Solubility of Nesquehonite and Calcite in Pressurized Carbonated

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

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Solubility of Nesquehonite and Calcite in Pressurized Carbonated Water from 293.15 to 343.15 K Jing Bo,†,‡,§ Yifei Zhang,*,†,‡ and Yi Zhang†,‡ †

Key Laboratory of Green Process and Engineering and ‡National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China § University of Chinese Academy of Sciences, Beijing 100049, China

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S Supporting Information *

ABSTRACT: The solubility of nesquehonite (MgCO3·3H2O) and calcite (CaCO3) in carbonated water with CO2 pressure of between 1 and 5 MPa was measured from 293.15 to 343.15 K by the inductively coupled plasma optical emission spectrometry (ICPOES) analysis method. The results showed that the solubility increased with CO2 pressure but decreased with temperature in all of the studied situations, and for the ones where the two solid phases coexisted, nesquehonite’s solubility changed little from that of the single-existing cases while calcite’s declined by 1 order of magnitude. The solubility was correlated with both temperature and CO2 pressure by empirical equations in a concise form.

1. INTRODUCTION The carbonation method is often used to produce basic magnesium carbonate or magnesium oxide from minerals rich in magnesium such as magnesite, dolomite, and boron mud.1−10 During our research of leaching magnesium hydroxide from boron mud,11 we found that pressurized leaching under a CO2 pressure of 1 to 5 MPa had an enhancing effect as the MgO concentration in the solution increased considerably while the impurities’ concentrations, especially the CaO concentration, were kept acceptably low. The solubility of nesquehonite and calcite, the solid phases precipitated during the carbonation, was considered to be the critical reason for the enhanced result of the carbonation process. However, few have reported experimental studies focused on this system under the pressurized carbonation conditions. Nesquehonite’s solubility in water was measured mainly under CO2 pressures of up to 1 atm12−19 and infrequently under certain CO2 pressures of between 2 to 21 atm at certain temperatures.19−21 Similarly, besides those measured at either temperatures higher than 348.15 K or much too high CO2 pressures,22−26 most of the solubility data of calcite in water were for CO2 pressures of up to 1 atm18,27−38 and sparse for certain CO2 pressures of between 2 and 56 atm at certain temperatures.20,38−40 The solubility of nesquehonite and calcite in carbonated water where the two solid phases coexisted was measured under the conditions of CO2 pressure of 1 atm and temperatures from 273.15 to 363.15 K.15 Cases for pressurized carbonation conditions needed to be investigated. In this work, the solubility of nesquehonite and calcite in carbonated water, both for the single solid-phase systems and the two coexisting systems, was measured at a CO2 pressure of 1 to 5 MPa and a temperature of 293.15 to 343.15 K by the inductively coupled plasma optical emission spectrometry © XXXX American Chemical Society

analysis method. Moreover, empirical correlation equations for the solubility with temperature and CO2 pressure were obtained.

2. EXPERIMENTAL SECTION 2.1. Materials. The materials used in this work are listed in Table 1 and were used without further purification. Nesquehonite was obtained by carbonating 200 g of magnesium hydroxide with 1 kg of deionized water in a 2 L high-pressure autoclave (4524, Parr) under the conditions of 5 MPa CO2 pressure, 700 rpm stirring speed, and 50 °C for 1 h, filtering the slurry, and freeze-drying the filter cakes for 48 h after washing with water three times. The synthesized nesquehonite product’s XRD (X’Pert PRO MPD, PANalytical) pattern is shown in Figure S1. Samples from every batch were dissolved by excess hydrochloric acid and diluted for ICP analysis, and an average mass fraction purity value was obtained. Other chemicals were commercial products of analytical reagent grade. All aqueous solutions were prepared with deionized water. 2.2. Solubility Measurement. Solutes of excess mass (138 g for nesquehonite and 2.5 g for calcite) were mixed with 500 g of water in a 2 L high-pressure autoclave. The temperature was automatically controlled by the electric heating jacket and the water in the cooling coils of the autoclave. After the reactant slurry was heated to a certain temperature, CO2 was quickly introduced into the autoclave through a tube for both gas inlet and sampling, and the pressure was maintained throughout the experiments. At the experimental reaction time, samples were filtered (with 0.22 μm pore-size paper) immediately Received: March 9, 2018 Accepted: June 19, 2018

A

DOI: 10.1021/acs.jced.8b00185 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

Table 1. Sources and Purities of Chemicals chemical name

CAS

mass fraction purity

source

magnesium hydroxide magnesium carbonate trihydrate calcium carbonate hydrochloric acid carbon dioxide

1309-42-8 5145-46-0 471-34-1 7647-01-0 124-38-9

≥0.98 0.9969 (6−130 μm) ≥0.99 (0.3−60 μm) 0.36−0.38 ≥0.99

Shantou Xilong Chemical Industry Co., Ltd. synthesis Shantou Xilong Chemical Industry Co., Ltd. Beijing Chemical Works Beijing Qianxijingcheng Gas Co., Ltd.

analysis method ICPa

a

Inductively coupled plasma optical emission spectrometry (ICP-OES, iCAP 6300, Thermo Scientific).

Table 2. Mole Fraction Solubility of Nesquehonite x1 in Carbonated Water at Tempereature T and CO2 Pressure Pa T/K

P/MPa

102x1

T/K

P/MPa

102x1

T/K

P/MPa

102x1

293.15

1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0

1.320 1.539 1.669 1.709 1.826 1.862 1.963 1.977 2.031 1.038 1.154 1.324 1.380 1.465 1.500 1.569 1.612 1.629

313.15

1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0

0.787 0.912 1.038 1.119 1.185 1.275 1.293 1.356 1.401 0.618 0.746 0.813 0.896 0.971 1.085 1.140 1.177 1.216

333.15

1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0

0.518 0.618 0.708 0.766 0.848 0.908 0.925 0.945 0.992 0.414 0.493 0.555 0.641 0.677 0.748 0.809 0.818 0.836

303.15

323.15

343.15

a

x1 is expressed as the mole fraction of MgCO3. Standard uncertainties u(T) = 1 K, u(P) = 0.01 MPa, and u(x1) = 0.001.

1.5 h for 303.15 and 313.15 K, 1 h for 323.15 K, and 0.5 h for 333.15 and 343.15 K. The equilibrium time of calcite single-existing cases was 4 h for 293.15 K, 2 h for 303.15 K, 1 h for 313.15 and 323.15 K, and 0.5 h for 333.15 and 343.15 K. The equilibrium time in coexisting cases was 48 h for 293.15 K, 24 h for 303.15 K, and 3 h for 313.15 to 343.15 K. The solid samples were dried in a freeze-dryer for phase analysis. The formal dissolution reactions of nesquehonite and calcite in carbonated water could be expressed as eqs 1 and 2, respectively, and the solubilities were obtained by analyzing the concentrations of magnesium or calcium in the solutions using the ICP method. As the solution volume was approximately changeless, the mole fraction solubilities x1 of nesquehonite in the single-existing cases, x2 of calcite in the single-existing cases, x1′ of nesquehonite in the coexisting cases, and x2′ of calcite in the coexisting cases were calculated on the basis of eqs 3 to 6, respectively. Figure 1. Experimental data of nesquehonite’s solubility from this work at T = 293.15, 303.15, 313.15, 323.15, 333.15, and 343.15 K (■, ●, ▲, ▼, ◆, and ◀, respectively) and from the literature at T = 298.15 K (□)20 and at T = 291.15 K (○).21 The lines are for visual guides only.

MgCO3 · 3H 2O + CO2 + H 2O F Mg 2 + + 2HCO3− + 3H 2O (1)

CaCO3 + CO2 + H 2O F Ca 2 + + 2HCO3−

after being withdrawn from the sampling tube. The filtrate was instantly diluted for composition analysis, and excess hydrochloric acid was added dropwise to ensure that no precipitation occurred. Dissolution equilibrium was considered to be achieved when three successive samples’ solution compositions were constant without solid-phase transformation. The equilibrium time of nesquehonite single-existing cases was 8 h for 293.15 K,

x1 =

(2)

(wMg /g· L−1)/(24.305/g· mol−1) −1

(wMg /g· L )/(24.305/g ·mol−1) + cCO2/mol · kg −1H 2O + 1000/18.015

(3) −1

x2 =

−1

(wCa /g ·L )/(40.078/g ·mol ) (wCa /g ·L−1)/(40.078/g· mol−1) + cCO2/mol· kg −1H 2O + 1000/18.015

(4) B



Article

Table 3. Mole Fraction Solubility of Calcite x2 in Carbonated Water at Tempereature T and CO2 Pressure Pa T/K

P/MPa

104x2

T/K

P/MPa

104x2

T/K

P/MPa

104x2

293.15

1.0 2.0 3.0 4.0 5.0 1.0 2.0 3.0 4.0 5.0

4.004 5.013 5.484 5.710 5.903 3.455 4.384 4.776 5.131 5.347

313.15

1.0 2.0 3.0 4.0 5.0 1.0 2.0 3.0 4.0 5.0

2.796 3.785 4.147 4.312 4.745 2.332 3.164 3.584 3.859 4.011

333.15

1.0 2.0 3.0 4.0 5.0 1.0 2.0 3.0 4.0 5.0

2.064 2.595 2.928 3.206 3.449 1.652 2.113 2.430 2.871 3.009

303.15

323.15

343.15

a

Standard uncertainties u(T) = 1 K, u(P) = 0.01 MPa, and u(x2) = 0.00001. x1′ =

x 2′ =

(wMg /g· L−1)/(24.305/g· mol−1) (wMg /g· L−1)/(24.305/g·mol−1) + (wCa /g· L−1)/(40.078/g· mol−1) + cCO2/mol ·kg −1H 2O + 1000/18.015

(5)

(wCa /g·L−1)/(40.078/g· mol−1) (wMg /g·L−1)/(24.305/g·mol−1) + (wCa /g· L−1)/(40.078/g· mol−1) + cCO2/mol ·kg −1H 2O + 1000/18.015

(6)

where wMg and wCa are the mass concentrations of magnesium and calcium in the solutions, respectively, and cCO2 is the solubility of CO2 in water, which could be obtained from a computational model in the literature41 (Table S1).

3. RESULTS AND DISCUSSION 3.1. Solubility of Nesquehonite in the Single-Existing System. The mole fraction solubility of nesquehonite in carbonated water within the temperature range of 293.15 to 343.15 K and the CO2 pressure range of 1 to 5 MPa is presented in Table 2. Nesquehonite’s solubility increased with CO2 pressure but decreased with temperature as higher CO2 pressure and lower temperature improved the solubility of CO2 in the solution.42 The comparison between experimental data from this work and the literature is shown in Figure 1. Data from Mitchell20 were lower than what we found while the ones from Haehnel21 were close. Nesquehonite was reported to transform into hydromagnesite at 313.15 to 333.15 K in an aqueous medium,16,43−49 and the existence of nesquehonite at high temperatures may contribute to the high CO2 pressure.43,49 However, transformation would still happen after a long enough time at temperatures higher than 313.15 K.

Figure 2. Experimental data of calcite’s solubility from this work at T = 293.15, 303.15, 313.15, 323.15, 333.15, and 343.15 K (■, ●, ▲, ▼, ◆, and ◀, respectively) and from the literature at T = 298.15 K (□,38 ○,20 and ▽),40 T = 291.15 K for (△),39 and T = 315.15, 323.15, 333.15, and 343.15 K (◇, ◁, ▷, and ☆, respectively).40 The lines are for visual guides only.

Table 4. Mole Fraction Solubility of Nesquehonite x1′ and Calcite x2′ in Carbonated Water for the Coexisting System at Tempereature T and CO2 Pressure Pa T/K

P/MPa

102x1′

105x2′

T/K

P/MPa

102x1′

105x2′

293.15

1.0 2.0 3.0 4.0 5.0 1.0 2.0 3.0 4.0 5.0

1.270 1.619 1.797 1.983 2.072 1.005 1.325 1.474 1.575 1.689

2.662 3.133 3.418 3.672 3.841 2.184 2.552 2.825 3.053 3.150

323.15

1.0 2.0 3.0 4.0 5.0 1.0 2.0 3.0 4.0 5.0

0.620 0.814 0.926 1.025 1.113 0.500 0.641 0.751 0.838 0.910

1.331 1.542 1.745 1.812 1.882 1.012 1.149 1.328 1.404 1.440

303.15

333.15

C



Article

Table 4. continued T/K

P/MPa

102x1′

105x2′

T/K

P/MPa

102x1′

105x2′

313.15

1.0 2.0 3.0 4.0 5.0

0.796 0.970 1.193 1.261 1.380

1.747 2.018 2.228 2.385 2.510

343.15

1.0 2.0 3.0 4.0 5.0

0.405 0.497 0.613 0.686 0.746

0.737 0.797 0.919 0.969 1.006

x1′ is expressed as the mole fraction of MgCO3. Standard uncertainties u(T) = 1 K, u(P) = 0.01 MPa, u(x1′ ) = 0.001, and u(x2′ ) = 0.000001.

a

Figure 3. Solubility of nesquehonite in the coexisting system under P = 1, 2, 3, 4, and 5 MPa (■, ●, ▲, ▼, and ◆, respectively) and in the single-existing system under P = 1, 2, 3, 4, and 5 MPa (□, ○, △, ▽, and ◇, respectively). The lines are for visual guides only. xMgCO3·3H2O is the mole fraction solubility of nesquehonite.

Figure 5. Correlation of nesquehonite’s solubility in the single-existing system with temperature and CO2 pressure. The balls with circle projections are experimental values, and the cross hatch is the fitting surface.

Figure 4. Solubility of calcite in the coexisting system under P = 1, 2, 3, 4, and 5 MPa (■, ●, ▲, ▼, and ◆, respectively) and in the singleexisting system under P = 1, 2, 3, 4, and 5 MPa (□, ○, △, ▽, and ◇, respectively). The lines are for visual guides only. xCaCO3 is the mole fraction solubility of calcite.

Figure 6. Correlation of calcite’s solubility in the single-existing system with temperature and CO2 pressure. The balls with circle projections are experimental values, and the cross hatch is the fitting surface.

3.2. Solubility of Calcite in the Single-Existing System. The mole fraction solubility of calcite in carbonated water at temperatures of 293.15 to 343.15 K and CO2 pressures of 1 to 5 MPa is as shown in Table 3. Calcite’s solubility also increased with CO2 pressure and decreased with temperature while the values were about 2 orders of magnitude lower than those of nesquehonite. Figure 2 exhibited the comparison between the experimental data from this work and

that of the literature. Data from Mitchell20 and Haehnel39 were higher than what we found while the ones from Miller40 were lower. The law of the change of solubility with pressure in the data showed consistency except for data from Visscher and Vanderdeelen,38 where the solubility decreased with increased CO2 pressure after 1.63 MPa. D



Article

3.3. Solubility of Nesquehonite and Calcite in the Coexisting System. The mole fraction solubility of nesquehonite and calcite in carbonated water for the two solid-phase coexisting cases was measured within the temperature range of 293.15 to 343.15 K and the CO2 pressure range of 1 to 5 MPa and presented in Table 4. As shown in Figures 3

and 4, nesquehonite’s solubility changed little from that of the single-existing cases while calcite’s decreased by 1 order of magnitude. This phenomenon of calcite was different from the reported data on its solubility under CO2 pressure lower than 1 atm in the presence of magnesium ions where the solubility was close to or higher than that of pure calcite.50,51 It may be attributed to no magnesian calcite of lower stability forming during this work’s experimental conditions and the ion pairing of magnesium ions with the bicarbonate ions in the solution. Moreover, the dissolution of nesquehonite gave high concentrations of HCO3−, and in order to preserve the solubility product for calcite, the calcium concentrations decreased. The XRD patterns of the equilibrium solid phases are shown in Figure S2. 3.4. Correlation of Solubility with Both Temperature and CO2 Pressure. The solubility was correlated with both temperature and CO2 pressure by empirical equations in the form of eq 7 (Figures 5−8), and the fitting results were summarized in Table 5. ln x =

a + b ln(P /MPa) + c T /K

(7)

where x is the mole fraction solubility, T is temperature, P is CO2 pressure, and a, b, c, d, e, and f are the parameters of the empirical equation. The predicted solubilities are in good agreement with the experimental data, indicating that the relationship of the solubility with temperature and CO2 pressure could be reproduced well by eq 7. The present results are convenient and practical for industrial applications and as investigative references relating to these systems.

Figure 7. Correlation of nesquehonite’s solubility in the coexisting system with temperature and CO2 pressure. The balls with circle projections are experimental values, and the cross hatch is the fitting surface.

4. CONCLUSIONS The solubility of nesquehonite and calcite in carbonated water with CO2 pressure of between 1 and 5 MPa was measured at from 293.15 to 343.15 K. It was found that nesquehonite’s solubility was about 2 orders of magnitude higher than that of calcite for the single-solid-phase cases, and when compared with the two-phase coexisting case, the former changed little while the latter decreased by 1 order of magnitude. The solubility was correlated with both temperature and CO2 pressure by empirical equations as ln x1 =

1975.43759 + 0.36678 ln(P /MPa) − 11.14619 T /K

ln x 2 =

1588.52467 + 0.31085 ln(P /MPa) − 13.24623 T /K

for the single-existing system and Figure 8. Correlation of calcite’s solubility in the coexisting system with temperature and CO2 pressure. The balls with circle projections are experimental values, and the cross hatch is the fitting surface.

ln x1 =

2215.12229 + 0.34882 ln(P /MPa) − 11.92996 T /K

Table 5. Parameters of Empirical Equations Correlated from Experimental Data parameters nesquehonite calcite coexisting

102b

a

solutes

nesquehonite calcite

1975.43759 1588.52467 2215.12229 2640.79986

± ± ± ±

34.59692 49.10804 31.07613 74.31183

36.678 31.085 34.882 22.449 E

± ± ± ±

adj. R2

c 1.161 1.467 0.928 2.219

−11.14619 −13.24623 −11.92996 −19.45682

± ± ± ±

0.10981 0.15566 0.0985 0.23555

0.98770 0.98095 0.99555 0.97917


Journal of Chemical & Engineering Data ln x 2 =

Article

2640.79986 + 0.22449 ln(P /MPa) − 19.45682 T /K

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for the coexisting system.

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ASSOCIATED CONTENT

* Supporting Information S

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jced.8b00185. The XRD patterns of the synthesized nesquehonite product (Figure S1) and the equilibrium solid phases in the two-solute coexisting system (Figure S2). (PDF)

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. Tel/Fax: +86-10-82544826. ORCID

Jing Bo: 0000-0002-5599-0799 Funding

We acknowledge the financial support from the National Natural Science Foundation of China (grant no. 21276258) and the National 863 Project of China (grant no. 2011AA060701). Notes

The authors declare no competing financial interest.

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REFERENCES

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Solubility of Nesquehonite and Calcite in Pressurized Carbonated

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