4.8 Article

Correlation between Electrolyte Chemistry and Solid Electrolyte Interphase for Reversible Ca Metal Anodes

期刊

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

  1. General Research Fund (GRF) scheme of the Hong Kong Research Grants Council [15306422]
  2. Hong Kong Polytechnic University [ZE2F]
  3. University Research Facility on Chemical and Environmental Analysis (UCEA) of PolyU
  4. Research Grants Council of Hong Kong [C5029-18E]

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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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