水系锌离子电池具有成本低廉、绿色环保、锌负极高比容量等优势，是大规模电化学储能领域的有力竞争者。然而锌金属负极表面难以彻底解决的析氢反应、腐蚀和枝晶生长的共性问题严重缩短了锌离子电池的循环寿命。此外，设计灵活、载量可调的锌粉负极结构在提高锌利用率和电池能量密度上具有突出优势。然而锌粉负极因其巨大比表面积和锌粉体积变化，存在电接触失效、电极结构崩塌的固有问题，严重阻碍了水系锌离子电池的实际应用。基于此，本论文立足水系锌离子电池锌金属负极界面调控，从电解液优化抑制副反应和制备高稳定锌粉负极两部分以实现高性能水系锌离子电池。主要工作有：（1）通过正丁醇和丁二酸二异辛酯磺酸钠（AOT）的协同作用，构建了反胶束结构“油包水”（W/O）电解液。反胶束外的正丁醇破坏了水分子间的氢键相互作用，降低水活度，抑制析氢反应。AOT组成的反胶束在电场下表现出定向移动和可逆的破乳行为，从而实现了快速的脱溶剂化动力学，并实现了锌金属负极的长期循环稳定性。W/O电解液使锌金属负极在1 mA cm?2与1 mAh cm?2条件下稳定循环5500 h。本研究中反向胶束结构的概念为研究锌金属电池中的电解液/锌金属负极界面调控提供了新的思路。（2）对锌粉制备工艺进行优化，确定材料配比，将聚丙烯腈（PAN）、聚丙烯酸（PAA）和丙三醇在干燥极片过程中原位酯化交联，形成高稳定锌粉负极。物理、化学双交联网络有效增强了粘结剂的力学性能，在循环中保持优异的极片完整性。双交联聚合物网络富含的氰基、酯基、羧基等极性基团与Zn2+存在较强的电荷相互作用，在均匀离子流的同时构建起高效的Zn2+传输网络，改变了Zn2+的沉积模式，实现致密锌沉积，有效提高了锌粉负极循环寿命。
Aqueous zinc-ion batteries (AZIBs) are strong contenders for large-scale electrochemical energy storage due to their low cost, eco-friendliness, and high specific capacity of zinc anodes. However, persistent issues on zinc metal anode surfaces, such as hydrogen evolution, corrosion, and dendrite growth, severely shorten battery cycle life. Moreover, while zinc powder anodes offer design flexibility and adjustable loading to improve zinc utilization and energy density, their large specific surface area and volume changes often lead to electrical contact failure and electrode collapse, hindering practical applications. In view of these challenges, this thesis focuses on interfacial control of zinc metal anodes in AZIBs by optimizing electrolytes to suppress side reactions and developing highly stable zinc powder anodes to achieve high-performance systems. The main contributions of this work are as follows:(1) Construction of Reverse Micelle-Based “Water-in-Oil” (W/O) Electrolyte: A reverse micelle electrolyte was developed through the synergistic effect of n-butanol and sodium bis(2-ethylhexyl) sulfosuccinate (AOT). The n-butanol in the reverse micelle disrupted hydrogen bonding between water molecules, reducing water activity and suppressing hydrogen evolution. Under an applied electric field, the reverse micelles exhibited directional motion and reversible demulsification behavior, enabling rapid desolvation kinetics and achieving long-term cycling stability for zinc metal anodes. The W/O electrolyte enabled the zinc metal anode to achieve stable cycling for 5500 h under conditions of 1 mA cm?2 and 1 mAh cm?2. The reverse micelle concept proposed in this study provides a novel approach for regulating electrolytes and zinc metal anodes in AZIBs.(2) Development of Zinc Powder-Based Anodes with Enhanced Electrode Integrity: The zinc powder fabrication process was optimized by determining the appropriate material ratios and enabling in situ esterification and crosslinking of polyacrylonitrile (PAN), polyacrylic acid (PAA), and glycerol during the electrode drying process, resulting in a highly stable zinc powder anode. The dual crosslinked polymer network, combining physical and chemical crosslinking, significantly enhances the mechanical properties of the binder and maintains excellent electrode integrity during cycling. Moreover, the network, rich in polar functional groups such as cyano, ester, and carboxyl groups, interacts strongly with Zn2⁺, constructing an efficient ion transport pathway that ensures uniform ion flow. This modification alters the Zn2⁺ deposition behavior, promotes dense zinc deposition, and effectively improves the cycling lifespan of the zinc powder anode.
