Prioritizing Hetero-Metallic Interfaces via Thermodynamics Inertia and Kinetics Zincophilia Metrics for Tough Zn-based Aqueous Batteries.

Poor thermodynamic stability and sluggish electrochemical kinetics of metallic Zn anode in aqueous solution greatly hamper its practical application. To solve such problems, to date, various zincophilic surface modification strategies have been developed, which can facilitate reversible Zn plating/stripping behavior. However, there is still a lack of systematic and fundamental understanding regarding the metrics of thermodynamics inertia and kinetics zincophilia in selecting zincophilic sites. Herein, w e prioritize hetero-metallic interfaces for the first time via optimizing different hetero metals (Fe, Co, Ni, Sn, Bi, Cu, Zn, etc.) and synthetic solvents (ethanol, ethylene glycol, n-propanol, etc.). Specifically, both theoretical simulations and experimental results suggest that this Bi@Zn interface can exhibit high efficiency owing to the thermodynamics inertia and kinetics zincophilia. A best practice for prioritizing zincophilic sites in a more practical metric is also proposed. As a proof of concept, the Bi@Zn anode delivers ultralow overpotential of ca. 55 mV at a high rate of 10 mA cm -2 and stable cycle life over 4700 cycles. The elaborated "thermodynamics inertia and kinetics metalphilia" metrics for hetero-metallic interfaces could benchmark the success of other metal-based batteries. This article is protected by copyright. All rights reserved.