水系锌离子电池金属锌负极的改性策略与作用机制研究进展

Research Advances in Modification Strategies and Mechanisms for the Metallic Zinc Anode in Aqueous Zinc-ion Batteries

摘要

水系锌离子电池采用环境友好、本质安全的水基电解液，契合大规模可持续能源存储的需求，近年来受到广泛关注，然而，其商业化应用仍然面临多重关键挑战. 其中，金属锌负极在充放电过程中易发生枝晶生长、析氢反应及腐蚀等一系列副反应，严重制约了电池的循环寿命和库仑效率. 针对上述问题，研究者围绕锌负极的性能优化提出了多种改性策略，主要集中在结构设计、界面修饰、电解液调控和功能化隔膜4个方面. 本文综合评述了近年来锌负极的最新研究进展: 在结构设计方面，重点总结了三维结构电极、合金电极和外延生长锌负极在提升比表面积和成核位点的作用机制；在界面修饰方面，探讨了碳基材料、金属有机框架和有机聚合物等功能材料对锌沉积/溶解行为的调控机制；在电解液改性方面，分析了锌盐结构优化、电解液添加剂开发与新型电解液设计对改善锌离子溶剂化结构及其输运行为的关键作用. 进一步地，结合静电屏蔽、吸附作用、去溶剂化效应、原位界面膜及晶面调控等作用机制，系统总结了水系锌离子电池金属锌负极性能优化的主要策略. 最后，拓展至隔膜功能化改性维度，重点阐述了功能化隔膜通过均化离子通量、构筑离子筛分通道及调控界面化学环境等机制对锌沉积行为的间接调控作用，并对未来高性能水系锌离子电池的研究方向进行了展望.

Abstract

Aqueous zinc-ion batteries utilize environmentally friendly and inherently safe water-based electrolytes, aligning with the demands of large-scale sustainable energy storage, and have garnered widespread attention in recent years. However, their commercialization still faces multiple critical challenges. Among them, the zinc metal anode is prone to a series of side reactions during charge and discharge processes, such as dendrite growth, hydrogen evolution reaction, and corrosion, which severely restrict the battery’s cycling life and Coulombic efficiency. To address these issues, researchers worldwide have proposed various modification strategies focused on optimizing the performance of zinc anodes, primarily in three aspects: structural design, interface modification, and electrolyte regulation. This review systematically summarizes recent advances in zinc anodes. In terms of structural design, it highlights the mechanisms of three-dimensional structured electrodes, alloy electrodes, and epitaxially grown zinc anodes in enhancing specific surface area and nucleation sites. Regarding interface modification, the regulatory mechanisms of functional materials such as carbon-based materials, metal-organic frameworks, and organic polymers on zinc deposition/stripping behavior are discussed. As for electrolyte modification, the critical role of zinc salt structural optimization, electrolyte additive development, and novel electrolyte design in improving the solvation structure and transport behavior of zinc ions is analyzed. Furthermore, by integrating mechanisms such as electrostatic shielding, adsorption effects, desolvation effects, in-situ interface films, and crystal plane regulation, this review systematically outlines the main strategies for optimizing the performance of zinc metal anodes in aqueous zinc-ion batteries. Finally, this discussion is further extended to the dimension of functional separator modification, with an emphasis on the indirect regulatory effects of functional separators on zinc deposition behavior through mechanisms such as homogenizing ion flux, constructing ion-sieving channels, and modulating the interfacial chemical environment. Finally, an outlook for future research directions toward high-performance aqueous zinc-ion batteries is provided.

关键词

水系锌离子电池 / 金属锌负极结构设计 / 界面修饰 / 电解液改性 / 隔膜

Key words

Aqueous zinc-ion battery / Design of zinc metal anode structure / Interface modification / Electrolyte modification / Separator

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基金资助

国家自然科学基金(52125202)

国家自然科学基金(52572104)

国家自然科学基金(52202100)

国家自然科学基金(U24A2065)

国家重点研发计划项目(2024YFB3815301)

江苏省重点研发项目(BK20243016)