Customized Electronic Modulations of Transition Metal Chalcogenide Electrodes Via Heterointerfacing/High‐Valence Doping Toward High‐Performance Water Electrolysis with Ampere‐Level Current Density

作者：Xinyu Qin, Bingyi Yan, Tianyu Chen, Zhishun Teng, Deok Ki Cho, Andi Haryanto, Hyun Woo Lim, Chan Woo Lee, Yuanzhe Piao, Lin Xu, Jin Young Kim · 发表于：Advanced Functional Materials · 年份：2024 · DOI：10.1002/adfm.202405262 · 被引用次数：26 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Advanced battery technologies research

Abstract Electrochemical water splitting offers an advancing approach to producing highly pure hydrogen and oxygen, motivated by the prevalence of a low‐carbon economy and the goal of a sustainable future. The customized modulation of electronic structures enables the electrocatalyst to directionally promote hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which is a promising shortcut to overall water splitting (OWS). Herein, 3D homologous WSeS/CoSeS heterojunction nanoarrays (WSeS/CoSeS NAs) and W‐doped CoSeS nanoarrays (W‐CoSeS NAs) are investigated. Abundant heterointerfaces within WSeS/CoSeS NAs facilitate HER kinetics, boosting mass diffusivity, and increasing carrier separation and transfer process. High‐valence W 6+ doping into CoSeS prevents phase separation and stabilizes Co sites by charge offset effect, leading to enhanced OER. Consequently, the WSeS/CoSeS NAs and W‐CoSeS NAs reach 10 mA cm −2 at an overpotential of 43.8 and 233.3 mV in 1.0 m KOH electrolyte for HER and OER, respectively. Moreover, when asymmetrically engaged as an electrolyzer, this configuration exhibits extraordinary electrocatalytic performances (cell voltage of 1.51 V at 10 mA cm −2 ) with satisfying stability and mechanical robustness (over 1000 h at 1000 mA cm −2 ). The modulation and manufacture of reaction‐property‐oriented materials are experimentally and theoretically validated potential, illuminating the light of inspiration for multiple applications.