Experimental Measurement of CO2 Solubility in Aqueous CaCl2

Article Cite This: J. Chem. Eng. Data XXXX, XXX, XXX-XXX

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Experimental Measurement of CO2 Solubility in Aqueous CaCl2 Solution at Temperature from 323.15 to 423.15 K and Pressure up to 20 MPa Using the Conductometric Titration Hamdi Messabeb,*,† François Contamine,*,† Pierre Cézac,† Jean Paul Serin,† Clémentine Pouget,† and Eric C. Gaucher‡ †

Laboratoire de Thermique, Energetique et Procedes-IPRA, University of Pau and Pays de l’Adour, EA1932, 64000, Pau, France TOTAL, CSTJF, Avenue Larribau, F-64018 Pau Cedex, France

‡

ABSTRACT: In the framework of the efforts of the scientific community developed for the reduction of CO2 emissions, the geological storage of CO2 in deep saline aquifers is under focus. An increase of salinity decreases the potential of CO2 solubilization into the water. In salty waters, the salinity is not only due to NaCl but also to others ions and in particular Ca and Mg. Experimental solubility data of CO2 in calcium chloride solution available in the literature at conditions relevant to carbon storage are particularly scarce. In this work, a new analytical method was developed for experimental measurement of CO2 solubility in calcium chloride solutions (1, 3, and 6 mol/kg) at high pressures (5−20 MPa) and temperatures (323.15, 373.15, and 423.15 K). This method is based on conductometric titration coupled with classical pH titration. The conductimetry shows sharper curves than the pH titration allowing a higher precision. Thirty-six new experimental data are reported in this paper. These data presented an experimental average uncertainty of 2.1% with the ANOVA calculation method based on repeatability and reproducibility experiments. The CO2 solubility in CaCl2 solutions is noticeable lower than in NaCl solution increasing the salting out effect. Considering our previous work on NaCl solutions and this paper for CaCl2 solutions, estimations of the real quantity of CO2 that may be dissolved in saline aquifers can be made with a significantly better precision.

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INTRODUCTION

The general purpose of this study is to provide CO2 solubility data in calcium chloride solution over a wide range of temperature (323.15−423.15 K) at three salinities (1, 3, and 6 mol/kg) and pressure up to 20 MPa. Original data presented in this paper were obtained by a new analytical method developed in order to increase the precision.

The concentration of CO2 in atmosphere continues to increase, reaching 406.31 ppm according to the latest measurement carried out by NASA in May 2017.1 To mitigate climate change the Intergovernmental Panel on Climate Change’s (IPCC’s) experts recommended that concentration of greenhouse gases in atmosphere shall not exceed 450 ppm in 2100.2 Carbon capture and storage is a seriously considered option to achieve significant reductions in carbon dioxide emissions. Storage capacity and long-term geochemical behavior depend, among other underground characteristics, on brine salinity and composition of fluids in deep saline aquifers and geological formation. Commonly, these fluids contain mainly Na+ and Cl− with minor quantities of K+, Ca2+, Mg2+, and SO42− in various proportions.3 In some cases, as Shiqianfeng and Liujiagou formations in China4 and Rotliegend Formation in Nederland,5 brine can contain a significant amount of calcium. Contrary to the CO2−H2O−NaCl system which has been extensively investigated over the range of pressure, temperature, and salinity relevant to carbon capture and storage,6−8 the CO2− H2O−CaCl2 has not been widely studied, and the experimental solubility data of CO2 in calcium chloride solution are relatively scarce especially at high temperature, pressure, and salinity.9,10 © XXXX American Chemical Society

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LITERATURE REVIEW The number of experimental study focusing on CO2 solubility in calcium chloride solution at geological storage conditions is limited. Data available in the literature at pressure above atmospheric are listed in the Table 1. Before 2010, only four studies have been published. Prutton and Savage11 provided an extensive study of CO2 solubility in CaCl2 solutions over a wide range of temperature, pressure, and salt molality. However, measurements were restricted to a maximum temperature of 393.15 K and maximum salinity of 3.9 mol/kg. Malinin12 studied the CO2−H2O−CaCl2 system at a range of temperature higher than temperatures relating to geological Received: June 28, 2017 Accepted: November 7, 2017

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DOI: 10.1021/acs.jced.7b00591 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

Table 1. Literature Experimental Data for CO2−H2O−CaCl2 System authors Prutton and Savage11 Malinin12 Malinin and Saveleva13 Malinin and Kurovskaya14 Liu et al.15 Tong et al.10 Bastami et al.16 Zhao et al.17

MCaCl2 /mol.kg−1

pressure /MPa

temperature/K

controls and regulates the reactor temperature, a stirrer composed of a Rushton turbine and a four blade impeller, a high pressure volumetric pump (Top Industrie PMHP 200-200) for the gas loading, and a sampling syringe connected to the bottom of the equilibrium reactor. Pressure transducer (PA 33X) from Keller and platinum probes (PT100) were used for the pressure and temperature measurement and monitoring. Considering the corrosive nature of brine, the cell, pump, and line were made of Hastelloy C276. Brines were prepared by weighing the select amounts of salt and pure water with respectively an electronic balance (Sartorius CPA 225D) with an accuracy of 0.01 mg and a Denver Instrument balance (MXX2001) with a resolution of 0.1 g. In a typical experiment, reactor and line are purged and put under vacuum. Brine is introduced into the evacuated cell, then the desired temperature is fixed and the carbon dioxide is loaded until the suitable pressure. During the gas loading, the stirrer is rotating to improve the contact between the aqueous and gas phases in order to promote the CO2 dissolution in brine. The equilibrium state is reached when the pressure remain unchanged within 2 h; this fact is checked and confirmed by the good repeatability of aqueous phase analysis. At equilibrium conditions, the CO2 dissolution acidifies the liquid phase. The sampling step consists to the withdrawal of an aqueous saturated sample in a syringe that contains beforehand a known amount of sodium hydroxide solution. The CO2 reacts with the hydroxide ion in excess so that the total amount of carbon dioxide present in the sample was converted to CO32− according to reaction 1. Then, the carbonate ion reacts with Ca2+ to form a CaCO3 precipitate according to the reaction 2.4

348.15−393.15 473.15−623.15 298.15−348.15 298.15−423.15

10−70 10−39 4.795 4.795

1−3.9 1 0.2−4.4 0.9−8.8

318.15 K 308−424.64 328.15−375.15 323.15−423.15

2.09−15.86 1.53−37.99 6.89−20.68 15

1 1−5 1.9−4.8 0.33−2

storage. The minimum temperature studied is 473.15 K; in addition, all data provides by this author are limited to one salt molality (1 mol/kg). Malinin and Saveleva13 and Malinin and Kurovskaya14 investigated the CO2 solubility in aqueous CaCl2 solution over a wide range of temperature and salinity; nevertheless, all experiments were conducted at low pressure 4.795 MPa. In the last five years, four papers have been published. Liu et al.15 investigated the CO2 solubility in 1 mol/kg CaCl2 solution at low temperature 318.15 K and Bastami et al.16 determined the solubility of carbon dioxide in 1.9 and 4.8 mol/kg CaCl2 solution up to 375.15 K. Zhao et al.17 studied the CO2 solubility in the range of 0.33 to 2 mol/kg calcium chloride solution at 323.15, 373.15, and 423.15 K but only at one pressure (15 MPa). For these three studies, a volumetric approach was utilized for the solubility measurements. Tong et al.10 measured CO2 solubility in calcium chloride solutions using a synthetic method, without resorting to any sampling and analysis steps. This method relies on the determination of the bubble point by visual observation. Phase composition is determined afterward at fixed temperature from the known amounts of CO2 and brine introduced initially in the view cell.

EXPERIMENTAL SECTION Chemicals. Compound, formula, source, and purity of all materials used in this work are summarized in Table 2. Table 2. Characteristics of the Chemicals Used in This Work chemical name

formula CO2 CaCl2

Air Liquide ACROS ORGANICS

0.997a 0.960a

NaOH

VWR

0.990a

HCl

VWR

H2O

Barnstead Easypure RoDi filtering system

between 0.998 and 1.002a 18.2 MΩ.cm

a

source

(1)

CO32 − + Ca 2 + → CaCO3(sd)

(2)

At the end of the sampling step, the sampling syringe contains a suspension of calcium carbonate (sd), excess of hydroxide ion (OH−), sodium ion (Na+), chloride ion (Cl−), and calcium ion (Ca2+). Carbonate ion (CO32−) is present as trace because of the mass action law related to the presence of calcium carbonate in the suspension; its concentration is typically less than 10−4 M. At this basic environments, pH level is higher than 11.5 due to the excess of NaOH. This fact leads to a shift in the equilibrium in reactions 1 and 2 to the right. The availability of carbonate ions favors the precipitation of calcite. For all experiment conditions, the concentration of calcium exceeds that of carbon dioxide in the saturated aqueous phase, so the excess reagent is calcium and limiting reagent is the carbonate ion. Thus, all amounts of CO2 initially present in the aqueous sample are converted to carbonate ion which completely turned into CaCO3. Analysis. Solution samples were analyzed by conductometric titration coupled with pH measurements. This method is based on the change of the solution conductivity with the volume of titrant added. Titrations were carried out using a titration unit (Titroline 7800) from SI Analytics and a 0.1 M hydrochloric acid solution, and the conductivity versus the volume of titrant added are plotted. In typical titration graph (Figure 2), three main parts can be distinguished: three straight lines and two intersection points are obtained. •The first straight line sharply decreases due to the neutralization of the excess of hydroxide ion according to reaction 3. The conductivity line having a constant slope and the

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carbon dioxide calcium chloride sodium hydroxide hydrochloric acid water

CO2 + 2OH− → CO32 − + H 2O

purity

Mass fraction purity stated by the supplier.

Apparatus and Operating Procedure. The experimental device, operating procedure, and sampling system used in this work are described in detail in our previous paper.6 The apparatus device (Figure 1) consists mainly of a high pressure and high temperature equilibrium reactor with a double jacket. It includes a thermostatic bath (Lauda Proline RP 845 C) that B



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Figure 1. Photograph of the experimental device.

Figure 2. Typical titration graph used for dosing the dissolved CO2.

pH curve confirm that only the OH− is dosed and the small amount of CO32− mentioned above can be neglected. OH− + H+ ↔ H 2O

•The second straight line gradually increases; this branch corresponds to the calcium carbonate dissolution following reactions 5a and 5b:

(3)

At this stage, the amount of calcium carbonate precipitated during the sampling process can be calculated from the difference between the amount of OH− initially present in the sampling syringe (n0(OH−)) and the amount of OH− in excess (the OH− which does not react at the end of the sampling step, n(OH−) but which is neutralized during the first titration step (= CHCl × V1, where V1 is the volume of added hydrochloric acid solution)). This first end point is reached at pH between 8.9 and 9.4. According to reactions 1 and 2 nCO2 = nCO32 − = nCaCO3 =

0 − − n n(OH ) (OH−)

2

=

CaCO3(sd) + H+ ↔ Ca 2 + + HCO−3

(5a)

HCO−3 + H+ ↔ H 2CO3

(5b)

The second end point is reached at pH of between 4 and 5, and the quantity of calcium carbonate can be calculated from the difference between the two end point volumes. nCO2 = nCO32 − = nCaCO3 =

C × (V 2 − V 1) n H+ = HCl 2 2

(6)

At this stage, the titration consistency can be checked, and carbon dioxide quantities determined at the first (eq 4) and second step (eq 6) should be the same (the amount of CaCO3 in the sampling syringe is equal to the quantity of CO32− obtained from the reaction between CO2 and OH−).

0 − − (C n(OH ) HCl × V 1)

2

(4) C



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•The third straight line sharply increases due to the excess of H+ added after the second end point. For each equilibrium condition, at least five samples are withdrawn and analyzed to obtain final results. Measurements of CO2 solubility in pure water were carried out according to the analytical method reported in our previous paper.6

Table 3. Experimental Data of CO2 Solubility in Water and Calcium Chloride Solutions at 323.15, 373.15, and 423.15 Ka

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EXPERIMENTAL UNCERTAINTY The experimental uncertainty was evaluated with analysis of variance (ANOVA) which consists of a statistical method based on repeatability and reproducibility experiments. The principle of ANOVA method was discussed and reported in detail in our previous paper along with the accuracy of measuring instruments (pressure sensor and temperature probes). Repeatability and reproducibility experiments were carried out at 323.15 K, 10 MPa, and 1 mol of CaCl2 per kilogram of water. Uncertainty was calculated from analysis results of 3 distinct experiments performed at the same conditions (reproducibility) with 10 titrations for each experiment (repeatability). The experimental average uncertainty obtained from ANOVA calculations is equal to 2.1%. The coverage factor is drawn from Student’s distribution for two degrees of freedom and a confidence level of 95%.

pressure/MPa

mCO2/mol·kg−1b

0

323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 323.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 373.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15 423.15

5.01 10.03 15.04 20.00 5.07 10.00 15.01 19.98 5.09 10.05 15.02 19.89 5.09 10.08 14.98 19.95 5.05 10.07 14.96 19.90 5.16 10.27 15.17 20.04 5.04 10.04 15.02 20.01 5.24 10.10 15.00 19.91 5.05 10.12 15.10 19.95 5.13 10.18 15.12 19.96 5.13 10.27 15.12 19.96 5.10 10.48 15.29 19.86

0.791c 1.164c 1.234c 1.308c 0.568 0.829 0.885 0.914 0.290 0.429 0.469 0.498 0.172 0.227 0.247 0.252 0.475 0.804 1.019 1.153 0.337 0.568 0.715 0.816 0.191 0.320 0.387 0.437 0.108 0.171 0.211 0.239 0.386 0.729 1.003 1.174 0.260 0.495 0.658 0.772 0.140 0.262 0.348 0.410 0.087 0.139 0.180 0.207

3

6

0

1

RESULTS AND DISCUSSION CO2 solubility in calcium chloride solutions were investigated at three molalities, 1, 3, and 6 mol/kg, and at three temperatures, 323.15, 373.15, and 423.15 K, in the pressure range between 5 and 20 MPa. Results obtained are reported in Table 3. Figures 3−5 compare experimental solubility data of CO2 in CaCl2 solution at 1 mol/kg obtained in this work with the data available in the literature respectively at 323.15, 373.15, and 423.15 K. These graphs show a good agreement between our experimental data and those reported by other authors. Our results were compared in more details with Zhao et al.17 data obtained at 15 MPa. A maximum deviation of 4.5% was observed at 373.15K. Therefore, we can validate the reliability of our operating procedure and analysis. The results obtained at 323.15, 373.15, and 423.15 K for the CO2−H2O−CaCl2 system at 3 mol/kg are plotted in Figures 6−8. In these conditions, experimental data available in the literature are scarce and only three data were published: data of Tong et al.10 at 374.65 K (5.99 and 15.72 MPa) and at 424.40 K (82.9 MPa). Our isotherm at 323.15 K is completely new. The results obtained at 323.15, 373.15, and 423.15 K for the CO2−H2O−CaCl2 system at 6 mol/kg are presented in Figure 9. The temperature increase leads to the reduction of CO2 solubility. The sensitivity of the CO2 solubility to temperature decreases in the high pressure range. As expected, the pressure increase promotes the dissolution of carbon dioxide in the aqueous phase. The influence of pressure depends on the pressure and we observe a convergence of the three isotherms as far as the pressure increase. It can be seen also that the pressure effect increase with the rise of temperature. The salting out (SO) effect is defined as the relative reduction of CO2 solubility in salty aqueous solution compared to carbon dioxide solubility in pure water.18 Salting out effect was calculated at each temperature, pressure, and molality conditions following eq 7 100 × (m0 − m) m0

temperature/K

1

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SO% =

MCaCl2/mol·kg−1b

3

6

0

1

3

6

a Standard uncertainties u are u(T) = 0.06 K, u(P) = 30 kPa. Relative uncertainties ur are ur(m(CaCl2)) = 0.0012 and ur(m(CO2)) = 0.021 for CO2 solubility in CaCl2 aqueous solutions and 0.035 for CO2 solubility in pure water. bMolalities are expressed in moles per kilogram of water. cData published in our previous paper.6

where m0 is the CO2 solubility in pure water and m is the CO2 solubility in brine at the same conditions of temperature and pressure.18,19 Figure10 clearly illustrates the salting out effect by showing that the influence of salinity on the CO2 solubility is much

(7) D



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Figure 3. Solubility of carbon dioxide in 1 mol/kg CaCl2 solution at 323.15 K up to 20 MPa: ○, this study; ▲, Zhao et al.17

Figure 6. Solubility of carbon dioxide in 3 mol/kg CaCl2 solution at T = 323.15 K up to 20 MPa: ○, this study.

Figure 4. Solubility of carbon dioxide in 1 mol/kg CaCl2 solution at T = 373.15 K up to 20 MPa: ○, this study; ▲, Zhao et al.;17 ◆, Tong et al.;10 ■, Prutton and Savage.11

Figure 7. Solubility of carbon dioxide in 3 mol/kg CaCl2 solution at T = 373.15 K up to 20 MPa: ○, this study; ◆, Tong et al.10

Figure 8. Solubility of carbon dioxide in 3 mol/kg CaCl2 solution at T = 423.15 K up to 20 MPa: ○, this study; ◆, Tong et al.10

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Figure 5. Solubility of carbon dioxide in 1 mol/kg CaCl2 solution at T = 423.15 K up to 20 MPa: ○, this study; ▲, Zhao et al.;17 ◆, Tong et al.10

CONCLUSIONS In this study, our literature review of experimental data of CO2 solubility in calcium chloride solution at high pressure, temperature, and concentration shows that data in the temperature, pressure, and salinity ranges are particularly scarce. An experimental device was used to conduct experience and a new analytical method based on conductometric titration coupled with pH measurement was implemented for the solubility determination. Analysis and operating procedure were validated through the comparison of our results for the CO2−H2O−CaCl2 1 mol/kg system with data available in the literature at the same conditions of pressure and temperature.

stronger than that of pressure and temperature in the range of condition studied. The Figure 11 shows a comparison between the salting out effect in CaCl2 solutions and NaCl solutions at 323.K. The salting out effect observed in CaCl2 solutions is greater than that observed in NaCl solution during our previous work,6 which agrees with Tong et al.10 and Jacob and Saylor.3 Bivalent cations lead to a salting out effect greater than monovalent cations. E



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The results of this work are important for the CO2 storage issues. Indeed, a high quantity of divalent ions (Ca2+, Mg2+) in salty aquifers experiences consequences when drastically reducing the quantity of CO2 that is able to be dissolved in the salty water. This reduction should be known by the modelers of CO2 storage in salty aquifers.

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AUTHOR INFORMATION

Corresponding Authors

*E-mail: [email protected]. *E-mail: [email protected]. ORCID

Hamdi Messabeb: 0000-0002-4317-9616 Funding

Figure 9. Solubility of carbon dioxide in 6 mol/kg CaCl2 solution up to 20 MPa: ○, this study at 323.15 K; gray fill, black outline ○, this study at 373.15 K ; ●, this study at 423.15 K.

This work was supported by ANR Grant SIGARRR (ANR-13SEED-0006) and TOTAL SA. (Project Carbon Capture, Use, and Storage). Notes

The authors declare no competing financial interest.

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REFERENCES

(1) Climate Change: Vital Signs of the Planet: Carbon Dioxide; available at: https://climate.nasa.gov/vital-signs/carbon-dioxide/. (2) Benson, S.; Cook, P.; Metz, B.; Davidson, O.; De Coninck, H.; Loos, M.; Meyer, L. IPCC Special Report on Carbon Dioxide Capture and Storage. Cambridge UP, UK 2005, 5, 431−431. (3) Jacob, R.; Saylor, B. Z. CO2 solubility in multi-component brines containing NaCl, KCl, CaCl2 and MgCl2 at 297 K and 1−14 MPa. Chem. Geol. 2016, 424, 86−95. (4) Wang, L.; Shen, Z.; Hu, L.; Yu, Q. Modelling and measurement of CO2 solubility in salty aqueous solutions and application in the Erdos Basin. Fluid Phase Equilib. 2014, 377, 45−55. (5) Ranganathan, P.; Van Hemert, P.; Rudolph, E. S. J.; Zitha, P. Z. J. Numerical Modeling of CO2 Mineralisation during Storage in Deep Saline Aquifers. Energy Procedia 2011, 4, 4538−4545. (6) Messabeb, H.; Contamine, F.; Cézac, P.; Serin, J. P.; Gaucher, E. C. Experimental Measurement of CO2 Solubility in Aqueous NaCl Solution at Temperature from 323.15 to 423.15 K and Pressure of up to 20 MPa. J. Chem. Eng. Data 2016, 61, 3573−3584. (7) Guo, H.; Huang, Y.; Chen, Y.; Zhou, Q. Quantitative Raman Spectroscopic Measurements of CO2 Solubility in NaCl Solution from (273.15 to 473.15) K at p = (10.0, 20.0, 30.0 and 40.0) MPa. J. Chem. Eng. Data 2016, 61, 466−474. (8) Hou, S.-X.; Maitland, G. C.; Trusler, J. P. M. Phase equilibria of (CO2 + H2O + NaCl) and (CO2 + H2O + KCl): Measurements and modeling. J. Supercrit. Fluids 2013, 78, 78−88.

Figure 10. Salting out effect in CaCl2 solutions (1, 3, and 6 mol/kg): ●, 423.15 K; ■, 373.15 K; ◆, 323.15 K.

The CO2 solubility in calcium chloride solution at molalities of 3 and 6 mol/kg was determined over a wide range of pressure (5, 10, 15, 20 MPa) and temperature (323.15, 373.15, 423.15 K). CO2 solubility data in CaCl2 solution are reported in 36 different conditions. Our experimental solubility data presented an uncertainty of 2.1% obtained from repeatability and reproducibility experiment with ANOVA calculations. A strong salting out effect was observed and it was remarked that the pressure and temperature effects on the quantity of dissolved carbon dioxide decrease as the temperature and pressure increase.

Figure 11. Comparison between the salting out effect in NaCl solution and CaCl2 solutions at 323 K. ●, Salting out effect in NaCl solution; ■, salting out effect in CaCl2 solution. F



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(9) Tsai, E. S.; Jiang, H.; Panagiotopoulos, A. Z. Monte Carlo simulations of H2O−CaCl2 and H2O−CaCl2−CO2 mixtures. Fluid Phase Equilib. 2016, 407, 262−268. (10) Tong, D.; Trusler, J. P. M.; Vega-Maza, D. Solubility of CO2 in Aqueous Solutions of CaCl2 or MgCl2 and in a Synthetic Formation Brine at Temperatures up to 423 K and Pressures up to 40 MPa. J. Chem. Eng. Data 2013, 58, 2116−2124. (11) Prutton, C. F.; Savage, R. L. The solubility of carbon dioxide in calcium chloride-water solutions at 75, 100, 120°C and high pressures. J. Am. Chem. Soc. 1945, 67, 1550−1554. (12) Malinin, S. D. The system water-carbon dioxide at high temperature and pressures. Geochem. 1959, 3, 292−306. (13) Malinin, S. D.; Saveleva, N. I. The solubility of CO2 in NaCl and CaCl2 solutions at 25, 50 and 75 °C under elevated CO2 pressures. Geochem. Int. 1972, 9, 410−418. (14) Malinin, S. D.; Kurovskaya, N. A. Solubility of CO2 in chloride solutions at elevated temperatures and CO2 pressures. Geochem. Int. 1975, 12, 199−201. (15) Liu, Y.; Hou, M.; Yang, G.; Han, B. Solubility of CO2 in aqueous solutions of NaCl, KCl, CaCl2 and their mixed salts at different temperatures and pressures. J. Supercrit. Fluids 2011, 56, 125−129. (16) Bastami, A.; Allahgholi, M.; Pourafshary, P. 2014. Experimental and modelling study of the solubility of CO2 in various CaCl2 solutions at different temperatures and pressures. Pet. Sci. 2014, 11, 569−577. (17) Zhao, H.; Dilmore, R. M.; Lvov, S. N. Experimental studies and modeling of CO2 solubility in high temperature aqueous CaCl2, MgCl2, Na2SO4, and KCl solutions. AIChE J. 2015, 61, 2286−2297. (18) Mohammadian, E.; Hamidi, H.; Asadullah, M.; Azdarpour, A.; Motamedi, S.; Junin, R. Measurement of CO2 Solubility in NaCl Brine Solutions at Different Temperatures and Pressures Using the Potentiometric Titration Method. J. Chem. Eng. Data 2015, 60, 2042−2049. (19) Koschel, D.; Coxam, J. Y.; Rodier, L.; Majer, V. Enthalpy and solubility data of CO2 in water and NaCl(aq) at conditions of interest for geological sequestration. Fluid Phase Equilib. 2006, 247, 107−120.

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Experimental Measurement of CO2 Solubility in Aqueous CaCl2

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