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Revision History 1
Contents
Revision History ......................................................................................................1
Contents..................................................................................................................2
Introduction ............................................................................................................3
1 Components .........................................................................................................4
2 Physical Properties...............................................................................................5
3 Reactions ...........................................................................................................16
6 Conclusions ........................................................................................................22
References ............................................................................................................23
2 Contents
Introduction
This file describes an Aspen Plus model of the CO2 and H2S capture process by
mixed solvent composed of sulfolane, MDEA 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-MDEA 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 and Rinker et al.
(1997)[4] and Pinsent et al. (1956) [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
4 1 Components
2 Physical Properties
6 2 Physical Properties
between sulfolane and H 2O is validated by experimental sulfolane-H2O
density data from the literature[14,30,43-52]. The Clarke model parameter
VLCLK/1 is also regressed for main electrolytes (MDEAH+, HCO 3 ) and
(MDEAH+, CO3-2 ) against experimental density data of the MDEA-H2O-CO2
system from Weiland et al. (1998)[53], and that for (MDEAH +, HS-) is
regressed against experimental data of the MDEA-H2O-H2S system from
Rinker et al. (2000) [54]. The Clarke model parameters VLCLK/1 are left to
the default for other electrolytes.
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-MDEA model always uses the
Jones-Dole correction model. 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 MDEA and H2O in the ASPEN liquid mixture viscosity
model, MUKIJ and MULIJ, are regressed against experimental MDEA-H2O
viscosity data from Teng et al. (1994)[55]. MUKIJ and MULIJ for sulfolane-
H2O binary are regressed against experimental sulfolane-H2O viscosity
data from the literature[14,43-51,56]. The Jones-Dole model parameter,
IONMUB, for MDEAH+ is regressed against MDEA-H2O-CO2 viscosity data
from Weiland et al. (1998)[53], that of CO3-2 is regressed against K2CO3-
H2O viscosity data from Pac et al. (1984)[57], that of HCO3- is regressed
against KHCO3-H2O viscosity data from Palaty (1992)[58] and that of HS - is
regressed against MDEA-H2O-H2S viscosity data from Rinker et al.
(2000)[54].
For liquid surface tension, the Onsager-Samaras model, called SIG2ONSG
in Aspen Plus, is used with its option codes set to -9 (exponent in mixing
rule) and 1 (electrolyte system). The predictions of surface tension of the
MDEA-H2O-CO2 system can be in the range of the experimental data from
Weiland (1996)[59]. No additional adjusted parameters are used in the
surface tension model.
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 liquid volume and transport
properties, the aqueous phase Gibbs free energy (DGAQFM) and enthalpy
(DHAQFM) of formation at infinite dilution at 298.15 K and the heat capacity
at infinite dilution (CPAQ0) for MDEAH+ are regressed with VLE[31-33], heat of
absorption[34,35], heat capacity[36] and liquid phase concentration data[37]. 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 (1964)[60], and that of
S-2 is calculated from the Criss-Cobble correlation[60] with the entropy value
from Wagman et al. (1982) [61].
As the estimation results of various transport and thermal properties for the
MDEA-CO2/H2S-H2O ternary system have been summarized in the Aspen
1200
1000
800
Density, kg/m3
600
400
EST Sulfolane 5wt%+MDEA 5wt%
200 EST Sulfolane 10wt%+MDEA 10wt%
EST Sulfolane 15wt%+MDEA 15wt%
EST Sulfolane 20wt%+MDEA 20wt%
0
0 0.1 0.2 0.3 0.4 0.5
CO2 loading (m ol CO2/ m ol MDEA)
1200
1000
800
Density, kg/m3
600
400
EST Sulfolane 5wt%+MDEA 5wt%
200 EST Sulfolane 10wt%+MDEA 10wt%
EST Sulfolane 15wt%+MDEA 15wt%
EST Sulfolane 20wt%+MDEA 20wt%
0
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/m ol MDEA)
8 2 Physical Properties
0.01
Viscosity, PaS
0.001
0.0001
0 0.1 0.2 0.3 0.4 0.5
CO2 loading (m ol CO2/ m ol MDEA)
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 MDEA)
0.07
0.06
Surface Tension, N/m
0.05
0.04
0.03
0
0 0.1 0.2 0.3 0.4 0.5
CO2 loading (m ol CO2/ m ol MDEA)
0.08
0.07
0.06
Surface Tension, N/m
0.05
0.04
0.03
0
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/ m ol MDEA)
10 2 Physical Properties
0.6
0.5
0.3
0.2
0.6
0.5
Thermal Cnductivity, Watt/m-K
0.4
0.3
0.2
4500
4000
Heat Capacity, J/kg-K 3500
3000
2500
2000
1500
5000
4500
4000
Heat Capacity, J/kg-K
3500
3000
2500
2000
1500
1000 EST Sulfolane 5wt%+MDEA 5wt%
EST Sulfolane 10wt%+MDEA 10wt%
500 EST Sulfolane 15wt%+MDEA 15wt%
EST Sufolane 20wt%+MDEA 20wt%
0
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/ m ol MDEA)
12 2 Physical Properties
0
-20000
-60000
-80000
-100000
-10000
Integral Heat of Solution, J/mol
-20000
-30000
-40000
-50000
-80000
0 0.1 0.2 0.3 0.4 0.5
H2S loading (m ol H2S/ m ol MDEA)
1.0E+03
EXP 313.15 K
1.0E+01
EXP 373.15 K
1.0E+00
1.0E-01
0 0.5 1 1.5 2
CO2 loading (m ol CO2/ m ol MDEA)
1.0E+04
1.0E+03
H2 S partial pressure, kPa
1.0E+02
1.0E+01
EXP 313.15 K
EXP 373.15 K
1.0E+00
1.0E-01
0 0.5 1 1.5 2 2.5
H2S loading (m ol H2S/ m ol MDEA)
14 2 Physical Properties
1.0E+05
1.0E+03
1.0E+01
1.0E+01 1.0E+02 1.0E+03 1.0E+04 1.0E+05
Experim ental gas partial pressure, kPa
2 Equilibrium 2H 2 O H 3 O OH
3 Equilibrium CO 2 2H 2 O HCO 3 H 3 O
4 Equilibrium HCO 3- H 2 O CO 32 H 3 O
5 Equilibrium H 2 S H 2 O HS H 3 O
6 Equilibrium HS - H 2 O S 2 H 3 O
16 3 Reactions
B. Reaction ID: MDEA-REA
1 Equilibrium MDEAH H 2 O MDEA H 3 O
2 Equilibrium 2H 2 O H 3 O OH
3 Equilibrium HCO 3- H 2 O CO 32 H 3 O
4 Equilibrium H 2 S H 2 O HS H 3 O
5 Equilibrium HS - H 2 O S 2 H 3 O
6 Kinetic CO 2 OH - HCO 3
7 Kinetic HCO 3 CO 2 OH
8 Kinetic MDEA CO 2 H 2 O MDEAH HCO 3-
9 Kinetic MDEAH HCO 3- MDEA CO 2 H 2 O
The equilibrium constants for reactions 1-6 in MDEA are calculated from the
standard Gibbs free energy change. DGAQFM, DHAQFM and CPAQ0 of
MDEAH+, which are used to calculate the standard MDEAH+ Gibbs free energy,
are obtained from Zhang and Chen (2010) [1]. The DGAQFM (or DGFORM),
DHAQFM (or DHFORM) and CPAQ0 (or CPIG) parameters of the other
components can be obtained from the databank of Aspen Plus[3].
The power law expressions are used for the rate-controlled reactions
(reactions 6-9 in MDEA-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:
3 Reactions 17
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 6 in Table 3 are taken from the work of
Pinsent et al. (1956)[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. The kinetic parameters for reaction 8 are
taken from the work of Rinker et al. (1997)[4] and the kinetic parameters for
reaction 9 are calculated by using the kinetic parameters of reaction 8 and
the equilibrium constants of the reversible reactions 8 and 9.
18 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-MDEA-H2O.
Simulation Flowsheet – The absorber has been modeled with the
simulation flowsheet in Aspen Plus shown in Figure 17. CO2 and H2S in stream
GASIN are absorbed by the mixed solvent (40 wt% sulfolane + 40 wt% MDEA
+ 20 wt% H2O) in stream LEANIN in a FLASH2 block.
4 Simulation Approach 19
Unit Operations - Major unit operations in this model have been represented
by Aspen Plus blocks as outlined in Table 4.
Streams - Feeds to the absorber are GASIN containing CO2 and H2S and
LEANIN containing aqueous sulfolane-MDEA solution. Feed conditions are
summarized in Table 5.
20 4 Simulation Approach
5 Simulation Results
The simulation was performed using Aspen Plus. Key simulation results are
presented in Table 6.
5 Simulation Results 21
6 Conclusions
22 6 Conclusions
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Re fere nces 27