Hydrophobic Ion Barrier‐Enabled Ultradurable Zn (002) Plane Orientation towards Long‐Life Anode‐Less Zn Batteries

作者：Guigui Liu, Yongchao Tang, Yue Wei, Hongqing Li, Jianping Yan, Zhenfeng Feng, Wencheng Du, Qi Yang, Minghui Ye, Yufei Zhang, Zhipeng Wen, Xiaoqing Liu, Cheng Chao Li · 发表于：Angewandte Chemie International Edition · 年份：2024 · DOI：10.1002/anie.202407639 · 被引用次数：89 · 研究领域：Advanced battery technologies research、Advancements in Battery Materials、Advanced Battery Materials and Technologies

Abstract Gradual disability of Zn anode and high negative/positive electrode (N/P) ratio usually depreciate calendar life and energy density of aqueous Zn batteries (AZBs). Herein, within original Zn 2+ ‐free hydrated electrolytes, a steric hindrance/electric field shielding‐driven “hydrophobic ion barrier” is engineered towards ultradurable (002) plane‐exposed Zn stripping/plating to solve this issue. Guided by theoretical simulations, hydrophobic adiponitrile (ADN) is employed as a steric hindrance agent to ally with inert electric field shielding additive (Mn 2+ ) for plane adsorption priority manipulation, thereby constructing the “hydrophobic ion barrier”. This design robustly suppresses the (002) plane/dendrite growth, enabling ultradurable (002) plane‐exposed dendrite‐free Zn stripping/plating. Even being cycled in Zn‖Zn symmetric cell over 2150 h at 0.5 mA cm −2 , the efficacy remains well‐kept. Additionally, Zn‖Zn symmetric cells can be also stably cycled over 918 h at 1 mA cm −2 , verifying uncompromised Zn stripping/plating kinetics. As‐assembled anode‐less Zn‖VOPO 4 ⋅ 2H 2 O full cells with a low N/P ratio (2 : 1) show a high energy density of 75.2 Wh kg −1 full electrode after 842 cycles at 1 A g −1 , far surpassing counterparts with thick Zn anode and low cathode loading mass, featuring excellent practicality. This study opens a new avenue by robust “hydrophobic ion barrier” design to develop long‐life anode‐less Zn batteries.