Adaptive Zincophilic-Hydrophobic Interfaces via Additive Engineering for Robust Zinc-Based Flow Batteries

作者：Shengnan Wang, Ninggui Ma, Pu Zhang, Hu Hong, Qing Li, Qingshun Nian, Yiqiao Wang, Zhuoxi Wu, Jiaxiong Zhu, Shixun Wang, Jun Fan, Chunyi Zhi · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c05027 · 被引用次数：42 · 研究领域：Advanced battery technologies research、Supercapacitor Materials and Fabrication、Solar-Powered Water Purification Methods

Zinc-based flow batteries (Zn-FBs) have emerged as promising candidates for large-scale energy storage (ES) systems due to their inherent safety and high energy density. However, dendrite formation and water-induced parasitic reactions at the Zn anode critically compromise long-term operational stability. While aqueous Zn battery additives have been extensively explored, systematic selection criteria for high-areal-capacity Zn-FBs remain absent. Here, we establish zincophilicity and interfacial hydrophobicity as dual descriptors for additive screening. A dimensionless parameter η, defined as the ratio of the adsorption energy on Zn to the binding energy of free water molecules, identifies 1-ethylpyridinium bromide (EPD) as the most optimal pyridinium additive with the highest η value. Mechanistic studies reveal that EPD spontaneously assembles into a dynamic electric-field-responsive interface, which self-adapts to morphological perturbations during electrodeposition and guides Zn 2+ flux along equipotential contours, preventing surface roughening. The in situ formed zincophilic-hydrophobic interphase alters interfacial chemistry by displacing reactive water molecules, achieving dual suppression of hydrogen evolution and dendrite propagation. Implementation of this strategy in Zn–Br 2 flow batteries enables ultrastable cycling over 4000 cycles (166 days) at 40 mA cm –2, delivering a cumulative plating capacity of 80 Ah cm –2 ─about 11.4-fold improvement over the baseline syst...