Aspen Plus

Rate-Based Model of the CO2 Capture Process by

PZ using Aspen Plus
Copyright (c) 2008-2014 by Aspen Technology, Inc. All rights reserved.

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This software includes NIST Standard Reference Database 103b: NIST Thermodata Engine Version 7.1

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Revision History
Version Description

V7.1 First version

V7.1 CP1 1. Add O2, CO and H2 to the model as Henry components
2. Two corrections in the model:
(1) ID of the Henry Comp group: PZ-MEA (V7.1)  PZ(V7.1 CP1)
(2) VLQKIJ was missed in V7.1 and now it’s added
V7.2 Update Henry’s constant of CO2 in H2O by fitting VLE data of Takenouchi
(1964), Tödheide(1963), Dodds (1956), Drummond (1981), Zawisza
(1981), Wiebe (1940) and Houghton (1957).
Update NRTL parameters between PZ and H2O by fitting VLE data of
Wilson (1994), Kamps (2003) and Hilliard (2008), and heat capacity
data of Hilliard (2008).
Determine DGAQFM, DHAQFM, CPAQ0 of PZH+, PZCOO-, PZ(COO-)2 and
HPZCOO by fitting VLE data of Ermatchkov (2006) and Hilliard (2008),
absorption heat data of Hilliard (2008) and heat capacity data of Hilliard
(2008) together with the interaction energy parameters between H2O
and (PZH+, HCO3-) and those between H2O and (PZH+, PZCOO-).
Update the figures for properties.
Calculate chemical equilibrium constants from Gibbs free energy,
Update kinetics.
Update Simulation results.
Update figure 3 for surface tension and update reference for PZ surface
tension data from Moerke (1982).
V7.3 Update databank to PURE25.
Add missing transport properties parameters in the bkp file to be
consistent with the documentation.
Add the definition of acid gas loading and amine weight fraction
convention.
Update Figure 3b.
V7.3.2 Update databank to PURE26.
V8.0 Update databank to PURE27.
V8.2 Update databank to PURe28.
Update the simulation results.
V8.6 Update databank to PURE32.

Revision History 1
Contents
Revision History ......................................................................................................1

Contents..................................................................................................................2

Introduction ............................................................................................................3

1 Components .........................................................................................................4

2 Physical Properties...............................................................................................5

3 Reactions ...........................................................................................................12

4 Simulation Approach ..........................................................................................15

5 Simulation Results .............................................................................................17

6 Conclusions ........................................................................................................18

References ............................................................................................................19

2 Contents
Introduction

This file describes an Aspen Plus rate-based model of the CO2 capture process
by aqueous piperazine (PZ) solution. As there are no industrial or pilot plant
data publicly available for the CO2 capture process using aqueous PZ, a flash
model is used to test the feasibility of CO2 absorption from a gas stream
containing CO2 and N2 by PZ. Thermophysical property models and reaction
kinetic models are based on the recent works of Hilliard (2008)[1] and Bishnoi
and Rochelle (2000, 2002)[2,3]. Transport property models and model
parameters have been validated against available experimental data from
open literature.
The model 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

Introduction 3
1 Components

The following components represent the chemical species present in the

process:

Table 1. Components Used in the Model

ID Type Name Formula

PZ Conventional PIPERAZINE C4H10N2

H2O Conventional WATER H2O
CO2 Conventional CARBON-DIOXIDE CO2
H3O+ Conventional H3O+ H3O+
OH- Conventional OH- OH-
HCO3- Conventional HCO3- HCO3-
CO3-2 Conventional CO3-- CO3-2
PZH+ Conventional PZH+ C4H11N2+
PZH+2 Conventional PZH+2 C4H12N2+2
HPZCOO Conventional HPZCOO C5H10NO2
PZCOO- Conventional PZCOO- C5H9N2O2-
PZCOO-2 Conventional PZCOO-2 C6H8N2O4-2
N2 Conventional NITROGEN N2
O2 Conventional OXYGEN O2
CO Conventional CARBON-MONOXIDE CO
H2 Conventional HYDROGEN H2

4 1 Components
2 Physical Properties

The electrolyte NRTL method and RK equation of state are used to compute
liquid and vapor properties, respectively, in this rate-based PZ model. CO2,
N2, O2, CO and H2 are selected as Henry-components to which Henry’s law is
applied. Henry’s constants are specified for these components with water. 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 (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 Henry’s constant parameters of CO2 in water are regressed with the
binary VLE data[4-10]. The NRTL interaction parameters between CO2 and H2O
are set to zero, and those between PZ and H2O are obtained by fitting the
binary VLE data[1, 11, 12] and heat capacity data[1].
The interaction energy parameters between H2O and (PZH+, HCO3-) and those
parameters between H2O and (PZH+, PZCOO-), GMELCC, are regressed using
the heat of solution data of CO2 in aqueous PZ solution from Hilliard (2008)[1],
heat capacity data of CO2 loaded aqueous PZ solution from Hilliard (2008)[1]
and CO2 solubility data in aqueous PZ solution from Ermatchkov et al.
(2006)[13] and Hilliard (2008)[1].
The dielectric constants of nonaqueous solvents are calculated by the
following expression:

1 1
 T   A  B   (1)
T C 
The parameters A, B and C for PZ in Aspen databanks are 11.26958, 8796
and 298.15.
The liquid molar volume model and transport property models have been
validated and model parameters regressed when literature experimental data
are available. Specifications of the transport property models 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
PZ and H2O is regressed against experimental PZ-H2O density data from
Arunkumar and Syamalendu (2006)[14] and the data from Derks et al.
(2005)[15]. There are no density data available for the CO2-PZ-H2O system,
so no regression can be done for the Clarke model parameter VLCLK/1 of

2 Physical Properties 5
 the main electrolytes, such as (PZH+, HCO3-), (PZH+, PZCOO-) and (PZH+,
PZ(COO-)2).
 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 PZ 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. Arunkumar and Syamalendu
(2006)[14] and Derks et al. (2005)[15] reported some experimental viscosity
data for aqueous PZ solutions, which are no more concentrated than
15wt%. Regressed interaction parameters between PZ and H2O in the
Aspen liquid mixture viscosity model, MUKIJ and MULIJ, from these low
concentration data can result in unreasonable predictions for concentrated
solutions, so we leave these two interaction parameters between PZ and
H2O defaulted at zero. There are no viscosity data available for the CO2-
PZ-H2O system, so no regression can be done for the Jones-Dole model
parameters, IONMUB, for PZH+, PZCOO- and PZ(COO-)2. IONMUB of HCO3-
is regressed against KHCO3-H2O viscosity data from Palaty (1992)[16] and
that of CO32- is regressed against K2CO3-H2O viscosity data from Pac et al.
(1984)[17].
 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. The parameters of PZ for
the DIPPR liquid surface tension equation are regressed to fit the pure PZ
surface tension experimental data[18].
 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 aqueous
phase Gibbs free energy and heat of formation at infinite dilution and 25°C
(DGAQFM and DHAQFM) of PZH+ are determined from the dissociation
constant of PZ[19]. DGAQFM and DHAQFM of HPZCOO, PZCOO- and PZ(COO-)2,
and heat capacity at infinite dilution (CPAQ0) of PZH+, HPZCOO, PZCOO- and
PZ(COO-)2 are determined by fitting the CO2 absorption heat data[1], heat
capacity data[1] and CO2 solubility data[1, 13]
The estimation results of various transport and thermal properties are
summarized in Figures 1-7. Note that CO2 loading is defined as the ratio of
the moles of apparent CO2 to the moles of apparent PZ. Apparent means
before reaction, so for example if 1 mole of PZ 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 PZ after reacting. Weight percent of PZ is calculated without
CO2, so in the above example, it is calculated from the mixture of 1 mole of
PZ and 9 moles of water. Since PZ has a molecular weight of 86.1369 and
water has a molecular weight of 18.015, this is 86.1369/(86.1369+9*18.015)
= 0.34694 or about 35 wt% PZ.

6 2 Physical Properties
 1100

1050

1000

Density, kg/m3
950
EXP05 298K
EXP06 298K
900 EST 298K
EXP05 313K
EXP06 313K
850 EST 313K
EXP05 323K
EXP06 323K
EST 323K
800 EST 298.15K
0 0.2 0.4 0.6 0.8 1
PZ Mass Fraction

Figure 1a. Liquid Density of PZ-H2O, experimental data from Arunkumar and
Syamalendu (2006)[4] and Derks et al. (2005)[5]

1030

1020

1010
Density, kg/m3

1000

990

980

970
EST PZ=2m LD=0.16
960 EST PZ=2m LD=0.27
950
20 40 60 80 100 120 140
Tem perature, C

Figure 1b. Liquid Density of PZ-CO2-H2O. ‘LD’ denotes CO2 loading.

2 Physical Properties 7
 10 EXP05 298K
EXP06 298K
EST 298K
EXP05 313K
EXP06 313K
EST 313K
EXP05 323K

Viscosity, mPaS
EXP06 323K
EST 323K
1

0.1
0 0.2 0.4 0.6 0.8 1
PZ Mass Fraction

Figure 2a. Liquid Viscosity of PZ-H2O, experimental data from Arunkumar

and Syamalendu (2006)[4] and Derks et al. (2005)[5]

1
Viscosity, mPaS

EST PZ=2m LD=0.16

EST PZ=2m LD=0.27

0.1
20 40 60 80 100 120 140
Tem perature, C

Figure 2b. Liquid Viscosity of PZ-CO2-H2O. ‘LD’ denotes CO2 loading.

8 2 Physical Properties
 0.05

0.04

Surface Tension, N/m

0.03

0.02 EXP
EST
0.01

0
250 300 350 400 450
T, K

Figure 3a. Surface tension of pure PZ, experimental data from Moerke and
Roscher (1982)[18]

0.07

0.06
Surface tension, N/m

0.05

0.04

0.03
EST, LD = 0.16
0.02 EST, LD = 0.27

0.01

0
20 40 60 80 100 120 140

Temperature, C

Figure 3b. Surface tension of PZ-CO2-H2O (PZ concentration is 2m). ‘LD’

denotes CO2 loading.

2 Physical Properties 9
 0.5

0.45

Thermol Conductivity, Watt/m-K

0.4

0.35
0.3

0.25
0.2

0.15
0.1 EST PZ=2m LD=0.16
0.05 EST PZ=2m LD=0.27

0
20 40 60 80 100 120 140
Tem perature, C

Figure 4. Liquid Thermal Conductivity of PZ-CO2-H2O. ‘LD’ denotes CO2

loading.

4.5

3.5
Heat capacity, kJ/kg.K

2.5

2
EXP Loading = 0.31
1.5
EST Loading = 0.31
1 EXP Loading = 0.80
0.5 EST Loading = 0.80

0
300 320 340 360 380 400

Temperature, K

Figure 5. Liquid Heat Capacity of PZ-CO2-H2O (PZ concentration is 2m),

experimental data from Hilliard (2008)[1]. ‘LD’ denotes CO2 loading.

10 2 Physical Properties
 120

100

Absorption heat, kJ/mol CO2

80

60

40 EX P 40C
EX P 80C
EX P 120C
ES T 40C
20 ES T 80C
ES T 120C

0
0 0.2 0.4 0.6 0.8 1 1.2

CO2 loading

Figure 6 Differential CO2 absorption heat in aqueous PZ solution (PZ

concentration is 2.4m) , experimental data from Hilliard (2008)[1]

100
EX P 40C
ES T 40C
EX P 60C
10 ES T 60C
CO2 pressure, kPa

0.1

0.01
0 0.2 0.4 0.6 0.8 1

CO2 loading

Figure 7. CO2 Partial Pressure of PZ-CO2-H2O (PZ concentration is 2m),

experimental data from Hilliard (2008)[1]

2 Physical Properties 11
3 Reactions

PZ is a cyclic amine, as shown in Figure 8. It can associate with H3O+ to form

an ion PZH+, and can also react with CO2 to form a carbamate ion PZCOO-
and a dicarbamate ion PZ(COO-)2.

Figure 8. PZ Molecular Structure

The electrolyte solution chemistry has been modeled with a CHEMISTRY
model with CHEMISTRY ID = PZ. 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 PZ. In addition, a
REACTION model called PZ-REA has been created. In PZ-REA, all reactions
are assumed to be in chemical equilibrium except those of CO2 with OH- and
CO2 with PZ and PZCOO-.

A. Chemistry ID: PZ
1 Equilibrium 2H 2 O  H 3 O   OH 
2 Equilibrium CO 2  2H 2 O  HCO 3  H 3 O 
3 Equilibrium HCO 3  H 2 O  CO 32   H 3 O 
4 Equilibrium PZH   H 2 O  PZ  H 3 O 
5 Equilibrium PZ  HCO 3-  PZCOO -  H 2 O
6 Equilibrium HPZCOO  H2O  PZCOO -  H 3 O 
7 Equilibrium 
PZCOO -  HCO 3-  PZ COO - 
2  H 2O

B. Reaction ID: PZ-REA

1 Equilibrium 2H 2 O  H 3 O   OH 

12 3 Reactions
 2 Equilibrium HCO 3  H 2 O  CO 32   H 3 O 
3 Equilibrium PZH   H 2 O  PZ  H 3 O 
4 Equilibrium HPZCOO  H 2 O  PZCOO   H 3 O 
5 Kinetic CO 2  OH   HCO 3
6 Kinetic HCO 3  CO 2  OH 
7 Kinetic PZ  CO 2  H 2 O  PZCOO -  H 3 O 
8 Kinetic PZCOO -  H 3 O   PZ  CO 2  H 2 O
9 Kinetic PZCOO -  CO 2  H 2 O  PZ (COO - ) 2  H 3 O 
10 Kinetic PZ(COO - ) 2  H 3 O   PZCOO -  CO 2  H 2 O
The equilibrium constants are calculated from the standard Gibbs free energy
change. DGAQFM, DHAQFM and CPAQ0 of PZH+, PZCOO-, PZ(COO-)2 and
HPZCOO, which are used to calculate the standard Gibbs free energy, are
determined in this work. 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.
The power law expressions (T0 not specified) are used for the rate-controlled
reactions (reactions 5-10 in PZ-REA):

  E  1 1  N
r  k T T0  exp     C i i
n a
(2)
 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;
Ci = Concentration 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 (  ) C i i
a
(3)
RT i 1

3 Reactions 13
 In this work, the reduced expression is used. In equation (3), the
concentration basis is Molarity, the factor n is zero, k and E are given in
Table 2.
The kinetic parameters for reaction 5 are taken from the work of Pinsent et al.
(1956)[20] , and the kinetic parameters for reaction 6 are calculated by using
the kinetic parameters of reaction 5 and the equilibrium constants of the
reversible reactions 5 and 6. The kinetic parameters for reactions 7-10 in
Table 2 are derived from the work of Bishnoi and Rochelle (2000, 2002)[2,3].

Table 2. Parameters k and E in Equation (1)

Reaction No. k E , cal/mol
5 4.32e+13 13249
6 2.38e+17 29451
7 4.14e+10 8038.3
8 7.94e+21 15758
9 3.62e+10 8038.3
10 5.56e+25 18372

14 3 Reactions
4 Simulation Approach

As we are unable to find industrial or pilot plant data publicly available for the
aqueous PZ Separation process, we use a single equilibrium stage model
(flash calculations) to simulate the CO2 absorption by PZ.
Simulation Flowsheet – In the following simulation flowsheet in Aspen Plus
(Figure 9), CO2 is absorbed by PZ from a mixture of CO2 and N2 in an
absorber.

GASOUT

LEANIN
ABSOR BER

GASIN

RIC HOUT

Figure 9. PZ Simulation Flowsheet in Aspen Plus

4 Simulation Approach 15
 Unit Operations - Major unit operations in this model have been represented
by Aspen Plus blocks as outlined in Table 3.

Table 3. Aspen Plus Unit Operation Blocks Used in the PZ

Model
Unit Aspen Plus Block Comments / Specifications
Operation
Flash Flash2 1. Temperature is set at 40 °C
2. Pressure is set at 1 atm

Streams - Feeds to the absorber are gas stream GASIN containing N2 and
CO2 and liquid solvent stream LEANIN containing aqueous PZ solution. Feed
conditions are summarized in Table 4.

Table 4. Feed specifications

Stream ID GASIN LEANIN

Substream: MIXED
Temperature: °C 40 40
Pressure: atm 1 1
Flow rate mole/hr mole/hr
H2O 0 72000
PZ 0 3000
CO2 3000 300
N2 27000 0

Prop-Sets – Prop-Set XAPP is used to report apparent mole fraction of CO2,

N2, PZ and H2O in liquid streams

16 4 Simulation Approach
5 Simulation Results

The simulation has been run successfully in Aspen Plus. Key simulation results
are presented in Table 5. Here the RICHOUT compositions are the mole
fraction of apparent components.

Table 5. Key Simulation Results

Stream ID GASOUT RICHOUT

Substream: MIXED
Temperature: °C 40 40
Pressure: psig 0 0
Total flow 30100 mol/hr 72878 mol/hr
Mole-Frac Mole-Frac
H2O 0.071 0.929
PZ 0 0.040
CO2 0.031 0.031
N2 0.898 0

5 Simulation Results 17
6 Conclusions

The Rate-Based PZ model provides a simple simulation of the CO2 capture

process using aqueous PZ solutions with rigorous electrolyte thermodynamics
and solution chemistry and reaction kinetics for the liquid phase reactions.
The model is meant to be used as a guide for modeling the CO2 capture
process with PZ. Users may use it as a starting point for more sophisticated
models for process development, debottlenecking, plant and equipment
design, among others. This simple PZ model has been validated with limited
experimental thermophysical and transport properties data. Further validation
of this PZ model will be done when industrial or pilot plant data become
available, as well as more transport property data.

18 6 Conclusions
References

[1] M.D. Hilliard, "A Predictive Thermodynamic Model for an Aqueous Blend of
Potassium Carbonate, Piperazine, and Monoethanolamine for Carbon Dioxide
Capture from Flue Gas", Ph.D. Dissertation, University of Texas at Austin,
(2008)
[2] S. Bishnoi, G. Rochelle, “Absorption of Carbon Dioxide into Aqueous
Piperazine: Reaction Kinetics, Mass Transfer and Solubility”, Chemical
Engineering Science, 55, 5531-5543 (2000)
[3] S. Bishnoi, G. Rochelle, “Absorption of Carbon Dioxide into Aqueous
Piperazine/Methyldiethanolamine”, AIChE Journal, 48, 2788-2799 (2002)
[4] S. Takenouchi and G.C. Kennedy, “The Binary System H2O–CO2 at High
Temperatures and Pressures”. Am. J. Sci., 262, 1055–1074 (1964)
[5] K. Tödheide and E.U. Franck, Zeitschrift fur Physikalische Chemie Neue
Folge, BD. 37, S.387-401 (1963)
[6] W.S. Dodds, L.F. Stutzman and B.J. Sollami, "Carbon Dioxide Solubility in
Water", industrial and engineering chemistry, 1 (1), 92-95 (1956)
[7] S.E. Drummond, “Boiling and Mixing of Hydrothermal Fluids: Chemical
Effects on Mineral Precipitation”, Ph.D. Thesis, Pennsylvania State University,
(1981)
[8] A. Zawisza and B. Malesiska, “Solubility of Carbon Dioxide in Liquid Water
and of Water in Gaseous Carbon Dioxide in the Range 0.2-5 Mpa and at
Temperature up to 473K", J. Chem. Eng. Data, 26, 388-391 (1981)
[9] R. Wiebe and V.L. Gaddy, “The solubility of Carbon Dioxide in Water at
Various Temperatures from 12 to 40 ◦C and at Pressures to 500 atm”, J. Am.
Chem. Soc., 62, 815–817 (1940)
[10] G. Houghton, A.M. Mclean, and P.D. Ritchie, "Compressibility, Fugacity,
and Water-solubility of Carbon Dioxide in the Region 0-36 atm and 0-100 C",
Chemical engineering science, 6, 132-137 (1957)
[11] H. L. Wilson, W. V. Wilding, “Vapor-Liquid and Liquid-Liquid Equilibrium
Measurements on Twenty-two Binary Mixtures”, DIPPR Data Ser., 2. 63-
115(1994)
[12] A. P.–S. Kamps, J.–Z. Xia, G. Maurer, “Solubility of CO2 in (H2O +
Piperazine) and in (H2O-MDEA-Piperazine)”, AIChE J. 49, 2662-2670(2003)

References 19
 [13] V. Ermatchkov, A. P.–S. Kamps, S. Speyer, G. Maurer, “Solubility of
Carbon Dioxide in Aqueous Solutions of Piperazine in the Low Gas Loading
Region”, J. Chem. Eng. Data., 51, 1788-1796(2006)
[14] S. Arunkumar, S.B. Syamalendu, "Density and Viscosity of Aqueous
Solutions of Piperazine and (2-Amino-2-methyl-1-propanol + Piperazine) from
298 to 333 K ", J. Chem. Eng. Data, 51, 467- 470 (2006)
[15] P.W.J. Derks, K.J. Hogendoorn, G.F. Versteeg, "Solubility of N2O in and
density, viscosity, and surface tension of aqueous piperazine solutions", J.
Chem. Eng. Data, 50, 1947-1950 (2005)
[16] Z. Palaty, “Viscosity of diluted aqueous K2CO3/KHCO3 solutions”, Collect.
Czech. Chem. Commun., 57, 1879 (1992)
[17] 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)
[18] Moerke, K., Roscher, T., “Determination of the surface tension of some
ethyleneamines”, Leuna protocol, 9101 (1982)
[19] E. S. Hamborg, G. F. Versteeg, “Dissociation Constants and
Thermodynamic Properties of Amines and Alkanolamines from (293 to 353)
K”, J. Chem. Eng. Data, 54, 1318-1328(2009)
[20] B.R. Pinsent, L. Pearson, F.J.W. Roughton, “The Kinetics of Combination
of Carbon Dioxide with Hydroxide Ions”, Trans. Faraday Soc., 52, 1512-1520
(1956)

20 References