Aspen Plus

Rate-Based Model of the CO2 Capture Process by

Diglycolamine 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

V7.0 First version

V7.1 Re-verified simulation results using Aspen Plus V7.1
V7.1 CP1 Add N2, O2, CO and H2 to the model as Henry components
V7.2 Updated results for V7.2
V7.3 Update databank to PURE25.
Add the definition of acid gas loading and amine weight fraction
convention.
Use “Diglycolamine” (full name) to replace “DGA” (acronym) in the title
and in the first paragraph of the introduction because “DGA” is a
registered trademark of Huntsman corporation.
V7.3.2 Update databank to PURE26.
V8.0 Update databank to PURE27.
V8.2 Update databank to PURE28.
V8.6 Update databank to PURE32.

Revision History 1
Contents
Introduction ............................................................................................................3

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

2 Process Description..............................................................................................5

3 Physical Properties...............................................................................................6

4 Reactions ...........................................................................................................12

5 Simulation Approaches.......................................................................................15

6 Simulation Results .............................................................................................18

7 Conclusions ........................................................................................................20

References ............................................................................................................21

2 Contents
Introduction

This file describes an Aspen Plus rate-based model of the CO2 capture process
by Diglycolamine (DGA) from a gas mixture of CH4, CO2 and H2S. The model
consists of only an absorber. The performance test data of a commercial
absorber reported by Dingman and Weiland (2001) [1] were used to specify
feed conditions and unit operation block specifications in the model.
Thermophysical property models and reaction kinetic models are based on the
works of Aspen Technology (2007)[2] and Pacheco et al. (2000)[3]. Transport
property models and model parameters have been validated against
experimental data from open literature.
The model presented here includes the following key modeling 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 with valve trays

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

DGA Conventional DIGLYCOLAMINE C4H11NO2-2

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
DGAH+ Conventional DGA+ C4H12NOO+
DGACOO- Conventional DGACOO- C5H10NOO3-
H2S Conventional HYDROGEN-SULFIDE H2S
HS- Conventional HS- HS-
S-2 Conventional S-- S-2
CH4 Conventional METHANE CH4
N2 Conventional NITROGEN N2
O2 Conventional OXYGEN O2
CO Conventional CARBON-MONOXIDE CO
H2 Conventional HYDROGEN H2

4 1 Components
2 Process Description

The absorber data are reported by Dingman and Weiland (2001)[1] for CO2
capture by aqueous DGA solutions. Table 2 represents the typical operation
data:

Table 2. Data of the Pyote Unit

Absorber

Diameter 66 inches
Tray 16 Nutter trays on 2ft spacing

Feeds and Products

Sour Gas to Absorber 17.22 MMscfd

CO2 in Sour Gas 5.82 vol%
H2S in Sour Gas 0.38 vol%
H2S in Sweet Gas 1 ppmv
DGA solution 46.3%(wt)
CO2 Loading in Lean Amine 0.034 mole CO2 /mole DGA
H2S Loading in Lean Amine 0.0001 mole H2S /mole DGA

2 Process Description 5
3 Physical Properties

The electrolyte NRTL method and RK equation of state are used to compute
liquid and vapor properties respectively. Interaction parameters between
molecules and electrolytes have been regressed against literature CO2 and
H2S solubility data from Maddox et al. (1987)[4], Dingman et al. (1983)[5] and
Martin et al. (1978)[6].
CH4, N2, O2, CO, H2, CO2 and H2S are selected as Henry-components to which
Henry’s law is applied and the Henry’s constants are retrieved from Aspen
Plus databanks for these components with water and regressed against CO2
and H2S solubility data from Maddox et al. (1987)[4], Dingman et al. (1983)[5]
and Martin et al. (1978)[6] for CO2 and H2S with DGA. 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 model and transport property models have been
updated and model parameters regressed from literature experimental data.
Specifications of the transport property 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
DGA and H2O is regressed against experimental data from Henni et al.
(2001)[7] and Valtz et al. (2004)[8]. The Clarke model parameter VLCLK/1

is also regressed for main electrolytes (DGAH+, HCO 3 ), (DGAH+, DGACOO
 2
) and (DGAH+, CO 3 ) against experimental data from Huntsman Co.[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 solvent. There are three models for
electrolyte correction and the DGA 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 DGA and H2O in the ASPEN liquid mixture viscosity model, MUKIJ
and MULIJ, are regressed against DGA-H2O viscosity experimental data
from Henni et al. (2001)[7]. The Jones-Dole model parameters, IONMUB,
for DGAH+ and DGACOO- are regressed against DGA-H2O-CO2 viscosity

6 3 Physical Properties
 2
data from Huntsman Co.[9]; that of CO 3 is regressed against K2CO3-H2O
viscosity data from Pac et al. (1984)[13]; and that of HCO3- is regressed
against KHCO3-H2O viscosity data from Palaty (1992)[14].
 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 aqueous
phase heat of formation at infinite dilution and 25°C (DHAQFM) for DGAH+
and DGACOO- and the heat capacity at infinite dilution (CPAQ0) for DGAH+
and DGACOO- are adjusted to fit to the literature data on heat of solution
from Christensen et al. (1986)[10].
The estimation results of various transport and thermal properties are
summarized in Figures 1-8. Note that acid gas loading is defined as the ratio
of the moles of apparent acid gas to the moles of apparent DGA. Apparent
means before reaction, so for example if 1 mole of DGA 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 DGA after reacting. Weight percent of DGA
is calculated without CO2, so in the above example, it is calculated from the
mixture of 1 mole DGA and 9 moles of water. Since DGA 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% DGA.

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

3 Physical Properties 7
 1200
EST DGA 10w t%
EST DGA 20w t%
EST DGA 30w t%
1150 EST DGA 40w t%

Density, kg/m3 1100

1050

1000

950

900
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

Figure 1. Liquid Density of DGA-CO2-H2O at 298.15K

0.1
EST DGA 10w t%
EST DGA 20w t%
EST DGA 30w t%
EST DGA 40w t%

0.01
Viscosity, PaS

0.001

0.0001
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

Figure 2. Liquid Viscosity of DGA-CO2-H2O at 298.15K

8 3 Physical Properties
 0.08

0.07

0.06
Surface Tension, N/m
0.05

0.04

0.03

0.02

EST DGA 10w t%

0.01 EST DGA 20w t%
EST DGA 40w t%
EST DGA 60w t%
0
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

Figure 3. Surface tension of DGA-CO2-H2O at 298.15K

0.7

0.6
Thermal Conductivity, Watt/m-K

0.5

0.4

0.3

0.2

EST DGA 10w t%

0.1 EST DGA 20w t%
EST DGA 40w t%
EST DGA 60w t%
0
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

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

3 Physical Properties 9
 120

100

Heat Capacity, J/mol-K 80

60

40

20 EST DGA 10w t%

EST DGA 20w t%
EST DGA 40w t%
EST DGA 60w t%
0
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

Figure 5. Liquid Heat Capacity of DGA-CO2-H2O at 298.15K

0
EXP Christensen86 DGA10w t%
EST DGA 10w t%
EXP Chistensen86 DGA20w t%
EST DGA 20w t%
-30000 EXP Christensen86 DGA40w t%
EST DGA 40w t%
EXP Christensen86 DGA60w t%
Heat of Solution, J/mol

EST DGA 60w t%

-60000

-90000

-120000

-150000
0 0.1 0.2 0.3 0.4 0.5
CO2 Loading

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

from Christensen et al. (1986)[10]

10 3 Physical Properties
 10000000
EXP Maddox87 313K
EST 313K
EXP Maddox87 333K
EST 333K
1000000
Pressure, Pa

100000

10000

1000
0.1 1
CO2 Loading

Figure 7. CO2 Partial Pressure of DGA-CO2-H2O (DGA mass fraction = 0.40),

experimental data from Maddox et al. (1987)[4]

10000
EXP Martin78 323K
EST 323K
EXP Martin78 373K
EST 323K
1000
Pressure, KPa

100

10

1
0.01 0.1 1 10
H2S Loading

Figure 8. H2S Partial Pressure of DGA-H2S-H2O (DGA mass fraction = 0.60),

experimental data from Martin et al. (1978)[6]

3 Physical Properties 11
4 Reactions

DGA is a primary ethanolamine, as shown in Figure 9. It can associate with

H3O+ to form DGAH+ and can also react with CO2 to form carbamate
DGACOO-.

Figure 9. DGA Molecular Structure

The electrolyte solution chemistry has been modeled with a CHEMISTRY
model with CHEMISTRY ID = DGA. 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 and is also used in the
calculations of absorber and stripper by specifying it in the Reaction part of
the absorber and stripper specifications. Chemical equilibrium is assumed with
all the ionic reactions in the CHEMISTRY DGA. In addition, a kinetic REACTION
model called DGA-REA has been created, which was also tried in calculations
of the absorber and stripper by specifying it in the Reaction part of the
absorber and stripper specifications but not used in the final model because of
convergence problems. In DGA-REA, all reactions are assumed to be in
chemical equilibrium except the reactions of CO2 with OH- and the reactions of
CO2 with DGA.

A. Chemistry ID: DGA

1 Equilibrium
DGAH   H 2 O  DGA  H 3 O 

2 Equilibrium
2H 2 O  H 3 O   OH 

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

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

5 Equilibrium
DGACOO   H 2 O  DGA  HCO 3

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

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

12 4 Reactions
 B. Reaction ID: DGA-REA

1 Equilibrium
DGAH   H 2 O  DGA  H 3 O 

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
DGA  CO 2  H 2 O  DGACOO -  H 3 O 

7 Kinetic
DGACOO -  H 3 O   DGA  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. (1989)[11]. The power law expressions are used for the rate-
controlled reactions (reactions 4-7 in DGA-REA) 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 components 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 file, 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 3. The kinetic parameters for reactions 6-7 in Table 3 are derived from
the work of Pacheco et al. (2001)[3]. The kinetic parameters for reaction 4 are

4 Reactions 13
 taken from the work of Pinsent et al. (1956)[12] , 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.

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 1.94e+15 15813
7 3e+26 25287

14 4 Reactions
5 Simulation Approach

The case of the commercial absorber[1] for CO2 capture by a aqueous DGA
solution reported by Dingman and Weiland (2001)[1] is used in the simulation.
Simulation Flowsheet – The absorber has been modeled with the following
simulation flowsheet in Aspen Plus, shown in Figure 10.

GASOU T

LEANIN

ABSORBER

GASIN

R IC HOUT

Figure 10. Rate-Based DGA Simulation Flowsheet in Aspen Plus

5 Simulation Approach 15
 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

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

Absorber RadFrac 1. Calculation type: Rate-Based

2. 16 Stages
3. Top Pressure: 980 psig
4. Reaction: Chemistry ID is DGA for all stages
5. Tray Type: Nutter Float Valve
6. Tray Diameter: 66 in
7. Tray Spacing: 2 ft
8. Mass transfer coefficient method: Scheffe and
Weiland (1987)
9. Interfacial area method: Scheffe and Weiland (1987)
10. Interfacial area factor: 0.8
11. Heat transfer coefficient method: Chilton and
Colburn
12. Film resistance options: Filmrxn for liquid film; Film
for vapor film
13. Flow model: Mixed
14. Estimates: provide temperature, liquid and vapor
flow rate and composition estimates for all stages.
These estimates are intended to aid convergence

16 5 Simulation Approach
 Streams - Feeds to the absorber are gas stream GASIN containing CH4, CO2
and H2S and liquid solvent stream LEANIN containing aqueous DGA solution.
Feed conditions are summarized in Table 5. As the flow rate of LEANIN is not
provided in the literature [1], we estimate the value of LEANIN flow rate
under the assumption that the acid gas in GASIN are totally absorbed into the
DGA solution and the acid gas loading in RICHOUT is 0.5.

Table 5. Feed specifications

Stream ID GASIN LEANIN
Substream: MIXED
Temperature: F 88 119
Pressure: psig 980 980
Total flow 905 kmol/hr 27750 kg/hr
Mole-Frac Mole-Frac
DGA 0 0.12877
H2O 0 0.866842
CO2 0.0582 0.004378
H2S 0.0038 1e-05
CH4 0.938 0
Prop-Sets - A Prop-Set named XAPP was used to report apparent mole
fractions of CO2, H2S, and DGA in liquid streams to facilitate calculations of
acid gas loadings of the streams.

5 Simulation Approach 17
6 Simulation Results

The simulation was performed using Aspen Plus. The rate-based calculation
method is used in dealing with the mass transfer. Furthermore, there are two
possible approaches in deal with the chemical reactions in the liquid phase. In
the first approach, reaction kinetics for CO2 absorption by DGA and OH- are
considered while the remaining reactions are in chemical equilibrium by using
REACION DGA-REA of the model in the calculation of the absorber. In the
second approach, all liquid phase reactions are assumed to reach chemical
equilibrium by using the CHEMISTRY DGA of the model in the calculations of
the absorber.
It is found that, due to the extremely high reaction rate between CO2 with
DGA, Aspen Rate-Based Distillation is not able to converge reliably when the
kinetic treatment for the reactions is used in the simulation. Considering the
fact that the reaction rates of CO2 with DGA are so high that the equilibrium
treatment is a reasonable approximation, we used the equilibrium reaction
treatment in this simulation. The simulation converges reliably with use of
CHEMISTRY DGA for all stages of the absorber and the key simulation results
are presented in Table 6. The measured versus calculated absorber liquid and
vapor temperature profiles are presented in Figure 11.

Table 6. Key Simulation Results

Variable Measurement Rate-Based DGA Model

CO2 mole fraction in GASOUT na 0.77ppm

H2S mole fraction in GASOUT 1ppm 0.05ppm
Loading of RICHOUT, MolAcidGas/MolDGA na 0.49

18 6 Simulation Results
 240
Measured
220
AspenPlus, Liquid
200
AspenPlus, Vapor
Temperature, F
180

160

140

120

100
0 5 10 15 20
Stage Num ber

Figure 11. The Absorber Temperature Profile

The column produced better than 1 ppm H2S treated gas, but unfortunately
the gas was not analyzed for CO2 and the rich solvent was not measured for
acid gas loading[1]. The Aspen Plus simulation yields a treated gas containing
0.05 ppm H2S and 0.77 ppm CO2 (Table 6). These results are quite
reasonable. Finally, the agreement between the measured and simulated
column temperature profiles is excellent (See Figure 11).

6 Simulation Results 19
7 Conclusions

The DGA model provides a rate-based rigorous simulation of the process. Key
features of this rigorous simulation include electrolyte thermodynamics and
solution chemistry, chemical equilibrium 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 DGA. You may use it as a starting point for more sophisticated
models for process development, debottlenecking, plant and equipment
design, among others.
The Rate-Based DGA model with liquid phase reaction kinetics is found to be
too difficult to converge. It is recommended that chemical equilibrium
treatment for the DGA liquid phase reactions be used for the time being to
provide a satisfactory approximation. This model will be updated when Aspen
Rate-Based Distillation convergence capability is further advanced.

20 7 Conclusions
References

[1] J.C. Dingman, R.H. Weiland, “How to Increase CO2 Slip”, Laurance Reid
Gas Conditioning Conference, 2001
[2] Aspen Technology Inc., 2007
[3] M.A. Pacheco, S. Kaganoi, G.T. Rochelle, “CO2 Absorption into Aqueous
Mixture of Diglycolamine and Methyldiethanolamine”, Chem. Eng. Sci., 55,
5125-5140(2000)
[4] R.N. Maddox, A.H. Bhairi, J.R. Diers, P.A. Thomas, “Equilibrium Solubility
of Carbon Dioxide or Hydrogen Sulfide in Aqueous Solutions of
Monoethanolamine, Diglycolamine, Diethanolamine and
Methyldiethanolamine”, GPA Research Report, NO. 104, 1987
[5] J.C. Dingman, J.L. Jackson, T.F. Moore, J.A. Branson, “Equilibrium Data
for the H2S-CO2-Diglycolamine Agent-Water System”, 62nd Annual GPA
Convention, 1983
[6] J.L. Martin, F.D. Otto, A.E. Mather, “Solubility of Hydrogen Sulfide and
Carbon Dioxide in a Diglycolamine Solution”, J. Chem. Eng. Data, 23, 163-
180(1978)
[7] A. Henni, P. Tontiwachwuthikul, A. Chakma, A.E. Mather, “Volumetric
Properties and Viscosities for Aqueous Diglycolamine Solutions from 25 C to
70 C”, J. Chem. Eng. Data, 46, 56-62(2001)
[8] A. Valtz, M. Teodorescu, I. Wichterle, D. Richon, “Liquid Densities and
Excess Molar Volumes for Water + Diethylene Glycolamine, and Water,
Methanol, Ethanol, 1- Propanol + Triethylene Glycol Binary Systems at
Atmospheric Pressure and Temperatures in the Range of 283.15 - 363.15 K”,
Fluid Phase Equilib., 215, 129-142(2004)
[9] Huntsman Co. Brochure, “Diglycolamine Agent Product Information”
[10] S.P. Christensen, J.J. Christensen, R.M. Izatt, “Enthalpies of Solution of
Carbon Dioxide in Aqueous Diglycolamine Solutions”, Thermochimica Acta,
106, 241-251(1986)
[11] D.M. Austgen, “A Model of Vapor-Liquid Equilibria for Acid Gas-
Alkanolamine-Water”, PhD thesis, the University of Texas at Austin, 1989
[12] 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)

References 21
 [13] 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)
[14] Z. Palaty, “Viscosity of diluted aqueous K2CO3/KHCO3 solutions”, Collect.
Czech. Chem. Commun., 57, 1879(1992)

22 References