed conditions and unit operation block specifications.
Thermophysical property models and reaction kinetic models are based on the
works of Aspen Technology (2007)[2] and Rinker et al. (1996)[3]. Transport
property models and model parameters have been validated against
experimental data from open literature.
The model presented here includes the following key features:
 True species including ions
 Electrolyte NRTL method for liquid and RK equation of state for vapor
 Concentration-based reaction kinetics
 Electrolyte transport property models
 Rate-based models for absorber and stripper with valve trays

Introduction 5
1 Components

The following components represent the chemical species present in the

process:

Table 1. Components Used in the Model

ID Type Name Formula

H2O Conventional WATER H2O

DEA Conventional DIETHANOLAMINE C4H11NO2-1
CO2 Conventional CARBON-DIOXIDE CO2
H3O+ Conventional H3O+ H3O+
OH- Conventional OH- OH-
HCO3- Conventional HCO3- HCO3-
CO3-2 Conventional CO3-- CO3-2
DEAH+ Conventional DEA+ C4H12NO2+
DEACOO- Conventional DEACOO- C5H10NO4-
H2S Conventional HYDROGEN-SULFIDE H2S
HS- Conventional HS- HS-
S-2 Conventional S-- S-2
CH4 Conventional METHANE CH4
C2H6 Conventional ETHANE C2H6
C3H8 Conventional PROPANE C3H8
N2 Conventional NITROGEN N2
O2 Conventional OXYGEN O2
CO Conventional CARBON-MONOXIDE CO
H2 Conventional HYDROGEN H2

6 1 Components
2 Process Description

The Pyote Unit[1] flowsheet for CO2 capture by DEA includes three absorbers
and two strippers. However, only one absorber and one stripper data are
reported. Table 2 represents the typical operation data:

Table 2. Data of the Pyote Unit

Absorber

Diameter 66 inch
Tray 20
Stripper

Diameter 72 inch
Tray 31

Feeds and Products

Sour Gas to Absorber 2.92 MM scfh

Lean Amine to Absorber 188 gpm
Rich Amine to Stripper 380 gpm
CO2 in Sour Gas 0.013(mole fraction)
H2S in Sour Gas 0.00054(mole fraction)
CO2 in Sweet Gas 150 ppm (mole fraction)
H2S in Sweet Gas 0.15 ppm (mole fraction)
DEA solution 28.69%(wt)

2 Process Description 7
3 Physical Properties

The Electrolyte NRTL method and RK equation of state are used to compute
liquid and vapor properties respectively in this rate-based DEA model. The
NRTL parameters were regressed against CO2 solubility data from Maddox et
al. (1987, 1989)[4,5] and H2S solubility data from Barreau et al. (2006)[6] and
data from Lawson and Garst (1976)[7].
CH4, C2H6, C3H8, N2, O2, CO, H2, CO2 and H2S are treated as Henry-
components (solutes) to which Henry’s law is applied. Henry’s constants are
retrieved from Aspen Plus databanks for these components with water and
are regressed against CO2 solubility data from Maddox et al. (1987, 1989)[4, 5]
for CO2 with DEA and against H2S solubility data from Barreau et al. (2006)[6]
and data from Lawson and Garst (1976)[7] for H2S with DEA. In the reactions
calculations, the activity coefficient basis for the Henry’s components is
chosen to be Aqueous. Therefore, in calculating the unsymmetric activity
coefficients (GAMUS) of the solutes, the infinite dilution activity coefficients
will be calculated based on infinite-dilution condition in pure water, instead of
in mixed solvents.
The liquid molar volume and transport property models have been updated
and their model parameters regressed from literature experimental data.
Specifications of these models include:
 For liquid molar volume, the Clarke model, called VAQCLK in Aspen Plus,
is used with option code of 1 to use the quadratic mixing rule for solvents.
The interaction parameter VLQKIJ for the quadratic mixing rule between
DEA and H2O is regressed against experimental density data of the DEA-
H2O system from Maham et al. (1994)[8]. The Clarke model parameter

VLCLK/1 is also regressed for main electrolytes (DEAH+, HCO 3 ), (DEAH+,
 2
DEACOO ) and (DEAH+, CO 3 ) against experimental density data of the
DEA-H2O-CO2 system from Weiland (1998)[9].
 For liquid viscosity, the Jones-Dole electrolyte correction model, called
MUL2JONS in Aspen Plus, is used with the mass fraction based ASPEN
liquid mixture viscosity model for the solvents. The three option codes for
MUL2JONS are set to: 1 (mixture viscosity weighted by mass fraction), 1
(always use Jones and Dole equation when the parameters are available),
and 2 (ASPEN liquid mixture viscosity model), respectively. The
interaction parameters between DEA and H2O in the ASPEN liquid mixture
viscosity model, MUKIJ and MULIJ, are regressed against experimental
DEA-H2O viscosity data from Oyevaar et al. (1989)[10], Rinker et al.
(1994)[11], Hsu and Li (1997)[12], Weiland (1998)[9], and Mandal(2003) et

8 3 Physical Properties
 al. [13]. The Jones-Dole model parameters, IONMUB, for DEAH+ and
DEACOO- are regressed against DEA-H2O-CO2 viscosity data from Weiland
2
(1998)[9]; that of CO 3 is regressed against K2CO3-H2O viscosity data from
Pac et al. (1984)[14]; and that of HCO3- is regressed against KHCO3-H2O
viscosity data from Palaty (1992)[15].
 For liquid surface tension, the Onsager-Samaras model, called SIG2ONSG
in Aspen Plus, is used with its option codes being -9 (exponent in mixing
rule) and 1 (electrolyte system), respectively. No additional adjusted
parameters are used in the surface tension model and the estimation
results are somewhat higher than the experimental data from Weiland
(1996)[16] (Figure 3).
 For thermal conductivity, the Riedel electrolyte correction model, called
KL2RDL in Aspen Plus, is used.
 For binary diffusivity, the Nernst-Hartley model, called DL1NST in Aspen
Plus, is used with option code of 1 (mixture viscosity weighted by mass
fraction).
In addition to the updates to the above properties, the aqueous phase heat of
formation at infinite dilution and 25°C (DHAQFM) for DEAH+ and DEACOO-
and the heat capacity at infinite dilution (CPAQ0) for DEAH+ and DEACOO- are
adjusted to fit to the literature data on heat of solution from Carson et al.
(2000)[17] and heat capacity from Weiland (1997)[18].
The estimation results of various transport and thermophysical properties are
summarized in Figures 1-7. Note that acid gas loading is defined as the ratio
of the moles of apparent acid gas to the moles of apparent DEA. Apparent
means before reaction, so for example if 1 mole of DEA is added to 9 moles of
water, and then 0.3 moles of CO2 is added to this mixture at sufficient
pressure to dissolve all the CO2, then the CO2 loading is 0.3/1 = 0.3,
regardless of the forms of CO2 and DEA after reacting. Weight percent of DEA
is calculated without CO2, so in the above example, it is calculated from the
mixture of 1 mole DEA and 9 moles of water. Since DEA has a molecular
weight of 105.137 and water has a molecular weight of 18.015, this is
105.137/(105.137+9*18.015) = 0.39337 or about 39 wt% DEA.

3 Physical Properties 9
 1200
EXP DEA 10w t%
EXP DEA 20w t%
EXP DEA 30w t%
EXP DEA 40w t%
1150 EST DEA 10w t%
EST DEA 20w t%
EST DEA 30w t%
EST DEA 40w t%
1100
Density, kg/m3

1050

1000

950

900
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading, m ol/m ol

Figure 1. Liquid Density of DEA-CO2-H2O at 298.15K, experimental data from

Weiland (1998)[9]

10
Viscosity, mPaS

EXP DEA 20w t%

EXP DEA 30w t%
EXP DEA 40w t%
EST DEA 20w t%
EST DEA 30w t%
EST DEA 40w t%
0.1
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading, m ol/m ol

Figure 2. Liquid Viscosity of DEA-CO2-H2O at 298.15K, experimental data

from Weiland (1998)[9]

10 3 Physical Properties
 100

90

80

Surface Tension, mN/m

70

60

50

40
EXP DEA 10w t%
30 EST DEA 10w t%
EXP DEA 20w t%
EST DEA 20w t%
20 EXP DEA 30w t%
EST DEA 30w t%
10 EXP DEA 40w t%
EST DEA 40w t%
0
0.00 0.10 0.20 0.30 0.40 0.50
CO2 Loading, mol/mol

Figure 3. Surface tension of DEA-CO2-H2O at 298.15K, experimental data

from Weiland (1996)[16]

0.6
Thermal Conductivity, Watt/m-K

0.5

0.4

0.3

0.2

DEA 10w t%
0.1 DEA 20w t%
DEA 30w t%
DEA 40w t%
0
0 0.1 0.2 0.3 0.4 0.5 0.6

CO2 Loading, mol/mol

Figure 4. Liquid Thermal Conductivity of DEA-CO2-H2O at 298.15K

3 Physical Properties 11
 Figure 5. Liquid Heat Capacity of DEA-CO2-H2O at 298.15K, experimental data
from Weiland (1997)[18]

Figure 6. Heat of Solution of DEA-CO2-H2O at 298.15K, experimental data

from Carson (2000)[17]

12 3 Physical Properties
 Figure 7. CO2 partial pressure of DEA-CO2-H2O (DEA mass fraction = 0.20),
experimental data from Maddox et al. (1989)[5]

100000

10000

1000
H2S Pressure, mmHg

100

10

1 EXP 100F
EST 100F
EXP 150F
0.1 EST 150F
EXP 200F
0.01 EST 200F
EXP 250F
EST 250F
0.001
0.001 0.01 0.1 1 10
H2S Loading

Figure 8. H2S partial pressure of DEA-H2S-H2O (DEA mass fraction = 0.25),

experimental data from Lawson and Garst (1976)[7].

3 Physical Properties 13
4 Reactions

DEA is a secondary ethanolamine, as shown in Figure 8. It can associate with

H3O+ to form DEAH+ ion and can also react with CO2 to form carbamate ion
DEACOO-.

Figure 8. DEA Molecular Structure

The electrolyte solution chemistry has been represented with a CHEMISTRY

model with ID = DEA. This CHEMISTRY ID is used as the global electrolyte
calculation option in the simulation by specifying it on the Global sheet of the
Properties | Specifications form. Chemical equilibrium is assumed with all
the ionic reactions in the CHEMISTRY DEA. In addition, a REACTION model
called DEA-REA has been created, which is used in calculations of the
absorber and stripper by specifying it in the Reaction part of the absorber
and stripper specifications. In DEA-REA, all reactions are assumed to be in
chemical equilibrium except those of CO2 with OH- and CO2 with DEA.

A. Chemistry ID: DEA

1 Equilibrium
DEAH   H 2 O  DEA  H 3 O 

2 Equilibrium
CO 2  2H 2 O  H 3 O   HCO 3

3 Equilibrium
HCO 3  H 2 O  H 3 O   CO 32

4 Equilibrium
DEACOO   H 2 O  DEA  HCO 3

5 Equilibrium
2H 2 O  H 3 O   OH 

6 Equilibrium
H 2 O  H 2S  HS   H 3 O 

7 Equilibrium
H 2 O  HS   S 2  H 3 O 

B. Reaction ID: DEA-REA

1 Equilibrium
DEAH   H 2 O  DEA  H 3 O 

14 4 Reactions
 2 Equilibrium
2H 2 O  H 3 O   OH 

3 Equilibrium
HCO 3  H 2 O  H 3 O   CO 32

4 Kinetic
CO 2  OH   HCO 3

5 Kinetic
HCO 3  CO 2  OH 

6 Kinetic
DEA  CO 2  H 2 O  DEACOO -  H 3 O 

7 Kinetic
DEACOO -  H 3 O   DEA  H 2 O  CO 2

8 Equilibrium
H 2 O  H 2S  HS   H 3 O 

9 Equilibrium
H 2 O  HS   S 2  H 3 O 

The equilibrium expressions for the reactions are taken from the work of
Austgen et al. (1988)[19] and Jou et al. (1982, 1993)[20,21,22]. The power law
expressions are used for the rate-controlled reactions (reactions 4-7 in DEA-
REA) and the general power law expression is:

  E  1 1  N
r  k T To  exp     C i i
n a
(1)
 R  T To  i 1
Where:
r = Rate of reaction;
k = Pre-exponential factor;
T = Absolute temperature;
T0 = Reference temperature;
n = Temperature exponent;
E = Activation energy;
R = Universal gas constant;
N = Number of components in the reaction;
Ci = Concentration of component i;
ai = The stoichiometric coefficient of component i in the reaction equation.
If To is not specified, the reduced power law expression is used:

E N
r  kT n exp (  ) C i i
a
(2)
RT i 1
In this work, the reduced expressions are used. In equation (2), the
concentration basis is Molarity and the factor n is zero. k and E are given in
Table 3. The kinetic parameters for reactions 4-7 in Table 3 are derived from
the work of Rinker et al. (1996)[3]. The DEA concentration range of the data
of Rinker is 0.25-2.8 M and the temperature range is 292-343 K, these
conditions are the operating conditions of the absorber modeled in this work.
The kinetic parameters for reaction 4 are taken from the work of Pinsent et al.

4 Reactions 15
 (1956)[23] The kinetic parameters for reaction 5 are calculated by using the
kinetic parameters of reaction 4 and the equilibrium constants of the
reversible reactions 4 and 5.

Table 3. Parameters k and E in Equation (2)

Reaction No. k E (cal/mol)
4 4.32e+13 13249
5 2.38e+17 29451
6 6480000 5072
7 1.34e+17 11497

16 4 Reactions
5 Simulation Approach

The natural gas treating unit at Pyote[1] is simulated in this work and is
described in this section.
Simulation Flowsheet – The Pyote Unit has been modeled with the
following simulation flowsheet in Aspen Plus as shown in Figure 9.

GASOU T CO2OU T

LEANIN

ABSOR BER RIC HIN STRIPPER

GASIN

RIC HOUT LEANOUT

Figure 9. Rate-Based DEA Simulation Flowsheet in Aspen Plus

5 Simulation Approach 17
 Unit Operations – The major unit operation models have been represented
by Aspen Plus Blocks as outlined in Table 4.

Table 4. Aspen Plus Unit Operation Blocks Used in the

Rate-Based DEA Model
Unit Operation Aspen Plus Block Comments / Specifications

Absorber RadFrac 1. Calculation type: Rate-Based

2. 20 Stages
3. Top Pressure: 900 psig
4. Reaction: Reaction ID is DEA-REA for all stages; when
calculation type is equilibrium, Holdup is used, and in this
file, Holdup=0.001 m3, which is intended to aid convergence
5. Tray Type: Glitsch Ballast
6. Tray Diameter: 66 inch
7. Weir height: 0.06 m
8. Mass transfer coefficient method: Scheffe and Weiland
(1987)
9. Interfacial area method: Scheffe and Weiland (1987)
10. Interfacial area factor: 0.74
11. Heat transfer coefficient method: Chilton and Colburn
12. Holdup correlation: Bennett et al. (1983)
13. Holdup scale factor: 1
14. Film resistance: Discrxn for liquid film; Film for vapor
film
15. Additional discretization points for liquid film: 0.0001,
0.001, 0.01, 0.1 and 0.5
16. Flow model: Mixed
17. Estimates: provide temperature estimates for all stages.
These estimates are intended to aid convergence
18. Convergence: set basic convergence Algorithm to
Newton, set advanced convergence parameters Stable-
meth to Line search. These specifications are intended to
aid convergence

18 5 Simulation Approach
Unit Operation Aspen Plus Block Comments / Specifications

Stripper RadFrac 1. Calculation type: Rate-Based

2. 33 Stages
3. Partial vapor condenser
4. Kettle reboiler
5. Mole distillate rate: initialized at 0.03kmol/s with final
value of 0.02804509kmol/s obtained by Design-Spec 1
6. Mole reflux rates: 0.04kmol/sec
7. Top Pressure: 9.8 psig
8. Reaction: Reaction ID is DEA-REA for all stages; when
calculation type is equilibrium, Holdup is used, and in this
file, Holdup=0.001 m3, which is intended to aid convergence.
9. Design specs: Stage 1 temperature = 291.5K
10. Vary: Distillate rate
11. Tray Type: Glitsch Ballast
12. Tray Diameter: 72 inch
13. Mass transfer coefficient method: Scheffe and Weiland
(1987)
14. Interfacial area method: Scheffe and Weiland (1987)
15. Interfacial area factor: 2
16. Heat transfer coefficient method: Chilton and Colburn
17. Holdup correlation: Bennett et al. (1983)
18. Film resistance: Filmxrn for liquid film; Film for vapor
film
19. Flow model: Mixed
20. Estimates: provide temperature estimates for all stages;
these estimates are intended to aid convergence

5 Simulation Approach 19
 Streams - Feeds to the absorber are gas stream GASIN containing CH4, C2H6,
C3H8, N2, CO2 and H2S and liquid solvent stream LEANIN containing aqueous
DEA solution with few CO2 loaded in. Feed to the stripper is rich solvent
stream RICHIN containing aqueous DEA solution with absorbed CO2. Feed
streams conditions are summarized in Table 5.

Table 5. Feed specifications

Stream ID GASIN LEANIN RICHIN
Substream: MIXED
Temperature: F 72 102 212
Pressure: psig 900 900 10
Total flow 3689 kmol/hr 188 gal/min 380 gal/min
Mole-Frac Mass-Frac Mole-Frac
H2O 0 0.7118 0.91
DEA 0 0.2869 0.063
CO2 0.013 0.0012 0.026
H2S 0.00054 0.0001 0.001
CH4 0.924 0 0
C2H6 0.036 0 0
C3H8 0.016 0 0
N2 0.01 0 0

20 5 Simulation Approach
6 Simulation Results

The simulation was performed using Aspen Plus. Key simulation results are
presented in Table 6. The measured versus calculated absorber and stripper
liquid temperature profiles are presented in Figures 10 and 11, respectively.

Table 6. Key Simulation Results

Variable Measurement Rate-Based DEA Model

Absorber
CO2 mole fraction in GASOUT 150 ppm 152.0ppm
Loading of RICHOUT, MolAcidGas/MolDEA 0.50 0.424
Stripper
Loading of LEANOUT, MolAcidGas/MolDEA 0.01 0.011
Reboiler duty, lbs. steam/ gal. circ. solution 0.85 0.79

200

150
Temperature, F

100

AspenPlus: Liquid
50 AspenPlus: Vapor
Measure

0
0 5 10 15 20

Stage number

Figure 10. The Absorber Liquid Temperature Profile

6 Simulation Results 21
 250

200

Temperature, F

150

AspenPlus: Liquid
AspenPlus: Vapor
100
Measurement

50
0 5 10 15 20 25 30 35
Stage number

Figure 11. The Stripper Liquid Temperature Profile

22 6 Simulation Results
7 Conclusions

The rate-based DEA model provides a rate-based rigorous simulation of the

process. Key features of this rigorous simulation include electrolyte
thermodynamics and solution chemistry, reaction kinetics for the liquid phase
reactions, rigorous transport property modeling, rate-based multi-stage
simulation with Aspen Rate-Based Distillation which incorporates heat and
mass transfer correlations accounting for columns specifics and hydraulics.
The model is meant to be used as a guide for modeling the CO2 capture
process with DEA. You may use it as a starting point for more sophisticated
models for process development, debottlenecking, plant and equipment
design, among others.

7 Conclusions 23
References

[1] F.B. Butwell, C.R. Perry, “Performance of Gas Purification Systems

Utilizing DEA Solutions”. Laurance Reid Gas Conditioning Conference, 1975
[2] Aspen Technology Inc., 2007
[3] E.B. Rinker, S.S. Ashour, O.C. Sandall, “Kinetics and Modeling of Carbon
Dioxide Absorption into Aqueous Solutions of Diethanolamine”, Ind. Eng.
Chem. Res., 35, 1107-1114 (1996)
[4] R.N. Maddox, A.H. Bhairl, J.R. Diers, P.A. Thomas, “Equilibrium Solubility
of Carbon Dioxide or Hydrogen Sulfide in Aqueous Solutions of
Monoethanolamine, Diglycolamine, Diethanolamine and Methldiethanolamine”,
GPA Research Report, No. 104, 1987
[5] R.N. Maddox, E.M. Elizondo, “Equilibrium Solubility of Carbon Dioxide or
Hydrogen Sulfide in Aqueous Solutions of Diethanolamine at Low Partial
Pressures”, GPA Research Report, No. 124, 1989
[6] A. Barreau, E. Blanchon le Bouhelec, K.N. Habchi Tounsi, P. Mougin, and
F. Lecomte, "Absorption of H2S and CO2 in Alkanolamine Aqueous Solution:
Experimental Data and Modelling with the Electrolyte-NRTL Model", Oil & Gas
Science and Technology – Rev. IFP, 61, 3, 345-361(2006)
[7] J.D. Lawson and A.W. Garst, "Gas Sweetening Data: Equilibrium Solubility
of Hydrogen Sulfide and Carbon Dioxide in Aqueous Monoethanolamine and
Aqueous Diethanolamine Solutions", J. Chem. Eng. Data, 21, 20-30(1976)
[8] Y. Maham, T.-T. Teng, L.G. Hepler, A.E. Mather, “Densities, excess molar
volumes, and partial molar volumes for binary mixtures of water with
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Solution Chem., 23, 2, 195-205(1994)
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[10] M.H. Oyevaar, R.W.J. Morsinkhof, K.R. Westerterp, “Density, Viscosity,
Solubility, and Diffusivity of Diethanolamine in Aqueous Ethlyene Glycol at
298K”, J. Chem. Eng. Data., Vol. 34, Issue. 1, 77-82(1989)
[11] E.B. Rinker, D.W. Oleschager, A.T. Colussi, K.R. Henry, O.C. Sandall,
“Viscosity, Density, and Surface Tension of Binary Mixtures of Water and N-
Methyldiethanolamine and Water and Diethanolamine and Tertiary Mixtures of

24 References
 These Amines with Water over the Temperature Range 20-100°C”, J. Chem.
Eng. Data., 39, 392-395(1994)
[12] C.H. Hsu, M.H. Li, “Viscosities of aqueous blended amines”, J. Chem. Eng.
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[13] B.P. Mandal, M. Kundu, S.S. Bandyopadhyay, “Density and viscosity of
aqueous solutions of (N-methyldiethanolamine + monoethanolamine), (N-
methyldiethanolamine + diethanolamine), (2-amino-2-methyl-1-propanol +
monoethanolamine), and (2-amino-2-methyl-1-propanol + diethanolamine)”,
J. Chem. Eng. Data., 48, 703-707(2003)
[14] J.S. Pac, I.N. Maksimova, L.V. Glushenko, ”Viscosity of Alkali Salt
Solutions and Comparative Calculation Method”, J. Appl. Chem. USSR, 57,
846 (1984)
[15] Z. Palaty, “Viscosity of diluted aqueous K2CO3/KHCO3 solutions”, Collect.
Czech. Chem. Commun., 57, 1879(1992)
[16] R.H. Weiland, “Physical Properties of MEA, DEA, MDEA and MDEA-Based
Blends Loaded with CO2”, GPA Research Report, No. 152, 1996
[17] J.K. Carson, K.N. Marsh, A.E. Mather, “Enthalpy of solution of carbon
dioxide in (water + monoethanolamine, or diethanolamine, or N-
methyldiethanolamine) and (water + monoethanolamine + N-
methyldiethanolamine) at T = 298.15 K”, J. Chem. Thermodyn., 32, 1285-
1296 (2000)
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