期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 50, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202214796
关键词
Ca Deposition; Stripping; Electrolyte Formulation; Solid Electrolyte Interphase; Solvation Structure
资金
- General Research Fund (GRF) scheme of the Hong Kong Research Grants Council [15306422]
- Hong Kong Polytechnic University [ZE2F]
- University Research Facility on Chemical and Environmental Analysis (UCEA) of PolyU
- Research Grants Council of Hong Kong [C5029-18E]
This research demonstrates the reversibility of Ca deposition/stripping in rechargeable Ca metal batteries under a strong cation-solvent interaction, resulting in organic-rich/CaF2-poor solid electrolyte interphases (SEIs). The optimized electrolyte enables the pairing of organic cathode with RCMBs.
The development of rechargeable Ca metal batteries (RCMBs) is hindered by the Ca2+ passivating solid electrolyte interphases (SEIs). The cation solvation structure dictated by electrolyte chemistry plays a critical role in the SEIs properties. While a relatively weak cation-solvent binding is preferred in Li metal anodes to promote anion-derived SEIs, we demonstrate an enhanced Ca deposition/stripping reversibility under a strong cation-solvent interaction, which is materialized in strongly-solvating solvent and highly-dissociated salt combinations. Such electrolyte formulations benefit the formation of solvent-occupied solvation structure and minimize the anion reduction, resulting in organic-rich/CaF2-poor SEIs for reversible Ca metal anodes. Furthermore, RCMBs paired with an organic cathode using the optimized electrolytes are demonstrated as a proof-of-concept. Our work reveals the paradigm shift in SEIs design for Ca metal anodes, opening up new opportunities for emerging RCMBs.
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