Realizing Wide-Temperature Reversible Ca Metal Anodes through a Ca2+-Conducting Artificial Layer

Zhen Hou; Rui Zhou; Zhiwen Min; Ziheng Lu; Biao Zhang

doi:10.1021/acsenergylett.2c02366

Realizing Wide-Temperature Reversible Ca Metal Anodes through a Ca²⁺-Conducting Artificial Layer

Zhen Hou, Rui Zhou, Zhiwen Min, Ziheng Lu, Biao Zhang

Research output: Journal article publication › Journal article › Academic research › peer-review

12 Citations (Scopus)

Abstract

Room-temperature Ca deposition/stripping is impeded by the formation of ionic insulating interfaces. Electrolyte optimization could partially enhance Ca reversibility by tailoring the interfaces, but the precise regulation of the composition remains challenging. Herein, we construct an ex situ artificial layer on Ca metal via a facile displacement reaction between metal halides and Ca. These Ca-driven spontaneous layers with precisely controlled interfacial chemistry consist of a Ca metal alloy phase and a calcium halide matrix for conducting Ca²⁺ and insulating the electrons, as revealed by theoretical and experimental investigations. In particular, the Ca₃₁Sn₂₀/CaBr₂ interface enables Ca metal anodes to achieve low polarization and humid air stability over a wide temperature range from −25 to +50 °C. This proof-of-concept work provides an alternative approach to boost Ca²⁺ diffusivity through customized interfacial chemistry regulation.

Original language	English
Pages (from-to)	274-279
Number of pages	6
Journal	ACS Energy Letters
Volume	8
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.2c02366
Publication status	Published - 30 Nov 2022

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

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10.1021/acsenergylett.2c02366

http://hdl.handle.net/10397/98940

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title = "Realizing Wide-Temperature Reversible Ca Metal Anodes through a Ca2+-Conducting Artificial Layer",

abstract = "Room-temperature Ca deposition/stripping is impeded by the formation of ionic insulating interfaces. Electrolyte optimization could partially enhance Ca reversibility by tailoring the interfaces, but the precise regulation of the composition remains challenging. Herein, we construct an ex situ artificial layer on Ca metal via a facile displacement reaction between metal halides and Ca. These Ca-driven spontaneous layers with precisely controlled interfacial chemistry consist of a Ca metal alloy phase and a calcium halide matrix for conducting Ca2+ and insulating the electrons, as revealed by theoretical and experimental investigations. In particular, the Ca31Sn20/CaBr2 interface enables Ca metal anodes to achieve low polarization and humid air stability over a wide temperature range from −25 to +50 °C. This proof-of-concept work provides an alternative approach to boost Ca2+ diffusivity through customized interfacial chemistry regulation.",

author = "Zhen Hou and Rui Zhou and Zhiwen Min and Ziheng Lu and Biao Zhang",

note = "Funding Information: This work was supported by the General Research Fund (GRF) scheme of the Hong Kong Research Grants Council (Project No. 15306422). Z.L. thanks Bin Shao and Tie-Yan Liu from Microsoft Research for their help with computational resources. We are grateful to Prof. J. M. Tarascon for offering valuable comments on this work. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

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AU - Hou, Zhen

AU - Zhou, Rui

AU - Min, Zhiwen

AU - Lu, Ziheng

AU - Zhang, Biao

N1 - Funding Information: This work was supported by the General Research Fund (GRF) scheme of the Hong Kong Research Grants Council (Project No. 15306422). Z.L. thanks Bin Shao and Tie-Yan Liu from Microsoft Research for their help with computational resources. We are grateful to Prof. J. M. Tarascon for offering valuable comments on this work. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/11/30

Y1 - 2022/11/30

N2 - Room-temperature Ca deposition/stripping is impeded by the formation of ionic insulating interfaces. Electrolyte optimization could partially enhance Ca reversibility by tailoring the interfaces, but the precise regulation of the composition remains challenging. Herein, we construct an ex situ artificial layer on Ca metal via a facile displacement reaction between metal halides and Ca. These Ca-driven spontaneous layers with precisely controlled interfacial chemistry consist of a Ca metal alloy phase and a calcium halide matrix for conducting Ca2+ and insulating the electrons, as revealed by theoretical and experimental investigations. In particular, the Ca31Sn20/CaBr2 interface enables Ca metal anodes to achieve low polarization and humid air stability over a wide temperature range from −25 to +50 °C. This proof-of-concept work provides an alternative approach to boost Ca2+ diffusivity through customized interfacial chemistry regulation.

AB - Room-temperature Ca deposition/stripping is impeded by the formation of ionic insulating interfaces. Electrolyte optimization could partially enhance Ca reversibility by tailoring the interfaces, but the precise regulation of the composition remains challenging. Herein, we construct an ex situ artificial layer on Ca metal via a facile displacement reaction between metal halides and Ca. These Ca-driven spontaneous layers with precisely controlled interfacial chemistry consist of a Ca metal alloy phase and a calcium halide matrix for conducting Ca2+ and insulating the electrons, as revealed by theoretical and experimental investigations. In particular, the Ca31Sn20/CaBr2 interface enables Ca metal anodes to achieve low polarization and humid air stability over a wide temperature range from −25 to +50 °C. This proof-of-concept work provides an alternative approach to boost Ca2+ diffusivity through customized interfacial chemistry regulation.

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Realizing Wide-Temperature Reversible Ca Metal Anodes through a Ca²⁺-Conducting Artificial Layer

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