Borohydride Ammoniate Solid Electrolyte Design for All-Solid-State Mg Batteries

Abstract

Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries. In this work, we develop an amorphous Mg borohydride ammoniate, Mg(BH₄)₂·2NH₃, as a solid Mg electrolyte that prepared by a NH₃ redistribution between 3D framework-γ-Mg(BH₄)₂ and Mg(BH₄)₂·6NH₃. Amorphous Mg(BH₄)₂·2NH₃ exhibits a high Mg-ion conductivity of 5 × 10^-4 S cm^-1 at 75 °C, which is attributed to the fast migration of abundant Mg vacancies according to the theoretical calculations. Moreover, amorphous Mg(BH₄)₂·2NH₃ shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases, which can prevent further side reactions without hindering the Mg-ion transfer. Based on the above superiorities, amorphous Mg(BH₄)₂·2NH₃ enables the stable cycling of all-solid-state Mg cells, as the critical current density reaches 3.2 mA cm^-2 for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^-1 with a coulombic efficiency of 91.7% (first cycle) for Mg||TiS₂ cells.

Keywords

all-solid-state Mg batteries / amorphization / Mg borohydride ammoniate / Mg vacancy migration / solid electrolyte

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2022 The Authors. Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.