文献类型：期刊文献

英文题名：Optimizing the Electronic Structure of IrO x Sub-2 nm Clusters via Tunable Metal Support Interaction for Acidic Oxygen Evolution Reaction

作者：Chu, Qiuyan[1];Niu, Yanpu[2];Tao, Haolan[1,2];Liu, Honglai[1,2];Li, Quan[3];Lian, Cheng[1,2];Li, Jingkun[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Shanghai Xiangfenghua Technol Co Ltd, Shanghai 200949, Peoples R China

年份：2025

卷号：15

期号：3

起止页码：1942

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20250417739436);WOS:【SCI-EXPANDED(收录号:WOS:001399649100001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (22102114).

语种：英文

外文关键词：electronic structure; metal-supportinteraction; oxygen evolution reaction; proton exchangemembranewater electrolysis; sub-2 nm cluster

摘要：Iridium-based electrocatalysts are the most promising candidates for the acidic oxygen evolution reaction (OER). Considering their high cost and scarcity, it is imperative to maximize atom utilization and enhance the intrinsic activity of iridium. In this work, IrO x sub-2 nm clusters are stabilized on TiO2 supports via metal support interaction (MSI) induced by vacancy defects in TiO2. The strength of MSI is readily tuned by the type of vacancies: oxygen vacancies in TiO2 (VO-TiO2) induce the adsorbed MSI with relatively weak strength, while titanium vacancies in TiO2 (VTi-TiO2) lead to the strong embedded MSI. The tunable MSI further modulates the electronic structure of IrO x sub-2 nm clusters. IrO x /VO-TiO2 with adsorbed MSI exhibits an optimized electronic structure with a downshifted d-band center of IrO x , resulting in a reduced binding energy with oxygen and a low energy barrier of the rate-determining step for OER. Consequently, IrO x /VO-TiO2 delivers an activity twice that of commercial IrO2 and a good stability for 120 h in a practical proton exchange membrane water electrolyzer. Our study provides a guideline for the rational design of acidic OER catalysts based on modulating the electronic structure of IrO x sub-2 nm clusters via tunable MSI.