Correlation between Electrolyte Chemistry and Solid Electrolyte Interphase for Reversible Ca Metal Anodes. - National Genomics Data Center (CNCB-NGDC)

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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

Author Information

Zhen Hou: Department of Applied Physics & Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China. ORCID
Rui Zhou: Department of Applied Physics & Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China.
Yunduo Yao: Department of Applied Physics & Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China.
Zhiwen Min: Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, China.
Ziheng Lu: Microsoft Research AI4Science, Beijing, 100080, China.
Ye Zhu: Department of Applied Physics & Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China.
Jean-Marie Tarascon: Chimie du Solide-Energie, UMR 8260, Collège de France, Paris, France.
Biao Zhang: Department of Applied Physics & Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China. ORCID

PMID: 36259391 DOI: 10.1002/anie.202214796

The development of rechargeable Ca metal batteries (RCMBs) is hindered by the Ca 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/CaF -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.

Ca Deposition/Stripping Electrolyte Formulation Solid Electrolyte Interphase Solvation Structure

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Project No. 15306422; C5029-18E/Hong Kong Research Grants Council
ZE2F/Hong Kong Polytechnic University

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