In Situ Cross-Linking and Interfacial Engineering via Multifunctional Diamine Additive for High-Temperature Magnesium Metal Batteries.

Chen, Mingao; Zhang, Shu; Ge, Xuesong; Yang, Zhilin; Sun, Gaohao; Du, Aobing; Zhao, Jingwen; Li, Shengting et al. · Adv Mater · 2025

basic_science · Level V

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Abstract

The electrolyte and its interfacial chemistry are crucial for the development of high-temperature magnesium metal batteries. Here, a robust in situ cross-linked gel polymer electrolyte (MgB@CGPE) and its derived Mg<sub>3</sub>N<sub>2</sub>-rich (Mg<sub>3</sub>N<sub>2</sub> and related Mg─N─H complexes) interphase are obtained by a multifunctional diamine additive. The Mg<sub>3</sub>N<sub>2</sub>-rich interphase exhibits low magnesium ion migration activation energy and can effectively inhibit the continuous decomposition of electrolyte at the interface under elevated temperatures. Moreover, the MgB@CGPE can enable reversible magnesium deposition and dissolution over a wide temperature range of 30-180 °C. The assembled Mo<sub>6</sub>S<sub>8</sub>//MgB@CGPE//Mg cells demonstrate stable cycling over 200 cycles at 150 °C with 80% capacity retention. Additionally, these cells also address crucial mechanical and thermal safety concerns, indicating their potential for use under extreme conditions. This work presents a universal and practical strategy for designing polymer electrolytes that operate at elevated temperatures.