文献类型：期刊文献

英文题名：Asymmetrically coordinated nickel-based catalysts for enhanced hydrogen evolution reaction

作者：Li, Shiyi[1];Wang, Keyu[1];Liang, Chen[1];Lei, Linfeng[1,2];Wang, Yixing[1,2];Zhuang, Linzhou[1];Xu, Zhi[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Suzhou Lab, Suzhou, Peoples R China

年份：2025

卷号：71

期号：5

外文期刊名：AICHE JOURNAL

收录：;EI(收录号：20250917952273);WOS:【SCI-EXPANDED(收录号:WOS:001419021200001)】；

基金：The authors gratefully acknowledge the research funding provided by National Key R&D Program of China (Grant No. 2021YFB3801301), National Natural Science Foundation of China (Grant Nos. 22378119, 22075076, and 22208092), and Shanghai Pilot Program for Basic Research (22TQ1400100-4).

语种：英文

外文关键词：asymmetric structure; d-band center; hydrogen adsorption; hydrogen evolution reaction

摘要：Developing non-noble metal hydrogen evolution reaction (HER) catalysts with high efficiency for water dissociation in alkaline environments is crucial for achieving cost-effective alkaline water electrolyzer. Surface engineering offers immense potential to design promising HER catalysts with enhanced performance, but it faces multiple challenges such as optimizing hydrogen adsorption energy. Herein, Ni-based hydroxide catalysts doped with heteroatoms are synthesized via electrodeposition, forming a Co-doped asymmetric S-Ni-F coordination structure, which requires the overpotential of only 20 mV to reach a current density of -10 mA cm-2, and remains stable for over 100 h at -0.5 A cm-2. DFT calculations reveal that sulfur and fluorine doping could effectively mitigate the energy associated with active hydrogen adsorption and facilitate water molecule dissociation. Furthermore, the electron coupling within the d-orbital of the Ni-O-Co structure further amplifies the catalytic efficacy. This asymmetric structure offering a pathway for designing high-efficiency and non-noble metal alkaline HER catalysts.