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Aspen Plus

Rate-Based Model of the CO2 Capture Process by


NH3 using Aspen Plus
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Revision History
Version Description

V7.3.2 First version.


V8.0 Update databank to PURE27.
V8.2 Update databank to PURE28.
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 ...........................................................................................................13

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

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

6 Conclusion..........................................................................................................18

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

2 Contents
Introduction

This file describes an Aspen Plus model for the CO2 capture process by NH3.
This model consists of an absorber and a stripper. As there are no industrial
or pilot plant data available for aqueous ammonia separation processes,
single stage flash model is used for both the absorber and the stripper to
simulate the feasibility of CO2 removal by ammonia. The thermophysical
properties, transport properties and reaction kinetic models are based on the
works of Que and Chen (2011)[1] and Pinsent et al. (1956)[2] and, wherever
possible, 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 phase
nonideality and PC-SAFT equation of state for vapor phase
 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 NH3 Model


ID Type Name Formula

H2O Conventional WATER H2O


NH3 Conventional AMMONIA H3N
CO2 Conventional CARBON-DIOXIDE CO2
H3O+ Conventional H3O+ H3O+
OH- Conventional OH- OH-
NH4+ Conventional NH4+ NH4+
NH2COO- Conventional CARBAMATE NH2COO-
HCO3- Conventional HCO3- HCO3-
CO3-2 Conventional CO3-- CO3-2
N2 Conventional NITROGEN N2
O2 Conventional OXYGEN O2
CO Conventional CARBON-MONOXIDE CO
H2 Conventional HYDROGEN H2
NH4HCO3S Solid AMMONIUM-HYDROGEN-CARBONATE NH4HCO3

4 1 Components
2 Physical Properties

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


of state are used to compute liquid and vapor properties respectively in this
NH3 model. Henry’s law is applied to CO2, NH3, N2, O2, CO, and H2. 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
are calculated based on infinite-dilution condition in pure water, instead of in
mixed solvents.
The NRTL parameters and Henry’s law constant parameters for NH3 and water
have been regressed simultaneously against VLE data[3-7], enthalpy data[8],
and heat capacity data[9,10] of the NH3-H2O binary system.
The NRTL parameters for CO2 and water are set to zero. Henry’s law constant
for CO2 and water are taken from Yan and Chen (2010)[11] . Henry’s law
constant parameters for the other Henry components with water are retrieved
from Aspen Plus Databanks.
The NRTL parameters for major molecule-electrolyte pairs, such as H2O -
(NH4+, HCO3-), H2O - (NH4+, NH2COO-), H2O - (NH4+, CO3-2), and NH3 - (NH4+,
NH2COO-), and crystalline solid phase Gibbs energy and enthalpy of formation,
and heat capacity for the NH4HCO3 solid have been regressed simultaneously
against all the following data:
 VLE data of the NH3-H2O-CO2 system form 313 K to 373 K[12-13]
 Heat capacity data of the NH4HCO3-H2O system at 298 K[10]
[14]
 Speciation data of the (NH4)2CO3-H2O system from 298 K
 Solubility data of NH4HCO3 solid in water from 293 K to 323 K[15]
Heat capacities at infinite dilution (CPAQ0) of all species are assumed
constant, i.e., independent of temperature. CPAQ0 of H3O+, OH-, and NH4+
are taken as the values at 298 K of the Aspen Databank CPAQ0 correlation.
CPAQ0 of HCO3- and CO3-2 are taken from Criss and Cobble (1964)[16]. Infinite
dilution aqueous phase Gibbs energy and enthalpy of formation, and CPAQ0
for NH2COO- are derived from the chemical equilibrium constants reported by
Lichtfers and Rumpf (2004)[17] for the formation reaction for NH2COO- from
NH3 and HCO3-. The liquid molar volume model and transport property models
have been updated and model parameters regressed from literature
experimental data. Specifications of the transport property models include:

2 Physical Properties 5
 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 mixtures.
The interaction parameter VLQKIJ for the quadratic mixing rule between
NH3 and H2O is regressed against experimental data from Pleskov et al.
(1939)[18] and Denisov et al. (1998)[19]. The Clarke model parameter
VLCLK/1 for all electrolytes in the solution is set as 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 NH3 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 NH3 and H2O in the ASPEN liquid mixture viscosity model, MUKIJ
and MULIJ, are regressed against experimental NH3 - H2O viscosity data
from Pleskov et al. (1939)[18] and Frank et al. (1996)[20]. The Jones-Dole
2
model parameters, IONMUB, of CO 3 and HCO3- are regressed against
K2CO3-H2O viscosity data from Pac et al. (1984)[21] and KHCO3-H2O
viscosity data from Palaty (1992)[22], respectively. For NH4+, Aspen Plus
databank values are used.
 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.
 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).
The estimation results of various transport and thermal properties are
summarized in Figures 1-12.

6 2 Physical Properties
500

400

300
T, K

200

100

0
0 0.2 0.4 0.6 0.8 1
Mole fraction of NH3

Figure 1. Comparison of the experimental Txy data (symbols) for vapor-


liquid equilibrium of the NH3-H2O system and the model correlations at 0.1
MPa and the model calculations at 1 MPa (lines): (○ and —) 0.1 MPa from
Hoshino et al. [5], (∆ and ▲) 1 MPa from Chu et al.[25], (▬▬) 0.1 MPa, (▬ ▬) 1
MPa

4500

4000
Cp, J/kg-K

3500

3000

2500
150 200 250 300 350

T, K

Figure 2. Heat capacity of the NH3-H2O system, (○) data from Chan et al.
(1964)[9] , (▬▬) model results

2 Physical Properties 7
-25

Heat of solution, kJ/mol


-30

-35

-40
1E-6 1E-5 1E-4 1E-3 1E-2 1E-1 1E+0

Mole fraction of NH3

Figure 3. Comparison of the experimental data from Wagman et al.[8] (○) for
heat of solution of NH3 in water at 298 K and the model correlations (▬▬)

1E+7

1E+6
CO2 partial pressure, Pa

1E+5

1E+4

1E+3

1E+2
0 2 4 6 8 10 12
CO2 molality, mol/kg

Figure 4. Comparison of the experimental data of Göppert and Maurer[26]


(empty symbols) and Kurz et al.[13] (filled symbols) for CO2 partial pressure
of the NH3-CO2-H2O system at 353 K and the model results (lines): (○) 12.17
molal NH3, (—) 11.8 molal NH3, (∆) 9.03 molal NH3, (□) 5.93 molal NH3, (×)
2.01 molal NH3, (◊) 0.6 molal NH3, (▬▬) 12.17 molal NH3, (▬ ▬) 9.03 molal
NH3, (▬ · ▬) 5.93 molal NH3, (─ ─ ─) 2.01 molal NH3, (······) 0.6 molal NH3

8 2 Physical Properties
1.E+06

NH3 partial pressure, Pa


1.E+05

1.E+04

1.E+03
0 2 4 6 8 10
CO2 molality, mol/kg

Figure 5. Comparison of the experimental data of Göppert and Maurer[26]


(empty symbols) and Kurz et al.[13] (filled symbols) for NH3 partial pressure
of the NH3-CO2-H2O system at 353 K and the model results (lines): (○) 12.17
molal NH3, (—) 11.8 molal NH3, (∆) 9.03 molal NH3, (□) 5.93 molal NH3, (▬▬)
11.8 molal NH3, (▬ ▬) 9.03 molal NH3, (▬ · ▬) 5.93 molal NH3.

6000

5500

5000
Cp, J/kg-K

4500

4000

3500

3000
0 0.05 0.1 0.15
Weight fraction of NH4HCO3

Figure 6. Comparison of the experimental data from Chernen’kaya[10]


(symbols) for heat capacity of aqueous NH4HCO3 solution and the model
calculations (lines): (○) 298 K, (▬▬ ) 298 K, (▬ ▬ ) 323 K, (▬ · ▬ ) 348 K,
(─ ─ ─) 373 K, (······)393 K, (▬ · · ▬) 423 K.

2 Physical Properties 9
100

80

Carbon distribution, %
60

40

20

0
0 0.2 0.4 0.6 0.8 1
CO2 loading

Figure 7. Comparison of the experimental data from Zhao et al.[14] (symbols)


for carbon distribution in liquid phase in the NH3-CO2-H2O system at 298 K
and 1.34 molar NH3 and the model correlations (lines): (○) HCO3-, (∆)
NH2COO-, (□) CO3-2, (▬▬) HCO3-, (▬ ▬) NH2COO-, (▬ · ▬) CO3-2

0.15

0.12
Mole fraction of NH4HCO3

0.09

0.06

0.03

0
290 300 310 320 330
Temperature, K

Figure 8. Comparison of the experimental data from Trypuc and


Kielkowska[15] (○) for solubility of NH4HCO3 in water and the model
correlations (▬▬).

10 2 Physical Properties
20

Calculated enthalpy change, kJ


15

10

0
0 5 10 15 20
Measured enthalpy change, kJ

Figure 9. Parity plot for the model calculations for enthalpy change on partial
vaporization of the NH3-CO2-H2O system and data from Rumpf et al.[24] at
temperatures between 313 and 393 K, NH3 concentrations up to 12 molal and
CO2 concentrations up to 6 molal

1000

900
Density, kg/m3

800

700

600
0.0 0.2 0.4 0.6 0.8 1.0

NH3 Mass Fraction

Figure 10. Liquid Density of NH3-H2O at 298.15K, (○) experimental data from
Pleskov et al. (1939)[18], (▬▬) model results

2 Physical Properties 11
10

Vicsosity, mPaS

0.1
0 0.2 0.4 0.6 0.8 1
NH3 Mass Fraction

Figure 11. Liquid Viscosity of NH3-H2O, (—) experimental data from Pleskov et
al. (1939)[4] at 293 K, (○) data from Frank et al. (1996)[20] at 293 K, (∆) data
from Frank et al. (1996)[20] at 303 K, (□) data from Frank et al. (1996)[20] at
313 K, (▬▬) model results at 293 K, (▬ ▬) model results at 303 K, (▬ · ▬)
model results at 313 K

0.8
Thermal Conductivity, Watt/m-K

0.6

0.4

0.2

0
0 0.1 0.2 0.3 0.4

NH3 Mass Fraction

Figure 12. Liquid Thermal Conductivity of NH3-CO2-H2O at 298.15K, (○)


experimental data from Reidel (1951)[23], (▬▬) model results

12 2 Physical Properties
3 Reactions

The electrolyte solution chemistry has been represented as a CHEMISTRY


model with the ID = NH3. This CHEMISTRY ID is used as the global
electrolyte calculation option in the simulation by specifying it on the
Properties | Methods | Specifications | Global sheet. Chemical
equilibrium is assumed with all the ionic reactions in the CHEMISTRY NH3. In
addition, a kinetic REACTION model called NH3-REA has been created for
potential use when there are column models such as RadFrac which allow
kinetic reactions. In NH3-REA, all reactions are assumed to be in chemical
equilibrium except the reactions of CO2 with OH- and the reactions of CO2 with
NH3.
Because the absorber and stripper in this model are simulated by flash
models, which do not allow kinetic reactions in Aspen Plus and implicitly use
the global electrolyte calculation option, CHEMISTRY NH3 is used in their
calculations.

A. Chemistry ID: NH3


1 Equilibrium 2H 2 O  H 3 O   OH 
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 NH 3  H 2 O  NH 4  OH 
5 Equilibrium NH 3  HCO 3  H 2 NCOO   H 2 O
6 Salt NH 4 HCO 3 (S)  NH 4  HCO 3

B. Reaction ID: NH3-REA


1 Equilibrium NH 3  H 2 O  NH 4  OH 
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 

3 Reactions 13
6 Kinetic NH 3  CO 2  H 2O  H 2 NCOO -  H 3O 
7 Kinetic H 2 NCOO -  H 3O   NH 3  H 2O  CO 2
8 Salt NH 4 HCO 3 (S)  NH 4  HCO 3
The equilibrium constants are calculated by Gibbs free energy of the
participating species of the reactions. The power law expressions are used for
the rate-controlled reactions (reactions 4-7 in REA-NH3) and the general
power law expression is:

  E  1 1  N
r  k T T0  exp     C 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;
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
(2)
RT i 1
In this simulation, the reduced expressions are used. In equation (2), the
concentration basis is Molarity, the factor n is zero, k and E are given in
Table 2. The kinetic parameters for reactions 4-7 in Table 3 are derived from
the work of Pinsent et al. (1956)[2].

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


Reaction No. k E (cal/mol)
4 4.32e+13 13249
5 2.38e+17 29451
6 1.35e+11 11585
7 2.14e+21 17203

14 3 Reactions
4 Simulation Approach

The aqueous NH3 can remove CO2 in the flue gas. At the relatively low
temperature (60~100°F) of the absorber, CO2 will be absorbed by NH3 and
the major products include ammonium bicarbonate, carbonate and
carbamate. At the relatively high temperature (120~190°F) of the
regenerator, these heat-unstable salts decompose, so that CO2 in pure form is
released and can subsequently be separated. The released ammonia gas can
also be separated by taking advantage of ammonia’s high solubility in water.
In this manner, the ammonia (NH3) content in the heat-unstable salts can be
regenerated for recycling.
As there are no industrial or pilot plant data available for aqueous ammonia
separation processes, we use the equilibrium model (flash calculations) to
simulate the feasibility of CO2 removal by ammonia.
Simulation Flowsheet – In the following simulation flowsheet in Aspen Plus
(Figure 13), CO2 is absorbed by NH3 in the absorber from a gas mixture of
CO2 and N2. The rich ammonia solution is then fed into the stripper where
CO2 is separated and NH3 is regenerated.

GASOU T CO2OUT

LEANIN
ABSORBER STR IPPER

GASIN

R ICHOUT LEANOUT

Figure 13. Ammonia 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


NH3 Model
Unit Operation Aspen Plus Block Comments / Specifications

1.Temperature is set at 60 °F
Absorber Flash2
2. Pressure is set at 1 atm

1. Temperature is set at 140 °F


Stripper Flash2
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 NH3 solution. Feed
conditions are summarized in Table 4.

Table 4. Feed specifications


Stream ID GASIN LEANIN
Substream: MIXED
Temperature: °F 60 80
Pressure: atm 1 1
Total flow 10 kmol/hr 50 kmol/hr
Mole-Frac Mole-Frac
H2O 0 0.84
NH3 0 0.1
CO2 0.15 0.06
N2 0.85 0
Prop-Sets – Two Prop-Set properties are used: XAPP to report apparent mole
fraction of CO2, NH3, H2O and N2 in liquid streams and SOLINDEX to monitor
precipitation of NH4HCO3

16 4 Simulation Approach
5 Simulation Results

The simulation was performed using Aspen Plus. Key simulation results are
presented in Table 5. Here the RICHOUT and LEANOUT compositions are the
mole fraction of apparent components.

Table 5. Key Simulation Results


Stream ID GASOUT CO2OUT RICHOUT LEANOUT
Substream: MIXED
Temperature: °F 60 140 60 140
Pressure: atm 1 1 1 1
Total flow 9.17 kmol/hr 1.42 kmol/hr 44.64 kmol/hr 46.49 kmol/hr
Mole-Frac Mole-Frac Mole-Frac Mole-Frac
H2O 0.02 0.18 0.90 0.84
NH3 0.00 0.07 0.06 0.10
CO2 0.05 0.75 0.04 0.06
N2 0.93 0.00 0.00 0.00
NH4HCO3S frac 0.00 0.00 0.05 0.00
SOLINDEX
NH4HCO3S 1.00 0.33
We can see from Tables 4 and 5 that solid NH4HCO3 is formed due to the
enrichment of CO2 in stream RICHOUT. Accordingly, the CO2 mole fraction in
the gas phase decreased from 0.15 in GASIN to 0.05 in GASOUT. CO2 can be
separated from NH3 in the stripper and the solid NH4HCO3 disappears due to
this stripping operation and there is no solid in stream LEANOUT. Some NH3 is
also stripped into CO2OUT, causing a loss of NH3 in the liquid solvent stream.
As these results are derived from a single equilibrium stage separation
simulation (only one stage flash for the absorber and the stripper), we can
expect that more effective CO2 removal can be achieved by aqueous ammonia
when multi-stage separation is applied.
SOLINDEX in Table 5 is the Solubility index of a salt, which is defined as the
ratio of its activity in the mixture to its saturation activity. We can see that
the SOLINDEX in RICHOUT is 1 and some of the NH4HCO3 precipitates out as
NH4HCO3S.

5 Simulation Results 17
6 Conclusion

The NH3 model provides a starting point for rate-based rigorous simulation of
the process. Key features of this simulation model include electrolyte
thermodynamics and solution chemistry, reaction kinetics for the liquid phase
reactions, and rigorous transport property modeling. This model can be used
in developing 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 more sophisticated
CO2 capture processes with NH3 for process development, debottlenecking,
plant and equipment design, among others. This simple NH3 model has been
validated with experimental thermophysical and transport properties data.
Further validation of this NH3 model will be done when industrial or pilot plant
data become available.

18 6 Conclusion
References

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with Electrolyte NRTL Model. Ind. Eng. Chem. Res. 2011, 50, 11406-11421.
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[12] Müller, G.; Bender, E.; Maurer, G. Das dampf-fl€ussigkeitsgleichgewicht
des tern€aren systems ammoniak-kohlendioxid-wasser bei hohen
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References 19
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- H2O system based on Raman spectra. Ind. Eng. Chem. Res. 2011, 50,
5316–5325.
[15] Trypuc, M.; Kielkowska, U. Solubility in the NH4HCO3 + NH4VO3 + H2O
system. J. Chem. Eng. Data. 1996, 41, 1005-1007.
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to 200_. Entropies and heat capacities above 200_. J. Am. Chem. Soc. 1964,
86, 5390–5393.
[17] Lichtfers, U.; Rumpf, B. Thermodynamic Properties of Complex Fluid
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KGaA: Weinheim, Germany, 2004; pp 92_119.
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at 20 degrees Centigrade”, Zh. Fiz. Khim. 1939, 13, 701-702.
[19] Denisov, S.A.; Blokhina, E.E.; “Solubility of nickel ammonia complexes”,
Deposited Doc. Viniti N1912, 1998, 98, 14.
[20] Frank, M.J.W.; Kuipers, J.A.M.; van Swaaij, W.P.M.; “Diffusion
Coefficients and Viscosities of CO2 + H2O, CO2 + CH3OH, NH3 + H2O, and
NH3 + CH3OH Liquid Mixtures”, J. Chem. Eng. Data. 1996, 41, 297-302.
[21] Pac, J.S.; Maksimova, I.N.; Glushenko, L.V.;”Viscosity of Alkali Salt
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