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Minerals 2019, 9, 766 15 of 21 phyllosilicate-bearing strata. Other possible Li sources could be relictic metamorphic brines and organic compounds, which support enrichment of Li. To improve the understanding of the Li origin in saline brines in an evaporitic environment, leaching experiments using a Li-bearing phyllosilicate were performed. Instead of muscovite and chlorite, which are typical phyllosilicates of the silicate-bearing strata, the more Li-containing lepidolite was used as an analogue material. Lepidolite with a Li content of 2.42 wt. % was exposed to 18 solutions of different composition (17 saline solutions and double distilled H2O) for three years. The most intensive leaching effect (53.36 μg Li/g in the brine) was observed on the interaction with a 0.03 molal MgCl2 solution and the second most by a modern seawater interaction (50.59 μgLi/gbrine), followed by low concentrated KCl solutions (0.1 to 0.60 molal KCl). The experiments show that Li was leached from the lepidolite, dependent on duration of the interaction reaction, the composition and pH value of the brines. Independent of these basic conditions, in all interaction solutions, with the exception of double distilled H2O, lepidolite was leached, resulting in minimal contents of ca. 40 μgLi/gbrine. The experiments show that the reaction progress was not finished after three years. Additional elements were leached (e.g., Si, Rb and Cs), and composition-dependent, pH changes were detected as well. The results from the experiments, regarding principal rock–water interaction processes, are basically transferable to the natural occurrences of phyllosilicate-bearing strata of the Gorleben and Morsleben salt deposits, but do not provide resilient proof for the origin of the Li in the investigated brines. Li-bearing phyllosilicates like muscovite and chlorites are typical in the rock types [28] and are comparable to lepidolite, which certainly shows a higher Li concentration. The Mg-containing solutions are the most effective for Li leaching by trend, which was observed in the experiments as well as in the natural brines. These Mg- and Li-enriched natural brines occurred mainly in phyllosilicate-bearing strata and anhydrite rocks or migrated through them. The experiments lasted three years at a temperature of 22–25 ◦C, and it can be assumed that in geological times, much more Li might be leached due to much more reaction time and higher temperatures (maximum 150 ◦C, [38]). The maximum depth of the salt deposit of Gorleben and Morsleben, regarding the Zechstein basis, was 3500 m to 4000 m. The present lithostatic pressure in Gorleben is 17.6–19.3 MPa at the mining level, and the rock temperature is 30–38 ◦C [53]. Further investigations will be extended to Li-bearing phyllosilicates that are typical for the phyllosilicate-bearing strata, e.g., muscovite and chlorite. To estimate the source of Li in the brines of the salt deposits and to study brine–rock interaction processes, stable isotopic investigations will be performed. The δ7Li of seawater is ca. +31% and considerably higher compared to most other rock types [58]. Therefore, it should be possible to distinguish the marine origin of the brine, e.g., relictic Permian pore solutions, or freshwater. Further, the interaction between brine and allochthones-originated phyllosilicates could be determined. Author Contributions: The general conceptualization for this research was by M.S. and M.M. M.S. and M.M. did the writing and figure preparation. Calculations and thermodynamic modelling were performed by M.S. Microscopy and SEM were carried out by M.M. and M.S. The experiments, accompanied sampling, including preparation, density and electrical conductivity measurements, were performed by M.S. and M.M. XRD, XRF, ICP-OES and ICP-MS analyses were realised by BGR Labs and MAS Analytics. Funding: This research was funded by the Federal Ministry for Economic Affairs and Energy (BMWi), Germany, grant 9Y3215020000. Acknowledgments: Many thanks to the very helpful comments and considerations of three anonymous reviewers, the editor and Linda Godfrey, who significantly helped to improve the quality of the present paper. Special thanks to our BGR colleagues Maik Gern and Tobias Faust who prepared the lepidolite, and to our analytical team Anna Degtjarev, Marina Linnenschmidt, Ragna Bergmann, Juergen Rausch and Elke Wargenau. Additional special thanks to MAS Analytics (Jens Walter and Nicol Nolte) for the geochemical analyses of the lepidolites with ICP-OES and ICP-MS. Also, thanks to Lothar Fleckenstein, Joachim Kutowski, Hartmut Blanke and Mario Patzschke (all BGE) for the assistance in the Gorleben and Morsleben mines and providing the brine samples. Supervision and general support was from Jörg Hammer, until he passed away. Final English editing was by Alja Saßnowski.PDF Image | Lithium Occurrences in Brines from Two German Salt Deposits
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