Chang Zhi, Yang Huijun, Qiao Yu, Zhu Xingyu, He Ping, Zhou Haoshen
Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Umezono, Tsukuba, 305-8568, Japan.
National Laboratory of Solid State Microstructures & Department of Energy Science and Engineering, Nanjing University, Nanjing, 210093, P. R. China.
Adv Mater. 2022 Aug;34(34):e2201339. doi: 10.1002/adma.202201339. Epub 2022 Jul 17.
Solvent molecules within the solvation sheath of cations (e.g., Li , Na , Zn ) are easily to be dehydrogenated especially when coupled with high-voltage cathodes, and lead to detrimental electrolytes decompositions which finally accelerate capacity decays of rechargeable batteries. Tremendous efforts are devoted to tackle with this long-lasting issue. Among them, salt-concentrated strategies are frequently employed to tailor the solvation sheath of cations and improve the stabilities of electrolytes. However, the cost challenges caused by adding extra dose of expensive salts, additives/cosolvents in preparing highly concentrated electrolytes, hinder their further utilizations to some extent. Introducing porous materials-based electrode front-faces on the surface of electrodes even within dilute electrolytes can transfer the high-energy-state desolvated solvents from the reactive electrodes to the nonconductive porous material surfaces, thus eliminate the contact chances between desolvated solvents and electrode materials, and greatly reduce solvents-related decomposition issues. Herein, recent advances in using electrode front-faces to tailor the solvation sheath of metal ions for rechargeable batteries are discussed. Finally, perspectives to the future challenges and opportunities of constructing electrode front-faces to tailor the solvation sheath of cations by constructing electrode front-face for rechargeable batteries are provided.
阳离子（如Li⁺、Na⁺、Zn²⁺）溶剂化鞘层内的溶剂分子很容易脱氢，特别是当与高压阴极耦合时，会导致有害的电解质分解，最终加速可充电电池的容量衰减。人们为解决这一长期存在的问题付出了巨大努力。其中，盐浓缩策略经常被用于调整阳离子的溶剂化鞘层并提高电解质的稳定性。然而，在制备高浓度电解质时添加额外剂量的昂贵盐、添加剂/共溶剂所带来的成本挑战，在一定程度上阻碍了它们的进一步应用。在电极表面引入基于多孔材料的电极前端，即使在稀电解质中，也可以将高能态的去溶剂化溶剂从活性电极转移到非导电的多孔材料表面，从而消除去溶剂化溶剂与电极材料之间的接触机会，并大大减少与溶剂相关的分解问题。在此，讨论了利用电极前端调整可充电电池金属离子溶剂化鞘层的最新进展。最后，展望了通过构建可充电电池的电极前端来调整阳离子溶剂化鞘层所面临的未来挑战和机遇。
