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

Zhen Hou, Rui Zhou, Yunduo Yao, Zhiwen Min, Ziheng Lu, Ye Zhu, Jean Marie Tarascon, Biao Zhang

Research output: Journal article publicationJournal articleAcademic researchpeer-review

12 Citations (Scopus)

Abstract

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.

Original languageEnglish
Article numbere202214796
JournalAngewandte Chemie - International Edition
Volume61
Issue number50
DOIs
Publication statusPublished - 19 Oct 2022

Keywords

  • Ca Deposition/Stripping
  • Electrolyte Formulation
  • Solid Electrolyte Interphase
  • Solvation Structure

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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