A Theory‐Driven Moderation Strategy for Electrolyte Design Unlocks Stable Aqueous Zinc Deposition

作者：Jingyi Wang, Hangsheng Yang, Yunpeng Zhong, Jianrui Feng, Zhe Cui, Ruwei Chen, Jie Chen, Fangjia Zhao, Jiajia Huang, Guanjie He · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202518262 · 被引用次数：11 · 研究领域：Advanced battery technologies research、Advanced Battery Materials and Technologies、Electrocatalysts for Energy Conversion

Abstract How theoretically screened solvation characteristics of additives affect zinc deposition behavior has emerged as a critical question of both scientific and practical relevance. Here, using a series of structurally analogous alcohol‐based molecules as a model system and guided by theoretical calculations, we establish a non‐extremum empirical model for additive screening to balance the relationship between additive theoretically properties and the solvation/interface stability in aqueous Zn‐ion battery electrolytes. Solvation capability, adsorption strength, and interfacial electrostatic properties were calculated to directly probe the critical role of a balanced set of molecular parameters in modulating Zn 2+ coordination structure and interface stability. As a result, 1,6‐hexanediol, exhibited a set of balanced and non‐extremum molecular parameters, significantly enhanced the reversibility of zinc deposition/stripping, delivered the best electrochemical performance that extending the cycling lifespan to 2 600 h, which is consistent with the Sabatier principle. This study provides a new theoretical perspective for the rational screen of electrolyte additives and highlights the importance of expanding the selection criteria for optimizing interfacial stability.