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Minerals 2019, 9, 766 9 of 21 Minerals 2019, 9, x FOR PEER REVIEW 10 of 22 Figure 5. SEM photographs of altered lepidolite. (a) Overview of lepidolite. (b) Lepidolite aggregate. Figure 5. SEM photographs of altered lepidolite. (a) Overview of lepidolite. (b) Lepidolite aggregate. (c) Very fine-grained lepidolite cement between imbricated lepidolite crystals. (c) Very fine-grained lepidolite cement between imbricated lepidolite crystals. 3.2.2. Solutions—Starting Solutions and Reaction Solutions after One and Three Years 3.2.2. Solutions—Starting Solutions and Reaction Solutions after One and Three Years Table 1 shows the density, the pH and the composition of the starting solutions (upper part of Table 1 shows the density, the pH and the composition of the starting solutions (upper part of Table 1) and the reaction solutions (one year of reaction; middle part of Table 1 and three years of Table 1) arenadctitohne; broetatocmtiopnartsoflTuatbiolen1s).(one year of reaction; middle part of Table 1 and three years of The reactant (lepidolite) as well as the interacting solutions were analysed after one year, and reaction; bottom part of Table 1). again at the end of experiments after three years. During the first year, the electrical conductivity The reactant (lepidolite) as well as the interacting solutions were analysed after one year, and was measured every 24–26 days, in order to monitor the continuation of the reaction progress [44]. again at the end of experiments after three years. During the first year, the electrical conductivity was For the estimation of the reaction progress and the specimen distributions in the reacting measured every 24–26 days, in order to monitor the continuation of the reaction progress [44]. solutions, thermodynamic modelling using EQ3/6 was performed. For Si, Cs, Rb and Li, no For thermesotdimynaatmioincalodfatthaeofresatcitsifoyingpqrougalrietysshavnedbetheneismppelceimeenntedinsttrhibe uthteiormnosdinyntahmeicredactatibnagsesolutions, of EQ3/6 to date. Therefore, EQ3/6 modelling was performed only for Na, K, Ca, Mg, Cl and SO4 thermodynamic modelling using EQ3/6 was performed. For Si, Cs, Rb and Li, no thermodynamical data using the thermodynamic database hmw [43]. of satisfying quality have been implemented in the thermodynamic database of EQ3/6 to date. Therefore, All reaction solutions with the exception of double distilled H2O are low to very high saline EQ3/6 modelling was performed only for Na, K, Ca, Mg, Cl and SO4 using the thermodynamic database solutions. The degree of dissolved components, i.e., salinity, corresponds to the electrical hmw[43]c.onductivity: rising conductivity documents an increasing quantity of dissolved components representing an ongoing reaction progress. All reaction solutions with the exception of double distilled H2O are low to very high saline The measurements of the density show no significant differences between initial and reacting solutions. The degree of dissolved components, i.e., salinity, corresponds to the electrical conductivity: reaction progress. solutions. rising conductivity documents an increasing quantity of dissolved components representing an ongoing The geochemical analyses document changes in the pH values and the composition/concentration of the resulting solutions due to interaction reactions between solutions Theanmdelaespuidroelmiteesn(Ftsiguorfe 6t)h.eIndaellncsaisteys,stheowsoluntionsisghnoiwficeannritchmdieffnetsreonfcLeis, Sbi,eRtwbeaennd Cins,itial and independent from their initial geochemical composition. K is leached only by double distilled H2O, reacting solutions. NaCl and low concentration MgCl2 solution. The geochemical analyses document changes in the pH values and the composition/concentration The pH values of the investigated experimental saline solutions changed in comparison to the of the resulting solutions due to interaction reactions between solutions and lepidolites (Figure 6). In all initial pH of the solutions. After three years, the pH of the reaction solutions varied between 3.3 and cases,the8.s5o,lduetpioendsinsghowntheenrkiicnhdmofensotlsuotiofnLia,nSdi,reRabctiaondtimCse,(iTnadblep1e,nFdigeunrtef6r)o.mThethmeoirstinsigtniaiflicgaenotchemical change in the pH was observed for the KCl solutions: from the initial 5.5 to 5.8 to a pH in the reaction composition. K is leached only by double distilled H2O, NaCl and low concentration MgCl2 solution. solutions of 7.5 to 8.1 after one year and a pH of 6.8 to 7.5 after three years. The initial pH of the 0.42 The pH values of the investigated experimental saline solutions changed in comparison to the molal NaCl solution shifts from 5.6 to a pH of 7.9 in the reaction solution (after one year) and to a pH initial pH of the solutions. After three years, the pH of the reaction solutions varied between 3.3 and of 7.4 (after three years). The pH of the 0.03 molal MgCl2 solution increased from 5.7 to a pH value of 8.5, depending on the kind of solution and reaction time (Table 1, Figure 6). The most significant 7.2 in the reaction solution (after one year) and 6.8 after three years. Remarkable is the little decrease change ininththeepH wvaaluseoobfstehrevsedsoflourtiothnserKeaCctlinsgolaufteironons:e fyreoamr inthceominpiatriaislo5n.5totothe5.s8oltuotiaonpsHreainctitnhge reaction after three years (Figure 6). solutions of 7.5 to 8.1 after one year and a pH of 6.8 to 7.5 after three years. The initial pH of the 0.42 After a one-year duration of the experiments, the maximum enrichment with a content of 45 molal NaCl solution shifts from 5.6 to a pH of 7.9 in the reaction solution (after one year) and to a pH μg/g of Li was detected in the 5.74 molal NaCl solution (sample 4–22). After three years, the highest of 7.4 (after three years). The pH of the 0.03 molal MgCl2 solution increased from 5.7 to a pH value of Li concentration with 53 μg/g was shown by the solution with the lowest MgCl2 concentration of 7.2 in the reaction solution (after one year) and 6.8 after three years. Remarkable is the little decrease in 0.03 mol/kg H2O (sample 11–47). The maximum of reaction progress between one and three years of reaction was also observed in the MgCl2 solution with the lowest concentration, the second most the pH value of these solutions reacting after one year in comparison to the solutions reacting after reaction progress was detected in the modern seawater interaction solution (samples 15–33–51), three years (Figure 6). followed by lower concentrated K solutions (samples 5–23–41, 6–24–42). The results, especially After a one-year duration of the experiments, the maximum enrichment with a content of 45 μg/g related to the massive reaction increase between one and three years, suggest that the interaction of Li was detected in the 5.74 molal NaCl solution (sample 4–22). After three years, the highest Li reactions between lepidolite and these solutions are not finished after three years (Figure 6). concentration with 53 μg/g was shown by the solution with the lowest MgCl2 concentration of 0.03 mol/kg H2O (sample 11–47). The maximum of reaction progress between one and three years of reaction was also observed in the MgCl2 solution with the lowest concentration, the second most reaction progress was detected in the modern seawater interaction solution (samples 15–33–51), followed by lower concentrated K solutions (samples 5–23–41, 6–24–42). The results, especially related to the massive reaction increase between one and three years, suggest that the interaction reactions between lepidolite and these solutions are not finished after three years (Figure 6).PDF Image | Lithium Occurrences in Brines from Two German Salt Deposits
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