文献类型：期刊文献

英文题名：Promoted water dissociation via harnessing Ir oxidation-state boundary for robust hydrogen evolution catalysis

作者：Li, Shiyi[1];Duan, Ruidan[1];Wang, Keyu[1];Li, Jiankun[1];Lei, Linfeng[1,4];Wang, Yixing[1,4];Chen, Jun[5,6];Zhuang, Linzhou[1];Xu, Zhi[1];Yao, Xiangdong[2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Sun Yat Sen Univ, Sch Adv Energy, Shenzhen 518107, Peoples R China;[3]Sun Yat Sen Univ Shenzhen, IGCME, Shenzhen 518107, Peoples R China;[4]Suzhou Lab, Suzhou 215000, Peoples R China;[5]Univ Wollongong, Intelligent Polymer Res Inst, Inst Innovat Mat, Wollongong, NSW 2500, Australia;[6]Univ Wollongong, ARC Ctr Excellence Electromat Sci Australian Inst, Wollongong, NSW 2500, Australia

年份：2026

卷号：320

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20253619102758);WOS:【SCI-EXPANDED(收录号:WOS:001567962200001)】；

基金：The authors gratefully acknowledge the research funding provided by 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：Iridium nanoclusters; Oxidation state; Anodization; Water dissociation; Hydrogen evolution

摘要：Optimizing the electronic structure of active sites is critical for designing advanced hydrogen evolution reaction (HER) electrocatalysts, yet the precise role of the oxidation state remains debated. Here, we systematically tuned the oxidation state of iridium nanoclusters (similar to 2 nm) supported on a NiCoFe(OH)(x) substrate via a controlled anodization strategy. We establish a distinct volcano-type relationship between the Ir oxidation state and HER activity. The optimal catalyst, with a precisely tuned Ir average oxidation state of 1.34, delivers an exceptional HER current density of 507.7 mA cm(- 2) at a 100 mV overpotential and exhibits outstanding stability for over 250 h in both alkaline and seawater electrolysis. Mechanistic studies using in situ electrochemical impedance spectroscopy reveal that this enhancement originates from accelerated water dissociation and improved interfacial electron transfer. This work underscores that precisely tuning the noble metal oxidation state is a powerful strategy for designing highly active and robust electrocatalysts for energy conversion.