Water Activity and Solubility Measurements and Model Simulation of

Feb 6, 2018 - its sub-binary systems at 323.15 K were elaborately measured by an isopiestic method. Moreover ... CsCl−MgCl2−H2O system was obtaine...
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Water Activity and Solubility Measurements and Model Simulation of the CsCl−MgCl2−H2O Ternary System at 323.15 K Lijiang Guo,*,†,‡ Lanying Tu,§ Yaxiao Wang,§ and Jianqiang Li‡ †

Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, P. R. China National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology, Key Laboratory of Green Process and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China § College of Chemical Engineer, Qinghai University, Xining 810016, P. R. China ‡

ABSTRACT: Water activities in the ternary system CsCl−MgCl2−H2O and its sub-binary systems at 323.15 K were elaborately measured by an isopiestic method. Moreover, the solubility of the CsCl−MgCl2−H2O system at 323.15 K was also measured by the flow-cloud-point method. A Pitzer model was used to predict the measured water activity and solubility data. The binary parameters for the CsCl−H2O system at 323.15 K were obtained by fitting the measured water activities for this binary system. The calculated water activity and solubility isotherms for the CsCl−MgCl2−H2O system at 323.15 K, with binary parameters only, deviated from the experimental values. This means that it is insufficient with binary parameters only to predict the water activity and calculate the solubility isotherms of the CsCl−MgCl2−H2O system at 323.15 K. The calculated solubility isotherms with both binary and mixing parameters, obtained by fitting the measured water activity, also deviated from experimental values. A new set of reasonable ternary parameters for the CsCl−MgCl2−H2O system was obtained by fitting the measured water activity and solubility data of this work. The calculated solubility isotherms with these parameters agreed with experimental results.

1. INTRODUCTION There are abundant cesium resources in the Chaerhan Salt Lake, which is located in the Chaidamu Basin, northwest of China. However, these resources are not recovered and utilized during the potash production process. The solubility and thermodynamic properties of the cesium salt related to the ternary system CsCl−MgCl 2−H2O at different temperatures, and their simulation by the thermodynamic model, are of great importance for extracting cesium resources from the salt lake. We have studied the thermodynamic properties and solubility of the CsCl−MgCl2−H2O ternary system at 298.15 K in our previous work.1 As a continuous work, this paper focuses on the thermodynamic properties and solubility of this ternary system at 323.15 K. The water activities for the MgCl2−H2O system at 323.15 K have been reported in the literature.2,3 Up to now, there has been no report on the water activity and solubility for the CsCl−MgCl2−H2O ternary system at 323.15 K, nor on their thermodynamic model simulation. We measured the water activity for the CsCl−MgCl2−H2O system at 323.15 K by an isopiestic method and determined the solubility of this ternary system using the flow-cloud-point method.4−6 A Pitzer model7,8 was used to simulate the water activity and solubility of the ternary systems measured in this work.

the materials, the method of purification, the impurity, etc., and more detailed information is given in what follows. The procedures of preparing the stock solutions of NaCl, MgCl2, and CsCl were described in the literature.1,9−12 Water used in the experiment is purified twice by deionization, and the conductance was less than 1.5 × 10−4 S·m−1 The NaCl (G.R.) and MgCl2·6H2O (A.R.), obtained from Sinopharm Chemical Reagent Co., Ltd., were purified three times by recrystallization; the impurities were less than 0.01% and 0.02%, respectively. CsCl (metals basis, 99.95%), bought from Aladdin, was used directly without further purification. ICP emission spectrometry (Thermo Electron Corporation, ICAP 6500 DUO) was used to analysis the impurities. The stock solution concentrations of NaCl, MgCl2, and CsCl were determined gravimetrically with AgNO3 as precipitant, and the relative deviations were controlled below 0.05%. 2.2. Apparatus and Procedures. The isopiestic experiment apparatus and procedures are the same as with our previous work.1,9,11,12 The solubility for the CsCl−MgCl2−H2O ternary systems at 323.15 K were measured by the flow-cloud-point method4−6 as in our previous work,1,9,12 except for the samples, namely a series of different mole fractions of CsCl YCsCl m (YCsCl = m +CsCl ) mixture stock solutions. The isopiestic m CsCl

2. EXPERIMENTAL SECTION 2.1. Materials. The chemical materials used in this experiment are tabulated in Table 1, including the producer of © XXXX American Chemical Society

MgCl 2

Received: May 21, 2017 Accepted: January 22, 2018

A

DOI: 10.1021/acs.jced.7b00459 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Table 1. Chemical Agents Used in This worka agents

grade

producer

method of purification

final purity

impurity analysis method

NaCl MgCl2·6H2O CsCl

G.R. A.R. metals basisb

Sinopharm Chemical Reagent Co., Ltd. Sinopharm Chemical Reagent Co., Ltd. Aladdin

recrystallization recrystallization no further purification

99.99% 99.98% 99.95%

ICP ICP ICP

The final impurity of the chemical agents was determined in this work, and the purity basis is mass. bMetals basis means that the purity of the product is determined by the metal content of the material. a

Table 2. Isopiestic Measured Water Activities of the CsCl−MgCl2−H2O Ternary System at 323.15 K and 0.077 MPaa mixture solution no.

mCsCl/mol·kg

1

1.0318 0.8596 0.6218 0.4114 0 2.8579 2.2104 1.8240 1.2659 0.8114 0 1.7517 3.1885 4.8704 5.7239 4.3220 3.4667 2.3227 1.4342 0

2

3 4 5 6

−1

reference solution mMgCl2/mol·kg

−1

0.1829 0.2875 0.4288 0.5465 0.7647 0 0.3918 0.6101 0.8729 1.0779 1.4115 0 0 0 0 0.7661 1.1595 1.6016 1.9052 2.3341

mNaCl/mol·kg−1

aw

1.2165

0.9591 ± 0.0010

2.6213

0.9068 ± 0.0010

1.6058 2.7805 4.1649 4.8003

0.9452 ± 0.0010 0.9015 ± 0.0010 0.8430 ± 0.0008 0.8152 ± 0.0008

The water activity is calculated by eq 1 and eq 2 with the parameters reported in our previous work,13 fitting the osmotic coefficients of NaCl reported by Pitzer.14 mNaCl means concentration of NaCl reference solution. The experiment was performed in Xining, and the average atmospheric pressure is 0.077 MPa. The relative standard uncertainty is ur(m) = 0.003, u(T) = 0.1 K, ur(p) = 0.1. a

and flow-cloud-point experimental apparatus and procedures will not be described again here.

(2)

and mMgCl2 mean the concentration of CsCl and MgCl2 in the mixture solution. 3.2. Determined Solubility Results. The measured solubility for the CsCl−MgCl2−H2O ternary system at 323.15 K by the flow-cloud-point method is tabulated in Table 3. 3.3. Discussions. The measured water activities in the CsCl−H2O system at 323.15 K are inversely proportional to the concentration, as shown in Figure 1. The measured water activities in the MgCl2−H2O system at 323.15 K agree well with the values reported previously,2,3 as shown in Figure 2. The measured composition points at constant water activity in the CsCl−MgCl2−H2O system at 323.15 K are not in straight lines, as shown in Figure 3. This phenomenon is the same with the situation of this ternary system at 298.15 K, the mixture’s behavior does not obey the Zdanovskii rule. This conclusion can also be confirmed by the inference of Stewart and Zener15 for the formation of ion clusters in CsCl solutions. The solubility measured by the flow-cloud-point method for the CsCl− MgCl2−H2O at 323.15 K is shown in Figure 4.

where ν is the number of ions for the complete dissociation of one molecule of the reference solutions. Mw is the molar mass of H2O. The isopiestic determined water activities of the CsCl− MgCl2−H2O ternary system at 323.15 K are tabulated in Table 2. mNaCl means the concentration of NaCl reference solution. mCsCl

4. MODELING The Pitzer thermodynamic model7,8 was used to predict the water activities and solubility in the CsCl−MgCl2−H2O system at 323.15 K. Since the CsCl−MgCl2−H2O ternary system is unsymmetrical (Cs and Mg have different charge), higher-order

3. RESULTS AND DISCUSSION 3.1. Isopiestic Measured Results. The NaCl solution was used as reference in the water activity determination. The osmotic coefficients ϕ of NaCl at 323.15 K13 as a function of molalities (m) (eq 1) have been reported.14 ϕ = a + b(m)0.5 + c(m) + d(m)1.5 + e(m)2 + f (m)2.5 + g (m)3 + h(m)3.5

(1)

where a, b, c, d, e, f, g, and h are empirical parameters and m is in units of mol·kg−1. The water activity aw of the reference solutions can be calculated by eq 1 and 2, ln a w =

−ν × M w × m × ϕ 1000

B

DOI: 10.1021/acs.jced.7b00459 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

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Table 3. Solubility of the CsCl−MgCl2−H2O System Measured by the Flow-Cloud-Point Method at 323.15 K and 0.077 MPaa solubility in mixture aqueous solutions no.

mCsCl/mol·kg−1

mMgCl2/mol·kg−1

solid phaseb

1 2 4 5 6 7 8 10 11

1.0364 2.1758 3.1756 4.6774 6.1793 8.6048 9.7612 10.5779 11.8232

5.0814 4.6078 4.3442 4.1011 3.8273 3.7728 2.7063 1.8396 0.8921

A A A A A c B B B

Figure 3. Isopiestic measured water activities for the CsCl−MgCl2− H2O system at 323.15 K. ●, Isopiestic experimental point; ---, experimental equal water activity lines at constant water activity; , Zdanoviskii rule.

a

Note: m, molality, moles per kilogram of solvent (pure water). The experiment was performed in Xining where the average atmospheric pressure is 0.077 MPa. The relative standard uncertainty is ur(m) = 0.004, u(T) = 0.1 K, ur(p) = 0.1. bThe solid phases are estimated according to the Pitzer model calculated results, and not detected in the experiment. A = CsCl·MgCl2·6H2O(s); B = CsCl(s). cExperiment no. 7 is near the eutonic point, and it is difficult to estimate the solid phase exactly.

Figure 4. Solubility of the CsCl−MgCl2−H2O system at 323.15 K. Experimental solubility: □, ref 3 for MgCl2·6H2O(s); ■, ref 16 for CsCl(s); ●, this work. Pitzer model values: , MgCl2·6H2O(s), with binary or binary and mixing parameters. With binary parameters only, (····) CsCl·MgCl2·6H2O(s), (−·−) CsCl(s); with mixing parameters obtained by fitting water activity, (---) CsCl·MgCl2·6H2O(s); with mixing parameters obtained by fitting water activities and solubility, (−−−) CsCl·MgCl2·6H2O(s), (−··−) CsCl(s).

Figure 1. Water activity of the CsCl−H2O binary system at 323.15 K. ○, isopiestic experimental point measured in this work; ―, calculated water activity in CsCl−H2O system at 323.15 K with binary Pitzer model parameters obtained in this work.

The parameters for the CsCl−H2O system at 323.15 K were obtained by fitting the measured water activities. The values are tabulated in Table 4. The recalculated water activities agree well with the experimental result, as shown in Figure 1. Table 4. Model Parameters for Binary Systems system

β(0)

β(1)

Cϕ

ref

MgCl2−H2O CsCl−H2O

0.33703 0.048375

1.79758 0.286151

0.00403 −0.001216

2 this work

The reported2 binary model parameters for the MgCl2−H2O system at 323.15 K were used directly. The recalculated water activities for the MgCl2−H2O system at 323.15 K agreed with experimental values of this work and literature,2,3 as shown in Figure 2. We try to predict the water activity of the CsCl−MgCl2−H2O ternary system with binary parameters only. The predicted water activities (aw(Calc1)) and the deviation (Δaw1) are shown in Table 5, the maximum deviation is as large as 0.0262. The calculated constant activity lines also largely deviated from the experimental

Figure 2. Water activity in the MgCl2−H2O system at 323.15 K. Experimental values: □, ref 2; △, ref 3; ●, this work; ―, calculated water activity by Pitzer model with parameters in the literature.2

electrostatic terms for unsymmetrical mixing θE have been included for the calculation. C

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Table 5. Calculated Water Activities and Deviation from Experimental Values for the CsCl−MgCl2−H2O System at 323.15 Ka Δaw

aw(Calc)

mixture solution mCsCl

mMgCl2

aw (Exp)

aw(Calc1)

aw(Calc2)

aw(Calc3)

Δaw1

Δaw2

Δaw3

1.0318 0.8596 0.6218 0.4114 0.0000 2.8579 2.2104 1.8240 1.2659 0.8114 0.0000 5.7239 4.3220 3.4667 2.3227 1.4342 0

0.1829 0.2875 0.4288 0.5465 0.7647 0.0000 0.3918 0.6101 0.8729 1.0779 1.4115 0.0000 0.7661 1.1595 1.6016 1.9052 2.3341

0.9591 0.9591 0.9591 0.9591 0.9591 0.9068 0.9068 0.9068 0.9068 0.9068 0.9068 0.8152 0.8152 0.8152 0.8152 0.8152 0.8152

0.9579 0.9579 0.9580 0.9584 0.9597 0.9089 0.9051 0.9033 0.9043 0.9058 0.9112 0.8141 0.7945 0.7890 0.7908 0.7975 0.8173

0.9579 0.9580 0.9581 0.9585 0.9597 0.9089 0.9076 0.9067 0.9076 0.9084 0.9112 0.8141 0.8169 0.8156 0.8141 0.8135 0.8173

0.9582 0.9583 0.9584 0.9587 0.9597 0.9089 0.9073 0.9062 0.9072 0.9080 0.9112 0.8141 0.8079 0.8049 0.8050 0.8075 0.8173

0.0012 0.0012 0.0011 0.0007 −0.0006 −0.0021 0.0017 0.0035 0.0025 0.0010 −0.0044 0.0011 0.0207 0.0262 0.0244 0.0177 −0.0021

0.0012 0.0011 0.0010 0.0006 −0.0006 −0.0021 −0.0008 0.0001 −0.0008 −0.0016 −0.0044 0.0011 −0.0017 −0.0004 0.0011 0.0017 −0.0021

0.0009 0.0008 0.0007 0.0004 −0.0006 −0.0021 −0.0005 0.0006 −0.0004 −0.0012 −0.0044 0.0011 0.0073 0.0103 0.0102 0.0077 −0.0021

a

Note: aw(Exp), experimental water activity measured in this work; aw(Calc), water activity calculated by the Pitzer model: aw(Calc1), with binary parameters only; aw(Calc2), with binary and ternary parameters obtained by fitting water activity data measured in this work; aw(Calc3), with binary and ternary parameters obtained by fitting water activity and solubility data measured in this work.

binary and these ternary parameters, the water activities and equal water activity lines were calculated. The calculated water activities (aw(Calc2)) and deviation (Δaw2) from the experimental values are tabulated in Table 5. The maximum deviation is −0.0021. This indicates that the thermodynamic properties of the CsCl−MgCl2−H2O ternary system can be presented by the Pitzer model. We have investigated whether the solubility of the CsCl− MgCl2−H2O ternary system at 323.15 K can be accurately predicted by the Pitzer model with binary or binary plus ternary parameters. The thermodynamic solubility products of MgCl2· 6H2O(s) at 323.15 K have been reported,2 as tabulated in Table 7.

result, as shown in dotted line in Figure 5. It seems that binary parameters are insufficient in representing the water activity for

Table 7. Logarithm of the Thermodynamic Solubility Products ln Ksp at 323.15 K

Figure 5. Calculated equal water activity lines and their comparison with the isopiestic measured results: ●, experimental isopiestic point. All lines are calculated equal water activity lines by Pitzer model: ····, with binary parameters only; ---, with binary parameters and ternary parameters fitting the water activity data; , with binary and ternary parameters fitting water activity and solubility data.

Table 6. Ternary Parameters for the System CsCl−MgCl2− H2O at 323.15 K θMN

ψMNX

fitting data

−0.049417 −0.021113

aw in Table 2 aw and solubility data of this work

ln Ksp

ref

9.8650 4.48 11.4

2 this work this work

The thermodynamic solubility product of the solid phases CsCl(s) and CsCl·MgCl2·6H2O(s) have not been reported yet. According to the reported16 solubility data for CsCl(s) and measured solubility for CsCl·MgCl2·6H2O(s) in this work, 323.15 K, we obtained the corresponding thermodynamic solubility products, as shown in Table 7. With binary only parameters, the solubility isotherms of MgCl2·6H2O(s), CsCl·MgCl2·6H2O(s), and CsCl(s) solid phases at 323.15 K are calculated, as shown in the solid line, dotted line, and dot dash line in Figure 4, respectively. The calculated results deviate largely from the measured experimental results. This indicates that binary parameters only are insufficient in predicting the solubility of the CsCl−MgCl2−H2O system at 323.15 K. With binary and ternary parameters obtained by fitting the water activities, the solubility isotherms for MgCl2·6H2O(s) and CsCl·MgCl2·6H2O(s) are calculated. The calculated solubility

the CsCl−MgCl2−H2O ternary system at 323.15 K. Possibly, reasonable ternary parameters are needed. The ternary Pitzer model parameters for the CsCl−MgCl2− H2O system at 323.15 K were obtained by fitting the measured water activities, and the values are tabulated in Table 6. With

0.05687 −0.016078

solid phase MgCl2·6H2O CsCl CsCl·MgCl2·6H2O

D

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isotherms for MgCl2·6H2O(s) are the same with that calculated with binary parameters. The calculated results for CsCl·MgCl2· 6H2O(s) largely deviate from the experimental values, as shown in the short dash line in Figure 4. This indicates that the ternary Pitzer model parameters are not reasonable, at least in the aspect of calculating the solubility isotherms. The new Pitzer model ternary parameters for the CsCl− MgCl2−H2O system at 323.15 K are obtained by fitting water activities together with measured solubility data, as shown in Table 6. With the binary and new set of ternary parameters, the water activities, the equal water activity lines, and solubility isotherms for the CsCl−MgCl2−H2O ternary system are calculated. The calculated water activities (aw(Calc3)) and the deviation (Δaw3) from the experiment are shown in Table 5, and the maximum deviation is 0.0103. The calculated equal water activity lines slightly deviated from the experimental values, especially at low water activity, as shown by solid lines in Figure 5. The calculated solubility isotherms for the solid phases CsCl· MgCl2·6H2O(s) (dash line) and CsCl (dash dot dot line) are consistent with experimental solubility data, as shown in Figure 4.

REFERENCES

(1) Guo, L. J.; Wang, Y. X.; Tu, L. Y.; Li, J. Q. Thermodynamics and Phase Equilibrium of the System CsCl−MgCl2−H2O at T = 298.15 K. J. Chem. Eng. Data 2017, 62, 1397−1402. (2) Han, H. J.; Li, D. D.; Guo, L. J.; Yao, Y.; Yang, H. T.; Zeng, D. W. Isopiestic Measurements of Water Activity for the NaCl−KCl−MgCl2− H2O Systems at 323.15 K. J. Chem. Eng. Data 2015, 60, 1139−1145. (3) Christov, C. Isopiestic Determination of the Osmotic Coefficients of an Aqueous MgCl2 + CaCl2 Mixed Solution at (25 and 50) °C. Chemical Equilibrium Model of Solution Behavior and Solubility in the MgCl2 + H2O and MgCl2 + CaCl2 + H2O Systems to High Concentration at (25 and 50) °C. J. Chem. Eng. Data 2009, 54, 627−635. (4) Zhang, L. Z.; Gui, Q. L.; Lu, X. H.; Wang, Y. R.; Shi, J. Measurement of Solid-Liquid Equilibria by a Flow-Cloud-Point Method. J. Chem. Eng. Data 1998, 43, 32−37. (5) Zhang, L. Z.; Gui, Q. L.; Lu, X. H.; Wang, Y. R.; Shi, J. Measurement of Solid-Liquid Equilibrium for the System Containing Salts by a Flow Cloud-Point Method. J. Nanjing Univ. Chem. Technol., Nat. Sci. Ed. (in Chinese) 1997, 19, 19−24. (6) Shi, X. D.; Lu, X. H.; Wang, Y. R.; Shi, J. Measurement and Prediction of Liquid-liquid Equilibrium of Water-1-butanol in the Presence of Calcium Chloride. J. Nanjing Univ. Chem. Technol., Nat. Sci. Ed. (in Chinese) 2001, 23, 49−51. (7) Pitzer, K. S. Thermodynamics of Electrolytes. I. Theoretical Basis and General Equations. J. Phys. Chem. 1973, 77, 268−277. (8) Pitzer, K. S.; Mayorga, G. Thermodynamics of Electrolytes. II. Activity and Osmotic Coefficients for Strong Electrolytes with One or Both Ions Univalent. J. Phys. Chem. 1973, 77, 2300−2308. (9) Guo, L. J.; Han, H. J.; Dong, O. Y.; Yao, Y. Thermodynamics and Phase Equilibrium of the High Concentration Solid Solution-Aqueous Solution System KCl−RbCl−H2O from T= 298.15 K to T = 323.15 K. J. Chem. Thermodyn. 2017, 106, 285−294. (10) Guo, L. J.; Sun, B.; Zeng, D. W.; Yao, Y.; Han, H. J. Isopiestic Measurement and Solubility Evaluation of the Ternary System LiCl− SrCl2−H2O at 298.15 K. J. Chem. Eng. Data 2012, 57, 817−827. (11) Guo, L. J.; Zeng, D. W.; Yao, Y.; Han, H. J. Isopiestic Measurement and Solubility Evaluation of the Ternary System (CaCl2 + SrCl2 + H2O) at T = 298.15 K. J. Chem. Thermodyn. 2013, 63, 60−66. (12) Guo, L. J.; Wang, Y. X.; Tu, L. Y.; Li, J. Q. Water Activity and Solubility Measurement and Pitzer model Simulation of the MgCl2− RbCl−H2O Ternary System at 298.15 K. J. Solution Chem. 2017, 46, 1767−1777. (13) Pitzer, K. S.; Peiper, J. C.; Busey, R. H. Thermodynamic Properties of Aqueous Sodium Chloride Solutions. J. Phys. Chem. Ref. Data 1984, 13, 1−102. (14) Han, H. J.; Guo, L. J.; Li, D. D.; Dong, O. Y.; Yao, Y.; Zhang, N.; Zeng, D. W. Water Activity Measurements by the Isopiestic Method for the MCl−CaCl2−H2O (M = Na, K) Systems at 323.15 K. J. Chem. Eng. Data 2015, 60, 2285−2290. (15) Stewart, R. F.; Zener, C. Cluster Formation in Aqueous Solutions of Strong Electrolytes. J. Phys. Chem. 1988, 92, 1981−1985. (16) Plyushchev, V. E.; Tulinova, V. B.; Kuznetsova, G. P.; Korovin, S. S.; Shipetina, N. S. Investigation of the Ternary System Sodium Chloride-Cesium Chloride-Water. Zh. Neorg. Khim. 1957, 2, 2654− 2660.

5. CONCLUSIONS Water activities in the CsCl−MgCl2−H2O system and subbinary systems at 323.15 K were isopiestic measured. The measured water activities of the MgCl2−H2O binary system agree well with literature. The experimental equal water activity lines in the ternary system are not in a straight line, which means the mixture behavior does not obey the Zdanovskii rule. Solubility of the CsCl−MgCl2−H2O ternary systems at 323.15 K was measured by the flow-cloud-point method. The Pitzer model was used to predict the measured water activity and solubility of the CsCl−MgCl2−H2O ternary systems at 323.15 K. The binary Pitzer model parameters for the CsCl− H2O system at 323.15 K was obtained by fitting the measured water activities. The calculated water activities and solubility isotherms for the CsCl−MgCl2−H2O ternary system at 323.15, with binary parameters only, deviated largely from the experimental values. Two sets of ternary parameters of the CsCl−MgCl2−H2O system at 323.15 K were obtained by fitting water activities, water activity together with solubility data, respectively. The solubility isotherms for CsCl·MgCl2·6H2O(s) and CsCl(s) calculated with ternary parameters, fitting to water activities and solubility data, agree with the experimental solubility data.

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AUTHOR INFORMATION

Corresponding Author

*E-mail: [email protected]. ORCID

Lijiang Guo: 0000-0002-1018-4646 Funding

This work is financially supported by National Science Foundation of China (Grant Nos. 21303239, U1407137 and U1507101), Natural Science Foundation of Inner Mongolia (Grant No. 2017BS0201), and National Key Research and Development Plan of China (Grant No. 2016YFC0700905). Notes

The authors declare no competing financial interest. E

DOI: 10.1021/acs.jced.7b00459 J. Chem. Eng. Data XXXX, XXX, XXX−XXX