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无机材料学报

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动态合金化界面调控对Mg(OTf)2基电解液性能的优化

薛晓兰1, 张元香1, 崔茂盛1, 王潇潇1, 母振1, 金钟2   

  1. 1.中国矿业大学 材料与物理学院,徐州 221116;
    2.南京大学 化学化工学院,绿色化学与工程研究院,配位化学全国重点实验室,绿色能源催化与智能化学工程省高校重点实验室,南京 210023
  • 收稿日期:2026-05-18 修回日期:2026-07-02
  • 通讯作者: 金 钟, 教授. E-mail: zhongjin@nju.edu.cn
  • 作者简介:薛晓兰(1991–), 女, 博士研究生, 讲师. E-mail: xuexiaolan@cumt.edu.cn
  • 基金资助:
    国家自然科学基金(U25A20628, 22561160129, 22479074, 22475096); 装备预研教育部联合基金(8091B02052407); 江苏省基础研究计划重点项目(BK20253008); 江苏省科技重大专项(BG2024013); 江苏省科技成果转化专项基金(BA2023037); 江苏省学位与研究生教育改革项目(JGKT24_C001); 苏州市关键核心技术开放竞争项目(SYG2024122); 中央高校基本科研业务费专项资金和南京大学国际合作计划项目(020514380354)

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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摘要： 镁金属电池因镁负极具有资源丰富、理论比容量高和氧化还原电位低等优势,是极具发展前景的新一代高安全储能体系。然而,传统电解液中镁负极易发生界面钝化,形成Mg2+绝缘层,严重限制了镁沉积/剥离可逆性及电池循环稳定性。针对上述问题,本研究提出一种基于动态合金化界面调控的电解液优化策略,在Mg(OTf)2(OTf：三氟甲磺酸)基电解液中引入Sn(OTf)2添加剂,在Mg负极表面原位构建Sn/Mg2Sn动态界面层,实现对Mg沉积/剥离行为的优化。研究表明,Sn2+与Mg负极发生置换反应,形成Sn与Mg2Sn共存的复合界面层,为Mg沉积提供丰富的亲镁位点,有效抑制界面副反应并优化界面反应动力学。得益于该动态界面层的持续再生作用,Mg//Mg对称电池在1.0 mA·cm-2和1.0 mAh·cm-2条件下,稳定循环超过1300 h后的过电位仅为~0.26 V。Mg//Cu不对称电池在0.2 mA·cm-2下可循环超过1350 h,平均库仑效率达98.38%,沉积过电位最低仅为0.097 V。此外,Mg//CuS全电池也表现出良好的倍率性能。本研究提出的动态合金化界面调控策略,为开发高性能镁电池提供了新思路。

关键词: 镁金属电池, 镁负极, 动态合金化, 界面调控

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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