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Journal of Inorganic Materials

Journal of Inorganic Materials

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Dynamic Alloying Interfacial Regulation for Realizing the Performance Optimization of Mg(OTf)2-based Electrolytes

XUE Xiaolan1, ZHANG Yuanxiang1, CUI Maosheng1, WANG Xiaoxiao1, MU Zhen1, JIN Zhong2   

  1. 1. School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, China;
    2. School of Chemistry and Chemical Engineering, Institute of Green Chemistry and Engineering, State Key Laboratory of Coordination Chemistry, Jiangsu Key Laboratory of Green Energy Catalysis and Intelligent Chemical Engineering, Nanjing University, Nanjing 210023, China
  • Received:2026-05-18 Revised:2026-07-02
  • Contact: JIN Zhong, professor. E-mail: zhongjin@nju.edu.cn
  • About author:XUE Xiao (1991–), female, PhD candidate, lecturer. E-mail: xuexiaolan@cumt.edu.cn
  • Supported by:
    National Natural Science Foundation of China (U25A20628, 22561160129, 22479074, 22475096); Equipment Pre-Research and Ministry of Education Joint Fund (8091B02052407); Fundamental Research Program Key Project of Jiangsu Province (BK20253008); Science and Technology Major Project of Jiangsu Province (BG2024013); Scientific and Technological Achievements Transformation Special Fund of Jiangsu Province (BA2023037); Academic Degree and Postgraduate Education Reforming Project of Jiangsu Province (JGKT24_C001), Key Core Technology Open Competition Project of Suzhou City (SYG2024122), Fundamental Research Funds for the Central Universities and Nanjing University International Collaboration Initiative (020514380354)

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Abstract: Magnesium metal batteries (MMBs) are considered promising next-generation high-safety energy storage systems owing to the abundant reserves, high theoretical volumetric capacity, and low redox potential of magnesium metal anodes. However, severe interfacial passivation of Mg anodes in conventional electrolytes readily leads to the formation of Mg2+-insulating layers, which greatly limits the reversibility of Mg plating/stripping and the cycling stability of MMBs. To address these issues, a dynamic alloying interfacial regulation strategy was proposed by introducing a Sn(OTf)2 (OTf: trifluoromethanesulfonate) additive into the conventional Mg(OTf)2-based electrolyte, enabling the in situ construction of a Mg2Sn/Sn dynamic alloy interfacial layer on the Mg anode surface to regulate Mg plating/stripping behaviors. The results demonstrate that Sn2+ cations can spontaneously react with the Mg substrate through a displacement reaction, forming a coexisting Sn/Mg2Sn alloy interfacial layer that provides abundant magnesiophilic active sites for Mg deposition, effectively suppresses interfacial side reactions, and improves interfacial reaction kinetics. Benefiting from the continuous regeneration of the dynamic interfacial layer, the Mg//Mg symmetric cell exhibits stable cycling for over 1300 h at 1.0 mA·cm-2 and 1.0 mAh·cm-2 with a low overpotential of ~0.26 V. Meanwhile, the Mg//Cu asymmetric cell achieves a cycling lifespan exceeding 1350 h at 0.2 mA·cm-2, delivering an average Coulombic efficiency of 98.38% and a low deposition overpotential of only ~0.097 V. Moreover, the Mg//CuS full battery exhibits a good rate capability. This work provides a new strategy for the development of high-performance MMBs through dynamic alloying interfacial regulation.

Key words: magnesium metal battery, magnesium anode, dynamic alloying, interfacial regulation

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