ENRTL-RK Rate Based Sulfolane-DIPA Model

Aspen Plus
Aspen Plus Sulfolane-DIPA Model

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Revision History
Version Description
V7.3 First version

V7.3.2 The VLE data of the DIPA-H2O binary system generated from UNIFAC
used for identifying NRTL binary parameters for the DIPA-H2O pair were
replaced by experimental VLE data of the DIPA-H2O system.
V8.0 Update databank to PURE27.
V10.0 Update GMENCC parameters between CO 2 and (DIPAH+, DIPACOO- ),
and those between CO 2 and (DIPAH+, HCO3 - ) to match the data of CO 2
activity coefficient.
Update simulation results.
Revision History 1
Contents
Revision History ......................................................................................................1
Contents..................................................................................................................2
Introduction ............................................................................................................3
1 Components .........................................................................................................4
2 Physical Properties...............................................................................................5
3 Reactions ...........................................................................................................26
4 Simulation Approach ..........................................................................................29
5 Simulation Results .............................................................................................31
6 Conclusions ........................................................................................................32
References ............................................................................................................33
2 Contents
Introduction
This file describes an Aspen Plus model of the CO2 and H2S capture process by
mixed solvent composed of sulfolane, DIPA and water. As process simulation
is not within the scope of current phase of this work, we only give a single
stage flash model to simulate the CO2 and H2S absorption by aqueous
sulfolane-DIPA solution. Thermophysical property models are developed
based on the work of Zhang and Chen (2010) [1,2] and Aspen Technology
(2011)[3]. Reaction kinetic models are based on the works of Pinsent et al.
(1956)[4] and Blauwhoff et al. (1985)[5]. Transport property models and model
parameters have been validated against experimental data from open
literature.
The model includes the following key features:
 True species including ions
 Unsymmetric electrolyte NRTL activity coefficient model for liquid and PC-
SAFT equation of state for vapor
 Activity-based reaction kinetics
 Electrolyte transport property models
Introduction 3
1 Components
The following components represent the chemical species present in the

process:
Table 1. Components Used in the Model

Component ID Conventional Component name Formula
SULFOLAN Conventional SULFOLANE C4H8O2S

DIPA Conventional DIISOPROPANOLAMINE C6H15NO2
H2O Conventional WATER H2O
CO2 Conventional CARBON-DIOXIDE CO2
DIPAH+ Conventional
DIPACOO- Conventional
H3O+ Conventional H3O+ H3O+
OH- Conventional OH- OH-
HCO3- Conventional HCO3- HCO3-
CO3-2 Conventional CO3-- CO3-2
H2S Conventional HYDROGEN-SULFIDE H2S
HS- Conventional HS- HS-
S-2 Conventional S-- S-2
CH4 Conventional METHANE CH4
C2H6 Conventional ETHANE C2H6
4 1 Components
2 Physical Properties
The unsymmetric electrolyte NRTL property method (ENRTL-RK) and PC-SAFT

equation of state are used to compute liquid and vapor properties in the
sulfolane-DIPA model. CO2, H2S, CH4 and C2H6 are selected as Henry
components to which Henry’s law is applied. Henry’s constants are specified
for these components with water, DIPA and sulfolane. In the reaction
calculations, the activity coefficient basis for the Henry’s components is
chosen to be Aqueous. Therefore, in calculating the unsymmetric activity
coefficients of the solutes, the infinite dilution activity coefficients will be
calculated based on the infinite-dilution condition in water, instead of in mixed
solvents.
The Henry’s constant parameters for CO2, H2S, CH4 and C2H6 are obtained
from the literatures or regressed with the VLE data (See Table 2).
Table 2. Henry’s constants

Solute Solvent Source
CO2 H2 O Yan and Chen (2010) [6]

H2 S H2 O Zhang and Chen (2010) [2]
CH4 H2 O Zhang and Chen (2010) [2]
C 2 H6 H2 O Zhang and Chen (2010) [2]
CO2 DIPA Calculation with N2 O analogy[7,8]
H2 S DIPA Regression with VLE data for the DIPA-H2 S-H2 O and
sulfolane-DIPA-H2 S-H2 O systems [9-12]
CH4 DIPA Let to be default
C 2 H6 DIPA Let to be default
CO2 Sulfolane Regression with CO 2 -sulfolane VLE data[13-17]
H2 S Sulfolane Regression with H2 S-sulfolane VLE data[13-16]
CH4 Sulfolane Regression with CH4 -sulfolane VLE data[13]
C 2 H6 Sulfolane Regression with C 2 H6 -sulfolane VLE data[13]
PC-SAFT pure component parameters for DIPA are regressed against the
vapor pressure data generated from the Antoine equation [3] and experimental
data on liquid density[7,18]. The parameters of the ideal gas heat capacity
correlations for DIPA and sulfolane are then respectively obtained by fitting
the experimental liquid heat capacity data of DIPA [19] and liquid heat capacity
2 Physica l Prope rties 5

data of sulfolane generated from DIPPR correlation [3]. In addition, dielectric
constants of solvent sulfolane are regressed against the dielectric constant
data[20-24]. The characteristic volume parameters of H2O for the Brelvi-
O’Connell model are taken from Brelvi and O’Connell (1972) [25], and those of
CO2 are obtained from Yan and Chen (2010) [6]. For the other selected
components, the parameters are taken from the Aspen databank [3].
Unless specified otherwise, the binary interaction parameters for all molecule-
molecule pairs and electrolyte-electrolyte pairs are defaulted to be zero. All
molecule-electrolyte binary parameters are defaulted to (8, -4), average
values of these parameters [26]. The nonrandomness factor is fixed at 0.2.
The NRTL parameters between DIPA and H 2O were regressed against
experimental VLE data[27], enthalpy of mixing data[28] and liquid heat
capacity[29]. The NRTL parameters for the sulfolane-H2O binary are identified
by fitting the experimental VLE data[22,30-32] and excess enthalpy data[22,30,31]
of the sulfolane-H2O system. The NRTL binary parameters for sulfolane-CO2
and sulfolane-H2S systems are respectively regressed against the
experimental solubility data[13-17] of CO2 and H2S in sulfolane solvent.
The NRTL interaction parameters between H 2O and (DIPAH+, HCO3-) and
those between H2O and (DIPAH+, DIPACOO-) are regressed against VLE data
for the DIPA-CO2-H2O ternary system [9-11,33]. The NRTL interaction parameters
between sulfolane and (DIPAH+, HCO3-) and those between sulfolane and
(DIPAH+, DIPACOO-) are then identified by the fitting of VLE data for the
sulfolane-DIPA-CO2-H2O quaternary system [12]. The NRTL binary parameters
for the H2O-(DIPAH+, HS-), DIPA-(DIPAH+, HS-), and sulfolane-(DIPAH+, HS-)
pairs are regressed together using the VLE data for the DIPA-H2S-H2O ternary
system [9-11] and sulfolane-DIPA-H2O-H2S quaternary system [12]. The NRTL
interaction parameters for the (DIPAH +, HCO3-)-(DIPAH+, HS-) pair and the
(DIPAH+, DIPACOO-)-(DIPAH+, HS-) pair are determined by the regression for
VLE of the DIPA-CO2-H2S-H2O system[9, 11].
For a detailed description of the thermodynamic model please see the article
from Zhang and Chen (2010) [1,2] for the MDEA-CO2-H2S-H2O system.
The liquid molar volume model and transport property models have been
updated and model parameters are regressed from literature data.
Specifications include:
 For liquid molar volume, the Clarke model, called VAQCLK in Aspen Plus,
is used with option code 1 to use the quadratic mixing rule for solvents.
The interaction parameter VLQKIJ for the quadratic mixing rule between
DIPA and H2O is regressed against experimental DIPA-H2O density data
from Henni et al. (2003)[18]. The interaction parameter VLQKIJ between
sulfolane and H 2O is validated by experimental sulfolane-H2O density data
from the literature[22, 32, 34-43].The Clarke model parameter VLCLK/1 for
main electrolytes (DIPAH +, HCO3-) and (DIPAH+, DIPACOO-) is regressed
against experimental density data of the DIPA-CO2-H2O system from
Dell’Era et al. (2010) [33]. VLCLK/1 for other electrolytes is left to the
default.
 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 solvent. There are three models for
electrolyte correction and the sulfolane-DIPA model always uses the
Jones-Dole correction model. The three option codes for MUL2JONS are
6 2 Physical Properties
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 DIPA and H 2O in the ASPEN liquid mixture viscosity
model, MUKIJ and MULIJ, are regressed against experimental DIPA-H2O
viscosity data from Henni et al. (2003)[18]. MUKIJ and MULIJ for sulfolane-
H2O binary are regressed against experimental sulfolane-H2O viscosity
data from the literature[22, 34-42, 44]. The Jones-Dole model parameters,
IONMUB, of CO3-2 is regressed against K 2CO3-H2O viscosity data from Pac
et al. (1984)[45], that of HCO3- is regressed against KHCO3-H2O viscosity
data from Palaty (1992)[46], and that of HS- is regressed against MDEA-
H2O-H2S viscosity data from Rinker et al. (2000) [47]. For DIPAH+ and
DIPACOO-, IONMUB/1 are missing and IONMUB/2 are defaulted as 0.
 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.
 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 with the above transport properties, the Gibbs free
energy in aqueous phase infinite dilution at 298.15 K (DGAQFM) and the
enthalpy of formation in aqueous phase infinite dilution at 298.15 K
(DHAQFM) for DIPAH+ are calculated from the experimental chemical
 
equilibrium constant of the reaction DIPAH  H 2 O  DIPA  H 3 O as
reported by Hamborg and Versteeg (2009) [48]. Likewise, DGAQFM and
DHAQFM for DIPACOO- are calculated from the experimental chemical
 
equilibrium constant of the reaction DIPACOO  H 2 O  DIPA  HCO 3 as
reported by Blauwhoff et al. (1985) [5]. The heat capacities in aqueous phase
at infinite dilution (CPAQ0) for DIPAH + and DIPACOO- are obtained by
assuming the aqueous phase infinite dilution heat capacity change for the
above two reactions to be zero. The CPAQ0 of HCO3-, CO3-2 and HS- are the
average values of heat capacity between 298 K and 473 K taken from Criss
and Cobble (1968) [49], and that of S -2 is calculated from the Criss-Cobble
correlation[49] with the entropy value from Wagman et al. (1982)[50].
The estimation results of various transport and thermal properties are
summarized in Figures 1-35:

1200
1100
1000
Density, kg/m3
EXP DIPA 10.1 w t% (298.03 K)

900
EXP DIPA 11 w t% (298.22 K)
EXP DIPA 33.9 w t% (298.23 K)
800 EST 10.1 w t%
EST 11 w t%
EST 33.9 w t%
700
600
0.4 0.6 0.8 1 1.2 1.4
CO2 loading (m ol CO2/ m ol DIPA)
Figure 1. Liquid density of DIPA-CO2-H2O at around 298.15 K, experimental

data from Dell’Era et al. (2010)[33]
1200
1000
800
Density, kg/m3
600
400
EST DIPA 10wt%

200 EST DIPA 20wt%
EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/m ol DIPA)
Figure 2. Liquid density of DIPA-H2S-H2O at 298.15 K
1200
1000
800
Density, kg/m3
600
400
EST Sulfolane 5wt%+DIPA 5wt%
200 EST Sulfolane 10wt%+DIPA 10wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 3. Liquid density of sulfolane-DIPA-CO2-H2O at 298.15 K
1200
1000
800
Density, kg/m3
600
400
0
0 0.1 0.2 0.3 0.4 0.5
Figure 4. Liquid density of sulfolane-DIPA-H2S-H2O at 298.15 K

0.1
EST DIPA 10wt%
EST DIPA 20wt%
EST DIPA 30wt%
EST DIPA 40wt%
0.01
Viscosity, PaS
0.001
0.0001
0 0.1 0.2 0.3 0.4 0.5
Figure 5. Liquid viscosity of DIPA-CO2-H 2O at 298.15 K
0.1
EST DIPA 10wt%
EST DIPA 20wt%
EST DIPA 30wt%
EST DIPA 40wt%
0.01
Viscosity, PaS
0.001
0.0001
0 0.1 0.2 0.3 0.4 0.5
Figure 6. Liquid viscosity of DIPA-H2S-H 2O at 298.15 K
0.01
Viscosity, PaS
0.001

0.0001
0 0.1 0.2 0.3 0.4 0.5
Figure 7. Liquid viscosity of sulfolane-DIPA-CO2-H 2O at 298.15 K
0.01
Viscosity, PaS
0.001

0.0001
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/ m ol DIPA)
Figure 8. Liquid viscosity of sulfolane-DIPA-H2S-H 2O at 298.15 K

0.07
0.06
Surface Tension, N/m

0.05
0.04
0.03
0.02
EST DIPA 10wt%
EST DIPA 20wt%
0.01 EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 9. Surface tension of DIPA-CO2-H2O at 298.15 K
0.07
0.06
0.05
0.04
0.03
0.02
EST DIPA 10wt%
0.01 EST DIPA 20wt%
EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 10. Surface tension of DIPA-H 2S-H 2O at 298.15 K
0.08
0.07
0.06
0.05
0.04
0.03
0.02 EST Sulfolane 5wt%+DIPA 5wt%

0
0 0.1 0.2 0.3 0.4 0.5
Figure 11. Surface tension of sulfolane-DIPA-CO2-H 2O at 298.15 K
0.08
0.07
0.06
0.05
0.04
0.03

0
0 0.1 0.2 0.3 0.4 0.5
Figure 12. Surface tension of sulfolane-DIPA-H 2S-H 2O at 298.15 K

0.6
0.5
Thermal Cnductivity, Watt/m-K

0.4
0.3
0.2
EST DIPA 10wt%

0.1 EST DIPA 20wt%
EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 13. Liquid thermal conductivity of DIPA-CO2-H2O at 298.15 K
0.6
0.5
0.4
0.3
0.2
EST DIPA 10wt%
EST DIPA 20wt%
0.1 EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 14. Liquid thermal Conductivity of DIPA-H2S-H2O at 298.15 K
0.6
0.5

0.4
0.3
0.2

0
0 0.1 0.2 0.3 0.4 0.5
Figure 15. Liquid thermal conductivity of sulfolane-DIPA-CO2-H2O at 298.15 K
0.6
0.5
0.4
0.3
0.2

0
0 0.1 0.2 0.3 0.4 0.5
Figure 16. Liquid thermal conductivity of sulfolane-DIPA-H2S-H2O at 298.15 K

5000
4500
4000
Heat Capacity, J/kg-K 3500
3000
2500
2000
1500
EST DIPA 10wt%
1000
EST DIPA 20wt%
500 EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 17. Liquid heat capacity of DIPA-CO2-H 2O at 298.15 K
5000
4500
4000
Heat Capacity, J/kg-K
3500
3000
2500
2000
1500
EST DIPA 10wt%
1000
EST DIPA 20wt%
500 EST DIPA 30wt%
EST DIPA 40wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 18. Liquid heat Capacity of DIPA-H 2S-H 2O at 298.15 K
5000
4500
4000
Heat Capacity, J/kg-K 3500
3000
2500
2000
1500

EST Sufolane 20wt%+DIPA 20wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 19. Liquid heat capacity of sulfolane-DIPA-CO2-H2O at 298.15 K
5000
4500
4000
Heat Capacity, J/kg-K
3500
3000
2500
2000
1500

EST Sufolane 20wt%+DIPA 20wt%
0
0 0.1 0.2 0.3 0.4 0.5
Figure 20. Liquid heat capacity of sulfolane-DIPA-H2S-H2O at 298.15 K

0
-20000
Integral Heat of Solution, J/mol

-40000
-60000
-80000
-100000
-120000 EST DIPA 10wt%

EST DIPA 20wt%
-140000 EST DIPA 30wt%
EST DIPA 40wt%
-160000
0 0.1 0.2 0.3 0.4 0.5
Figure 21. Integral heat of solution of CO 2 in DIPA-H 2O at 298.15 K
-10000
-20000
-30000
-40000
-50000
EST DIPA 10wt%
EST DIPA 20wt%
-60000
EST DIPA 30wt%
EST DIPA 40wt%
-70000
-80000
0 0.1 0.2 0.3 0.4 0.5
Figure 22. Integral heat of solution of H 2S in DIPA-H 2O at 298.15 K
0
-20000

-40000
-60000
-80000
-100000
-120000 EST Sulfolane 5wt%+DIPA 5wt%

-160000
0 0.1 0.2 0.3 0.4 0.5
Figure 23. Integral heat of solution of CO 2 in sulfolane-DIPA-H 2O at 298.15 K
-10000
-20000
-30000
-40000
-50000

-80000
0 0.1 0.2 0.3 0.4 0.5
Figure 24. Integral heat of solution of H 2S in sulfolane-DIPA-H 2O at 298.15 K

1.0E+04
1.0E+03
CO 2 partial pressure, kPa 1.0E+02
1.0E+01
1.0E+00 35 wt%DIPA, 283.15 K (ter Maat et al. 2004)

35 wt%DIPA, 298.15 K (ter Maat et al. 2004)
33 wt%DIPA, 313.15 K (Isaacs et al. 1977a)
1.0E-01 33 wt%DIPA, 313.15 K (Isaacs et al. 1977b)
33 wt%DIPA, 373.15 K (Isaacs et al. 1977b)
1.0E-02
0 0.2 0.4 0.6 0.8 1 1.2
Figure 25. CO2 partial pressure of the DIPA-CO2-H2O System, experimental

data from the literature[9-11]
1.0E+04
1.0E+03
Total pressure, kPa
1.0E+02
1.0E+01 EXP DIPA 10.1wt%(299.28 K)

EXP DIPA 11wt%(298.22 K)
EXP DIPA 33.9 wt%(298.23 K)
1.0E+00
0.4 0.6 0.8 1 1.2 1.4
Figure 26. Total pressure of the DIPA-CO2-H2O system at around 298.15 K,

experimental data from Dell’Era et al. (2010)[33]
0.06
EXP DIPA 10 wt%(96.2 kPa)
0.05
0.04
CO 2 mole fraction
0.03
0.02
0.01
0
290 300 310 320 330 340 350 360
Tem perature, K
Figure 27. VLE of the DIPA-CO2-H2O system at around 100 kPa total pressure,
experimental data from from Dell’Era et al. (2010) [33]
1.0E+04
1.0E+03
H2 S partial pressure, kPa
1.0E+02
1.0E+01 33 wt%DIPA, 313.15 K (Isaacs et al. 1977a)

33 wt%DIPA, 313.15 K (Isaacs et al. 1977b)
1.0E+00 33 wt%DIPA, 373.15 K (Isaacs et al. 1977b)
1.0E-01
0 0.5 1 1.5 2
Figure 28. H 2S partial pressure of the DIPA-H2S-H 2O system, experimental

data from the literature[9-11]

1.0E+04
EXP 0.1H2S
1.0E+03
EXP 0.2 H2S
EXP 0.3 H2S
CO 2 partial pressure, kPa
EXP 0.4 H2S
1.0E+02
EXP 0.5 H2S
EXP 0.6 H2S
1.0E+01 EXP 0.7 H2S

EXP 0.8 H2S
EXP 0.9 H2S
1.0E+00 EXP 1H2S

EXP 1.1H2S
EXP 1.2 H2S
1.0E-01
0.01 0.1 1 10
Figure 29. CO2 partial pressure of the DIPA-CO2-H2S-H2O system at 313.15 K,

experimental data from Isaacs et al. (1977) [11]
1.0E+04
EXP 0.1H2S
EXP 0.2 H2S
EXP 0.3 H2S
1.0E+03
EXP 0.4 H2S
EXP 0.5 H2S

EXP 0.6 H2S
EXP 0.7 H2S
1.0E+02
EXP 0.8 H2S
EXP 0.9 H2S
EXP 1H2S
1.0E+01
1.0E+00
0.001 0.01 0.1 1
Figure 30. CO2 partial pressure of the DIPA-CO2-H2S-H2O system at 373.15 K,

1.0E+04
EXP 0.1CO2
1.0E+03
EXP 0.2 CO2
EXP 0.3 CO2
EXP 0.4 CO2
1.0E+02
EXP 0.5 CO2
EXP 0.6 CO2
EXP 0.7 CO2
1.0E+01
EXP 0.8 CO2
EXP 0.9 CO2
EXP 1CO2
1.0E+00
EXP 1.1CO2
EXP 1.2 CO2
1.0E-01
0.001 0.01 0.1 1 10
Figure 31. H 2S partial pressure of the DIPA-CO2-H 2S-H2O system at 313.15 K,

1.0E+04
1.0E+03 EXP 0.1CO2

EXP 0.2 CO2

EXP 0.3 CO2
EXP 0.4 CO2
1.0E+02 EXP 0.5 CO2
EXP 0.6 CO2
EXP 0.7 CO2
EXP 0.8 CO2
1.0E+01
EXP 0.9 CO2
EXP 1CO2
1.0E+00
0.001 0.01 0.1 1 10
Figure 32. H 2S partial pressure of the DIPA-CO2-H 2S-H2O system at 373.15 K,


1.0E+02
H2 S partial pressure, kPa 1.0E+01
EXP 0.05 CO2, 283.15 K
EXP 0.15 CO2, 283.15 K
1.0E+00 EXP 0.3 CO2, 283.15 K
EXP 0.05 CO2, 298.15 K
EXP 0.15 CO2, 298.15 K
EXP 0.3 CO2, 298.15 K
1.0E-01
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7
Figure 33. H 2S partial pressure of the DIPA-CO2-H 2S-H2O system at 283.15 K

and 298.15 K, experimental data from ter Maat et al. (2004) [9]
1.0E+04
1.0E+03
1.0E+02
EXP 313.15 K
1.0E+01 EXP 373.15 K
1.0E+00
0 0.2 0.4 0.6 0.8 1 1.2 1.4
Figure 34. CO2 partial pressure of the sulfolane-DIPA-CO2-H2O system at

313.15 K and 373.15 K, experimental data from Isaacs et al. (1977) [12]
1.0E+04
1.0E+03
1.0E+02
EXP 313.15 K
1.0E+01
EXP 373.15 K
1.0E+00
0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 1.8 2 2.2
Figure 35. H 2S partial pressure of the sulfolane-DIPA-H2S-H 2O system at

313.15 K and 373.15 K, experimental data from Isaacs et al. (1977) [12]

3 Reactions
DIPA is a secondary ethanolamine, as shown in Figure 36. It can associate

with H3O+ to form an ion DIPAH+, and can also react with CO2 to form a
carbamate ion DIPACOO-.
Figure 36. DIPA Molecular Structure
The electrolyte solution chemistry has been modeled with a CHEMISTRY

model with the CHEMISTRY ID = DIPA. 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 DIPA. In addition,
a kinetic REACTION model called DIPA-REA has been created. In DIPA-REA,
all reactions are assumed to be in chemical equilibrium except those of CO 2
with OH- and CO2 with DIPA.
A. Chemistry ID: DIPA

1 Equilibrium DIPAH   H 2 O  DIPA  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 DIPACOO   H 2 O  DIPA  HCO 3
5 Equilibrium 2H 2 O  H 3 O   OH 
6 Equilibrium H 2 O  H 2 S  HS   H 3 O 
7 Equilibrium H 2 O  HS   S 2  H 3 O 
B. Reaction ID: DIPA-REA

1 Equilibrium DIPAH   H 2 O  DIPA  H 3 O 
2 Equilibrium 2H 2 O  H 3 O   OH 
3 Equilibrium HCO 3  H 2 O  CO 32  H 3 O 
26 3 Reactions
4 Kinetic CO 2  OH   HCO 3
5 Kinetic HCO 3  CO 2  OH 
6 Kinetic DIPA  CO 2  H 2 O  DIPACOO -  H 3 O 
7 Kinetic DIPACOO -  H 3 O   DIPA  CO 2  H 2 O
8 Equilibrium H 2 O  H 2 S  HS   H 3 O 
9 Equilibrium H 2 O  HS   S 2  H 3 O 
The equilibrium constants for reactions 1-7 in Chemistry DIPA are calculated
from the standard Gibbs free energy change.
The power law expressions are used for the rate-controlled reactions
(reactions 4-7 in DIPA-REA):
  E  1 1  N
r  k T T0  exp     xi  i  i
n a
(1)
 R  T T0  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;
xi = Mole fraction of component i;
γi = Activity coefficient of component i;
ai = The stoichiometric coefficient of component i in the reaction equation.
If T0 is not specified, the reduced power law expression is used:
E N
r  kT n exp   xi  i  i
a
(2)
 RT  i 1
In this work, the reduced expression is used. In equation (2), the factor n is
zero, and k and E are given in Table 3.
The kinetic parameters for reaction 4 are taken from the work of Pinsent et al.
(1956)[4], and 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.The kinetic parameters for reaction 6 in Table 3
are derived from the work of Blauwhoff et al. (1985) [5]. The kinetic
parameters for reaction 7 are calculated by using the kinetic parameters of
reaction 6 and the equilibrium constants of the reversible reactions 6 and 7.
3 Reactions 27
Table 3. Parameters k and E in Equation (2)
Reaction No. k E , cal/mol
4 1.33E+17 13249
5 6.62E+16 25656
6 1.26E+13 9563.1
7 2.08E+25 18278
28 3 Reactions
4 Simulation Approach
Process simulation is not within the scope of current phase of this work so we
decided to use a single stage flash model to simulate the CO 2 and H2S
absorption by the mixed solvent sulfolane-DIPA-H2O.
Simulation Flowsheet – The absorber has been modeled with the following
simulation flowsheet in Aspen Plus, shown in Figure 37. CO2 and H2S in
stream GASIN are absorbed by the mixed solvent (40 wt% sulfolane + 40
wt% DIPA + 20 wt% H 2O) in stream LEANIN in a FLASH2 block.
Figure 37. Sulfolane-DIPA simulation flowsheet in Aspen Plus
4 Simulation Approach 29
Unit Operations - Major unit operations in this model have been represented
by Aspen Plus blocks as outlined in Table 4.
Table 4. Aspen Plus Unit Operation Blocks Used in the

Sulfolane-DIPA Model
Unit Operation Aspen Plus Block Comments / Specifications
Absorber Flash2 1. Temperature is set at 313.15 K

2. Pressure is set at 10 atm.
Streams - Feeds to the absorber are GASIN containing CO2 and H2S and
LEANIN containing aqueous sulfolane-DIPA solution. Feed conditions are
summarized in Table 5.
Table 5. Feed specifications

Stream ID GASIN LEANIN
Substream: MIXED
Temperature: k 313.15 313.15
Pressure: atm 10 10
Total flow 0.2 kmol/sec 1 kmol/sec
Mole-Frac
SULFOLANE 0 0.191
DIPA 0 0.172
H2O 0 0.637
CO2 0.5 0
H2S 0.5 0
Prop-Sets - A Prop-Set, XAPP, has been created to report apparent mole

fraction of H2S, CO2, DIPA and sulfolane in liquid streams to facilitate
calculations of acid gas loadings of the streams.
30 4 Simulation Approach
5 Simulation Results
The simulation was performed using Aspen Plus. Key simulation results are
presented in Table 6.
Table 6. Key Simulation Results

Stream ID GASOUT RICHOUT
Temperature: K 313.15 313.15

Pressure: atm 10 10
Total flow, kmol/sec 0.0473 1.103
Component flow, kmol/sec
SULFOLANE 8.18E-8 0.191
DIPA 1.16E-10 0.0195
H2O 1.85E-4 0.617
CO2 0.0359 0.015
H2S 0.011 0.020
DIPAH+ 0.0 0.123
DIPACOO- 0.0 0.030
HCO3- 0.0 0.015
CO3-2 0.0 4.19E-3
HS- 0.0 0.0687
S2- 0.0 1.48E-5
5 Simulation Results 31
6 Conclusions
The sulfolane-DIPA model provides a thermodynamic basis for rigorous

simulation of acid gas removal process. Key features of this model include
electrolyte thermodynamics and solution chemistry, reaction kinetics for the
liquid phase reactions and rigorous transport property modeling.
The model is meant to be used as a guide for modeling the CO 2 capture
process with aqueous sulfolane-DIPA solution. You may use it as a starting
point for more sophisticated models for process development,
debottlenecking, plant and equipment design, among other uses. Further
validation of this sulfolane-DIPA model will be done when industrial or pilot
plant data become available.
32 6 Conclusions
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36 References

ENRTL-RK Rate Based Sulfolane-DIPA Model

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Aspen Plus

Aspen Plus Sulfolane-DIPA Model

Aspen Technology, Inc.

V7.3 First version

4 Simulation Approach ..........................................................................................29

5 Simulation Results .............................................................................................31

The following components represent the chemical species present in the

Table 1. Components Used in the Model

SULFOLAN Conventional SULFOLANE C4H8O2S

The unsymmetric electrolyte NRTL property method (ENRTL-RK) and PC-SAFT

Table 2. Henry’s constants

CO2 H2 O Yan and Chen (2010) [6]

2 Physica l Prope rties 5

2 Physica l Prope rties 7

EXP DIPA 10.1 w t% (298.03 K)

Figure 1. Liquid density of DIPA-CO2-H2O at around 298.15 K, experimental

EST DIPA 10wt%

Figure 2. Liquid density of DIPA-H2S-H2O at 298.15 K

Figure 3. Liquid density of sulfolane-DIPA-CO2-H2O at 298.15 K

Figure 4. Liquid density of sulfolane-DIPA-H2S-H2O at 298.15 K

2 Physica l Prope rties 9

Figure 5. Liquid viscosity of DIPA-CO2-H 2O at 298.15 K

Figure 6. Liquid viscosity of DIPA-H2S-H 2O at 298.15 K

EST Sulfolane 5wt%+DIPA 5wt%

Figure 7. Liquid viscosity of sulfolane-DIPA-CO2-H 2O at 298.15 K

EST Sulfolane 5wt%+DIPA 5wt%

Figure 8. Liquid viscosity of sulfolane-DIPA-H2S-H 2O at 298.15 K

2 Physica l Prope rties 11

Surface Tension, N/m

Figure 9. Surface tension of DIPA-CO2-H2O at 298.15 K

Figure 10. Surface tension of DIPA-H 2S-H 2O at 298.15 K

0.02 EST Sulfolane 5wt%+DIPA 5wt%

Figure 11. Surface tension of sulfolane-DIPA-CO2-H 2O at 298.15 K

0.02 EST Sulfolane 5wt%+DIPA 5wt%

Figure 12. Surface tension of sulfolane-DIPA-H 2S-H 2O at 298.15 K

2 Physica l Prope rties 13

Thermal Cnductivity, Watt/m-K

EST DIPA 10wt%

Figure 13. Liquid thermal conductivity of DIPA-CO2-H2O at 298.15 K

Figure 14. Liquid thermal Conductivity of DIPA-H2S-H2O at 298.15 K

Thermal Cnductivity, Watt/m-K

EST Sulfolane 5wt%+DIPA 5wt%

Figure 15. Liquid thermal conductivity of sulfolane-DIPA-CO2-H2O at 298.15 K

EST Sulfolane 5wt%+DIPA 5wt%

Figure 16. Liquid thermal conductivity of sulfolane-DIPA-H2S-H2O at 298.15 K

2 Physica l Prope rties 15

Figure 17. Liquid heat capacity of DIPA-CO2-H 2O at 298.15 K

Figure 18. Liquid heat Capacity of DIPA-H 2S-H 2O at 298.15 K

1000 EST Sulfolane 5wt%+DIPA 5wt%

Figure 19. Liquid heat capacity of sulfolane-DIPA-CO2-H2O at 298.15 K

1000 EST Sulfolane 5wt%+DIPA 5wt%

Figure 20. Liquid heat capacity of sulfolane-DIPA-H2S-H2O at 298.15 K

2 Physica l Prope rties 17

Integral Heat of Solution, J/mol

-120000 EST DIPA 10wt%

Figure 21. Integral heat of solution of CO 2 in DIPA-H 2O at 298.15 K

Figure 22. Integral heat of solution of H 2S in DIPA-H 2O at 298.15 K

Integral Heat of Solution, J/mol

-120000 EST Sulfolane 5wt%+DIPA 5wt%

Figure 23. Integral heat of solution of CO 2 in sulfolane-DIPA-H 2O at 298.15 K

-60000 EST Sulfolane 5wt%+DIPA 5wt%

Figure 24. Integral heat of solution of H 2S in sulfolane-DIPA-H 2O at 298.15 K

2 Physica l Prope rties 19

CO 2 partial pressure, kPa 1.0E+02