Phase Equilibria of the Ternary Systems ZnCl2âMgCl2âH2O and

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

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Phase Equilibria of the Ternary Systems ZnCl2−MgCl2−H2O and ZnCl2−PbCl2−H2O at 323 K Xiao-Feng He,† Yun-Yun Gao,† Shi-Hua Sang,*,†,‡,§ and Ning-fei Lei‡ †

College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China State Environmental Protection Key Laboratory of Synergetic Control and Joint Remediation for Soil & Water Pollution, Chengdu University of Technology, Chengdu 610059, P. R. China § Mineral Resources Chemistry Key Laboratory of Sichuan Higher Education Institutions, Chengdu 610059, P. R. China

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ABSTRACT: The solubility relationships of the ternary systems ZnCl2−MgCl2−H2O and ZnCl2−PbCl2−H2O at 323 K were studied by isothermal dissolution equilibrium method in this work. For the ternary system ZnCl2−MgCl2− H2O, the phase diagram contains two invariant points, three univariant curves, and three crystalline regions corresponding to MgCl2·6H2O, MgZnCl4·6H2O, and ZnCl2 at 323 K, while the double salt MgZnCl4·5H2O was produced in the same system at 373 K. The ternary system ZnCl2−PbCl2−H2O is a simple cosaturated system with only one invariant point that is saturated with PbCl2 and ZnCl2, two univariate curves and two crystallization zones corresponding to PbCl2 and ZnCl2, and the crystallization zone of PbCl2 is much larger than that of ZnCl2. galena concentrate was studied5,6 by continuously improving the experimental conditions. At the same time, the study on the leaching process of galena is also in full swing. The leaching of galena in CaCl2 and MgCl2 solutions has also been explored,7 and the concentration of PbCl2 solution leaching under this condition is 50% higher than that in saturated PbCl2. Hydrogen peroxide was used to leach lead in acetic acid solution.8 The experimental results showed that increasing the amount of hydrogen peroxide and the concentration of acetic acid to 3 mol/L can accelerate the dissolution of galena. Furthermore, the leaching of minerals containing silver, lead, and zinc at 130−170 °C under pressure was also studied,9 and it was found that the leaching rate of silver and lead can reach 90% and 80% in the case of 0.15 mol/L nitric acid at 130 °C, respectively. Therefore, the studies of the phase diagrams of the water− salt systems containing lead and zinc have practical significance. The crystallographic relationship provided by the phase diagrams has a certain guiding significance for the crystallization sequence of the leachate. The solubility relationships of various substances reflected in the phase diagrams of the systems containing Zn and Pb will play an important role in the separation and enrichment of leaching solution of the Pb−Zn ore, and also play a guiding role in understanding the solubility relationships between chlorides. Some related systems have been reported, such as the phase

1. INTRODUCTION As a branch of thermodynamics research, the studies of solubilities in water−salt systems play a vital role in basic thermodynamics. At the same time, due to the separation of valuable elements in brine extraction and other fields in Saline Lake, the researches on solubilities of the water−salt systems have been persistent for a long time. For example, to solve the salt separation process of lithium−magnesium−potassium− sulfate-type salt lakes in western China, the metastable phase diagrams of the ternary system K2SO4−MgSO4−H2O at 288 K and 308 K and the quaternary system Li2SO4−K2SO4− MgSO4−H2O at 288 K were studied.1,2 In addition, the studies of phase diagrams, especially in the synthesis of some special compounds, have their own advantages. The quaternary system KCl−ZnCl2−HCl−H2O containing 10.61% hydrochloric acid has been determined,3 and two different alien component salts 2KCl·ZnCl2·H2O and 5KCl·4ZnCl2·3H2O were prepared. This preparation can only be carried out by the phase equilibrium method. If the solution is formulated into a molar ratio and then evaporated to dryness, the two substances which are pure will not be obtained. China’s lead and zinc resources are abundant. When smelting lead-containing minerals, pyrometallurgical methods are often used, and the production of lead metal by pyrometallurgical production accounts for more than 80% of the world’s lead production.4 But there are a variety of environmental pollution problems in the metallurgical process. Although there is a certain or greater improvement, there is still no thorough solution. Therefore, the thought of wet lead smelting is used by scientists. The suspension electrolysis of © XXXX American Chemical Society

Received: July 14, 2018 Accepted: December 5, 2018

A

DOI: 10.1021/acs.jced.8b00605 J. Chem. Eng. Data XXXX, XXX, XXX−XXX

Journal of Chemical & Engineering Data

Article

equilibria of the ternary systems CaCl2−ZnCl2−H2O and KCl−ZnCl2−H2O at 373 K.10 The solubility relationships of the ternary system NaCl−ZnCl2−H2O at 260.35 and 250.15 K and the density relationships from 288.15 to 321.35 K were also studied,11 the values of which were used as a workover fluid for drilling in the petroleum industry. The phase diagrams of the ternary system CaCl2−ZnCl2−H2O at 0 and 25 °C12 were carried out, and a new compound CaCl2·ZnCl2·5H2O was produced. In addition, the phase diagram of the ternary system CaCl2−ZnCl2−H2O at 15 °C13 has also been studied. The solubility relationships between H+, Li+, NH4+, Na+, K+, Mg2+, Ca2+, Sr2+, Ba2+, Hg2+, and lead ion at 25 °C, and the solid phases were also identified.14 However, the phase equilibria of the ternary systems ZnCl2−MgCl2−H2O and ZnCl2−PbCl2−H2O at 323 K have not been reported. In this work, the phase equilibria of the ternary systems ZnCl2− MgCl2−H2O and ZnCl2−PbCl2−H2O at 323 K were studied by the isothermal dissolution equilibrium method, and the solubilities of the ternary systems listed above at 323 K were measured, the corresponding equilibrium solid phases were also determined. The results can provide theoretical support for element separation and enrichment in hydrometallurgy and heavy metals recovery from wastewater.

In the equilibrium liquid phase, the content of the elements was determined by chemical analysis combined with instrumental analysis. The chemical composition of the solid phases was determined by the Schreinemakers wet solid phase method combined with the X-ray powder crystal diffraction method. 2.3. Analytical Methods. In the ternary system ZnCl2− MgCl2−H2O, the content of zinc (Zn2+) was analyzed by EDTA volumetric method, it was titrated using hydrochloric acid-hexamethylenetetramine as buffer solution (pH = 5) and in the presence of xylenol orange as indicator. At this time, because of the effect of EDTA acid, the magnesium ion was masked, and the relative standard uncertainty of analysis results was not greater than 0.003. The determination of magnesium ion (Mg2+) was carried out by EDTA volumetric method, and chrome black T was used as an indicator. At this time, the titration result was the sum of magnesium and zinc ions, and the content of magnesium ion was obtained by subtracting the content of zinc ion. The relative standard uncertainty of analysis results was not greater than 0.005. In the ternary system ZnCl2−PbCl2−H2O, the amounts of zinc and lead ions were titrated with xylenol orange as indicator and hydrochloric acid−hexamethy−lenetetramine as buffer solution (pH = 5), whose relative standard uncertainty of analysis results was not greater than 0.003. The content of lead ion (Pb2+) was determined by flame atomic absorption. The relative standard uncertainty of analysis results was not greater than 0.02, and the content of zinc ion was obtained by subtraction. The samples were counted three times in parallel to obtain an average value.

2. EXPERIMENTAL SECTION 2.1. Reagents and Instruments. The chemical reagents used in the experiments are listed in Table 1. The deionized water was used to prepare and analyze samples. Table 1. Experimental Chemical Reagents reagents

purity

zinc chloride (ZnCl2)

≥98%

magnesium chloride hexahydrate (MgCl2·6H2O) lead chloride (PbCl2)

≥98% ≥99.5%

manufacturer Chengdu Kelong Chemical Reagent Manufactory, China Chengdu Kelong Chemical Reagent Manufactory, China Tianjin Kermel Chemical Reagent Manufactory, China

quality score

3. RESULTS AND DISCUSSION 3.1. The Ternary System ZnCl2−MgCl2−H2O at 323 K. After obtaining the equilibrium liquid phase of the samples and the wet solid phases, the results obtained by chemical analysis are listed in Table 2, and the phase diagram was plotted according to the experimental results, as is shown in Figure 1. As can be seen from Figure 1, the phase diagram of the ternary system ZnCl2−MgCl2−H2O contains two invariant points (E1 and E2), point E1 is saturated with MgCl2·6H2O and MgZnCl4·6H2O, which are identified by the X-ray diffraction photograph in Figure 2. The composition of the saturated solution at this point is w(MgCl2) = 30.23%, w(ZnCl2) = 24.86%.The other invariant point E2 is saturated with MgZnCl4·6H2O and ZnCl2, which are identified by the X-ray diffraction photograph in Figure 3. The composition of the saturated solution at this point is w(MgCl2) = 11.59%, w(ZnCl2) = 65.63%. It can be seen from the solubility curve A1E1 that the solubility of magnesium chloride gradually decreases with the addition of zinc chloride, and the solubility of ZnCl2 also decreases on the solubility curve B1E2, which can be attributed to the same ion effect of Cl−. The line E1E2 is the solubility curve of the double salt MgZnCl4·6H2O. The complex salt connecting lines can be obtained by connecting the point C with the point W1. The double salt connecting lines can pass through the corresponding solubility curve of the double salt. So the double salt is the same component double salt. There are three crystallization regions in this phase diagram, which correspond to the crystalline region of MgCl2·6H2O (AA1E1 region in Figure 1), the crystalline region of MgZnCl4·6H2O (CE1E2 region in Figure 1), and the crystalline region of ZnCl2

analytical purity analytical purity analytical purity

The samples were evaluated by the electronic balance (AL104, accuracy value 0.0001 g) that produced in the Mettler Toledo Instruments Co., Ltd. The deionized water was produced by the ultrapure water device (UPT-II-20T). The temperature was controlled by the water bath oscillator (HZSHA type, ±0.1 K) that was made by Harbin Donglian Electronic Technology Development Co., Ltd. The flame atomic absorption instrument (iCE3000) is produced by the Thermo Fisher Scientific (Germany). The solid-phases were identified by the X-ray diffractometer (DX-2700) made by Dandong Fangyuan Instrument Co., Ltd. 2.2. Experimental Method. The isothermal equilibrium method was used to study the phase equilibria of the two ternary systems, that is, the second salt was gradually added to the invariant points of the binary systems. The samples were prepared according to a certain ratio and placed in the reagent bottles (250 mL). Then they were placed into a constant temperature oscillating water bath. The temperature was set to be 323 K (±0.1 K). A certain amount of supernatant solution was taken out for chemical analysis every 2 days until the composition of the liquid phase was constant, that was, the dissolution equilibrium reached. B



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Table 2. Solubilities of the Ternary System ZnCl2−MgCl2− H2O at 323 K and 94.77 KPaa

no. 1,A1 2 3 4 5 6 7 8 9,E1 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24,E2 25 26 27 28 29 30,B1

composition of solution100·w(B)

composition of wet residue100·w(B)

w(ZnCl2) w(MgCl2)

w(ZnCl2) w(MgCl2)

0 2.86 5.52 9.49 14.57 17.13 19.31 24.28 24.86 30.30 33.06 35.83 37.84 39.51 41.88 47.52 50.52 52.15 52.86 55.10 57.13 61.72 63.88 65.63 70.58 74.35 76.22 78.33 81.00 82.57

37.25 36.01 35.21 33.72 32.17 31.39 30.83 30.04 30.23 27.00 25.30 23.82 22.79 21.77 20.55 18.25 16.83 16.37 16.22 15.04 14.47 13.33 12.48 11.59 8.44 6.41 5.40 3.38 1.78 0

5.20 8.49 9.34 9.89 13.22 25.85 35.79 37.12 38.37 39.16 39.96 41.39 43.35 45.69

40.73 40.15 38.98 38.87 39.51 31.91 27.87 26.56 26.23 25.58 25.15 24.46 23.82 23.07

48.21 49.92 51.43 52.75 61.52 65.48 85.28 91.79 91.21 90.79 96.70

21.74 20.49 19.46 19.69 14.98 14.35 4.88 2.57 2.23 1.87 0.78

equilibrium solids M M M M M M M M M+MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ MZ+Z Z Z Z Z Z Z

Figure 1. Phase diagram of the ternary system MgCl2−ZnCl2−H2O at 323 K.

Figure 2. Solid-phase XRD pattern of the ternary system MgCl2− ZnCl2−H2O at 323 K at the invariant point E1 (MgCl2·6H2O + MgZnCl4·6H2O).

a Note: M, MgCl2·6H2O; MZ, MgZnCl4·6H2O; Z, ZnCl2. w(B), mass fraction of component B in saturated solution. Standard uncertainties u are u(T) = 0.1 K, u(P) = 0.9 kPa. Relative standard uncertainties ur are ur(w(MgCl2)) = 0.005, and ur(w(ZnCl2)) = 0.003.

(BB1E2 region in Figure 1). It can be seen from the phase diagram that the three crystallization regions are not large, so the solubility of these substances is relatively large. The composition of the complex salt MgZnCl4·6H2O was determined by the wet slag method. To further identify the composition of MgZnCl4·6H2O, we selected the solid phases precipitated from the corresponding samples on the solubility curve E1E2 for X-ray diffraction analysis, as was shown in Figure 4. It was found that the spectrum corresponded to the standard diffraction card of MgZnCl 4·6H 2O, and the diffraction angle was better, but the peak intensity was not very good, which may be due to the poor crystallinity of the crystal. The detailed reports on the preparation and structure identification of MgZnCl4·6H2O have been made.15 The phase diagram of the ternary system ZnCl2−MgCl2− H2O at 373 K16 has also been studied by our research group, and a comparison chart at 373 and 323 K was plotted as is shown in Figure 5. As can be seen from the comparison diagram, the solubility of each salt at 373 K is larger than that at 323 K. It must be pointed out that the line F1F2 is the solubility curve of MgZnCl4·5H2O, and the line E1E2 is the solubility curve of MgZnCl4·6H2O, and the solubility curve of

Figure 3. Solid-phase XRD pattern of the ternary system MgCl2− ZnCl2−H2O at 323 K at the invariant point E2 (MgZnCl4·6H2O + ZnCl2).

MgZnCl4·5H2O is obviously longer than that of MgZnCl4· 6H2O. The solubility relationship of the ternary system ZnCl2−MgCl2−H2O at 297 K was also determined,15 and there is also a larger crystallization zone of MgZnCl4·5H2O in the phase diagram, that is, the double salt obtained at 297 K is MgZnCl4·5H2O. The law of the number of crystal water in a double-salt at these three temperatures goes against the C



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Table 3. Solubilities of the Ternary System ZnCl2−PbCl2− H2O at 323 K and 94.77 KPaa composition of solution100·w(B)

Figure 4. XRD pattern of the double salt MgZnCl4·6H2O in ternary system MgCl2−ZnCl2−H2O at 323 K.

no.

w(ZnCl2)

w(PbCl2)

1, J1 2 3 4 5 6 7 8 9 10 11,I 12 13 14 15 16,K1

0 5.92 11.68 19.66 27.17 37.57 51.57 63.62 73.70 80.58 81.98 82.35 82.56 82.33 82.75 82.57

1.70 0.45 0.41 0.29 0.22 0.19 0.11 0.13 0.42 1.28 1.41 1.34 0.69 0.39 0.16 0.00

composition of wet residue100·w(B) w(ZnCl2)

w(PbCl2)

0.56 1.01 0.37 2.62 4.17

96.74 97.16 97.31 92.65 90.40

6.82 11.42

86.15 83.41

94.14 98.82 98.53 98.29 98.04

2.88 0.12 0.12 0.05 0.02

equilibrium solids PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2 PbCl2+ZnCl2 ZnCl2 ZnCl2 ZnCl2 ZnCl2 ZnCl2

a

Note: w(B), mass fraction of component B in saturated solution. Standard uncertainties u are u(T) = 0.1 K, u(P) = 0.9 kPa. Relative standard uncertainties ur are ur(w(PbCl2)) = 0.02, and ur(w(ZnCl2)) = 0.003.

Figure 5. Comparison diagram of the ternary system MgCl2−ZnCl2− H2O at 323 and 373 K16

conclusion that the higher the temperature is, the lower the number of crystal water is. 3.2. The Ternary System ZnCl2−PbCl2−H2O at 323 K. The experimental data of the ternary system ZnCl2−PbCl2− H2O are listed in Table 3, the phase diagram (Figure 6) and the partial enlargement of the phase diagram (Figure 7) are obtained according to the experimental results. It can be seen from the figures that there is one invariant point I in this phase diagram, no hydrate, double salt, or solid solution is formed. The composition of each salt at the invariant point is w(ZnCl2) = 81.98%, w(PbCl2) = 1.41%. The chemical analysis results of the wet solid phases and the XRD patterns (Figure 8) indicate that the equilibrium solid phases corresponding to the invariant point are PbCl2 and ZnCl2. The system is a simple cosaturated type. There are two crystalline fields in the phase diagram, namely, the crystalline zone of zinc chloride and the crystalline zone of lead chloride. The most prominent feature of the whole phase diagram is that the crystallization zone of PbCl2 occupies most of the phase diagram, while the crystallization zone of zinc chloride is very small, indicating that the solubility of ZnCl2 is much larger than that of PbCl2, and PbCl2 is easier to be separated in solution. From the diagram combined with the data in Table 3, we can see that with the increase of the content of ZnCl2 in

Figure 6. Phase diagram of the ternary system ZnCl2−PbCl2−H2O at 323 K.

solution, the content of PbCl2 obviously decreases first and then increases. The reason for the decrease in solubility of lead chloride can be attributed to the same ion effect of chloride ions. With the increase of the content of zinc chloride, the activity of chloride ion increases and lead chloride can gradually form PbCln2‑n (n = 1−4),17 which makes the solubility increase. The ternary system ZnCl2−PbCl2−H2O at 298 K18 and 373 K19 have also been studied. At these three temperatures, the solubilities of the salts in the phase diagram are basically the same, and there is no formation of double salts, hydrates, or solid solutions. The liquid phase composition of the invariant D



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to the crystallization of lead chloride after leaching lead−zinc ore. The mother liquor after precipitation of lead chloride can be evaporated to precipitate zinc chloride.

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AUTHOR INFORMATION

Corresponding Author

*Tel.: 13032845233. E-mail: [email protected], [email protected]. ORCID

Shi-Hua Sang: 0000-0002-5948-3882 Funding

This project was supported by the National Natural Science Foundation of China (41873071,) and the National Natural Science Foundation of China-Qaidam Saline Lake Chemical Engineering Science Research Joint Fund of Qinghai Provincial People’s Government (U1407108). Notes

The authors declare no competing financial interest.

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Figure 7. Local enlarged phase diagram of ternary system ZnCl2− PbCl2−H2O at 323 K.

REFERENCES

(1) Deng, T.; Yu, X.; Li, D. Metastable Phase Equilibrium in the Aqueous Ternary System K2SO4 + MgSO4 + H2O at (288.15 and 308.15) K. J. Solution Chem. 2009, 38 (1), 27−34. (2) Deng, T.; Yu, X.; Sun, B. Metastable Phase Equilibrium in the Aqueous Quaternary System (Li2SO4 + K2SO4 + MgSO4 + H2O) at 288.15 K. J. Chem. Eng. Data 2008, 53 (11), 2496−2500. (3) Wang, H.; Gao, S. Y.; Zhang, H. Y.; Ren, Y. W.; Ran, X. Q. Study on Phase Diagram of KCl− ZnCl2−HCl(∼10.61%)-H2O System at 25°C and its Solid-Phase Compounds (in Chinese). Chinese Journal of Inorganic Chemistry. 2002, 18 (9), 945−948. (4) Radivojević, M.; Rehren, T.; Pernicka, E.; Sljivar, D.; Brauns, M.; Boric, D. On the origins of extractive metallurgy: new evidence from Europe. Journal of Archaeological Science. 2010, 37 (1), 2775−2787. (5) Paramguru, R. K.; Kammel, R. Bed performance in the direct electrowinning of lead from suspension galena anodes. Metall. Trans. B 1988, 19 (1), 67−72. (6) Paramguru, R. K.; Küzeci, E.; Kammel, R. Direct electrowinning of lead from suspension galena concentrate anode in different electrolytes. Metall. Trans. B 1988, 19 (1), 59−65. (7) Sinadinović, D.; Kamberović, Ž .; Š utić, A. Leaching kinetics of lead from lead (II) sulphate in aqueous calcium chloride and magnesium chloride solutions. Hydrometallurgy 1997, 47 (1), 137− 147. (8) Aydoğan, S.; Aras, A.; Uçar, G.; Erdemoğlu, M. Dissolution kinetics of galena in acetic acid solutions with hydrogen peroxide. Hydrometallurgy 2007, 89 (3), 189−195. (9) Zárate-Gutiérrez, R.; Lapidus, G. T.; Morales, R. D. Pressure leaching of a lead−zinc−silver concentrate with nitric acid at moderate temperatures between 130 and 170°C. Hydrometallurgy 2010, 104 (1), 8−13. (10) Zhang, X. P.; Wen, X. H.; He, X. F.; Sang, S. H. Measurement of Mineral Solubilities in the Ternary Systems CaCl2−ZnCl2−H2O and KCl−ZnCl2−H2O at 373 K. J. Solution Chem. 2016, 45 (10), 1504−1515. (11) Belova, E. V.; Mamontov, M. N.; Uspenskaya, I. A. A sodium chloride−zinc chloride−water system: solubility of solids and density of liquid in wide range of temperatures. J. Chem. Eng. Data 2016, 61 (7), 2426−2432. (12) Hudgins, C. M. Solubility and Density Studies of the CaCl2− ZnCl2−H2O System at 0 and 25°C. J. Chem. Eng. Data 1964, 9 (3), 434−436. (13) Helvenston, E. P.; Cuevas, E. A. Study of the System CaCl2− ZnCl2−H2O (NaCl Saturated) at 15°C. J. Chem. Eng. Data 1964, 9 (3), 321−323.

Figure 8. Solid-phase XRD pattern of the ternary system ZnCl2− PbCl2−H2O at 323 K at the invariant point I (ZnCl2 + PbCl2).

point at 298 K is w(PbCl2) = 2.58%, w(ZnCl2) = 76.74%, and that at 373 K is w(PbCl2) = 3.35%, w(ZnCl2) = 76.93%.

4. CONCLUSIONS The solubility data of two ternary systems ZnCl2−MgCl2− H2O and ZnCl2−PbCl2−H2O at 323 K were measured by the isothermal dissolution equilibrium method, and the phase diagrams were plotted, respectively. The complex salt MgZnCl4·6H2O was formed in the ternary system ZnCl2− MgCl2−H2O, the phase diagram consists of two invariant points, three univariant curves, and three crystallization areas. A comparison of the double salt forms produced at 373 K, 323 K, and 297 K shows that the double salt produced at 323 K is MgZnCl4·6H2O, while that produced at 373 and 297 K is MgZnCl4·5H2O. It is found that the number of waters in crystalline hydrate is not an inverse correlation with temperature. The ternary system ZnCl2−PbCl2−H2O is a simple cosaturated system with one invariant point, two solubility curves, and two crystallizing regions, and the crystallization zone of lead chloride is much larger than that of zinc chloride. The two phase diagrams show that the large solubility of zinc chloride makes it difficult to crystallize from the solution, and the solubility of lead chloride will be further reduced in a certain concentration of zinc chloride, so we can give priority E



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(14) Kendall, J.; Sloan, C. H. THE SOLUBILITY OF SLIGHTLY SOLUBLE CHLORIDES IN CONCENTRATED CHLORIDE SOLUTIONS. J. Am. Chem. Soc. 1925, 47 (9), 2306−2317. (15) Duhlev, R.; Macicek, J. Structure of magnesium zinc tetrachloride hexahydrate MgZnCl4·6H2O. Acta Crystallogr., Sect. C: Cryst. Struct. Commun. 1991, 47 (8), 1573−1575. (16) Zhang, X. P.; Zhang, W. Y.; Wang, D.; Zhang, H.; Sang, S. H. Measurement of mineral solubilities in the ternary systems NaCl− ZnCl2−H2O and MgCl2−ZnCl2−H2O at 373 K. Russ. J. Inorg. Chem. 2017, 62 (7), 995−1002. (17) Holdich, R. G.; Lawson, G. J. The solubility of aqueous lead chloride solutions. Hydrometallurgy 1987, 19 (2), 199−208. (18) Hagemann, S. Thermodynamische Eigenschaften des Bleis in Lö sungen der Ozeanischen Salze. Ph.D. Thesis, Braunschweig, Germany. 1999. (19) Zhang, X. P.; Cui, R. Z.; Liu, Q.; Sang, S. H. Phase equilibria in ternary systemsPbCl2−ZnCl2−H2O and CaCl2−PbCl2−H2O at 373 K (in Chinese). J. Chem. Ind. Eng. (China). 2016, 67 (11), 4552− 4557.

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