文献类型：期刊文献

英文题名：Inhibiting Overoxidation of Dynamically Evolved RuO2 to Achieve a Win-Win in Activity-Stability for Acidic Water Electrolysis

作者：Li, Wenjing[1];Chen, Dingming[2,3];Lou, Zhenxin[1];Yuan, Haiyang[1];Fu, Xiaopeng[1];Lin, Hao Yang[1];Lin, Miaoyu[1];Hou, Yu[1];Qi, Haifeng[4];Liu, Peng Fei[1];Yang, Hua Gui[1];Wang, Haifeng[2,3]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Ctr Computat Chem, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Cardiff Univ, Max Planck Cardiff Ctr Fundamentals Heterogeneous, Translat Res Hub, Cardiff CF24 4HQ, Wales

年份：2025

卷号：147

期号：12

起止页码：10446

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20251017987681);WOS:【SCI-EXPANDED(收录号:WOS:001435236000001)】；

基金：This project was supported by the National Key Research and Development Program of China (2021YFA1500700), National Natural Science Foundation of China (22239001, 51920105003, 22472053, 92045303, 51972111, 22202069, and 22379043), National Ten Thousand Talent Program for Young Top-notch Talent, Science and Technology Commission of Shanghai Municipality (23520710700, 23ZR1416800, and 22ZR1416400), "Dawn" Program of Shanghai Education Commission (22SG28), Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400), and Fundamental Research Funds for the Central Universities (JKD01231632).

语种：英文

外文关键词：Design for testability - Electric towers - Hydrogen evolution reaction - Oxygen evolution reaction - Solar buildings - Sustainable development

摘要：Proton exchange membrane (PEM) water electrolysis offers an efficient route to large-scale green hydrogen production, in which the RuO2 catalyst exhibits superior activity but limited stability. Unveiling the atomic-scale structural evolution during operando reaction conditions is critical but remains a grand challenge for enhancing the durability of the RuO2 catalyst in the acidic oxygen evolution reaction (a-OER). This study proposes an adaptive machine learning workflow to elucidate the potential-dependent state-to-state global evolution of the RuO2(110) surface within a complex composition and configuration space, revealing the correlation between structural patterns and stability. We identify the active state with distorted RuO5 units that self-evolve at low potential, which exhibits minor Ru dissolution and an activity self-promotion phenomenon. However, this state exhibits a low potential resistance capacity (PRC) and evolves into inert RuO4 units at elevated potential. To enhance PRC and mitigate the overevolution of the active state, we explore the metal doping engineering and uncover an inverse volcano-type doping rule: the doped metal-oxygen bond strength should significantly differ from the Ru-O bond. This rule provides a theoretical framework for designing stable RuO2-based catalysts and clarifies current discrepancies regarding the roles of different metals in stabilizing RuO2. Applying this rule, we predict and confirm experimentally that Na can effectively stabilize RuO2 in its active state. The synthesized Na-RuO2 operates in a-OER for over 1800 h without any degradation and enables long-term durability in PEM electrolysis. This work enhances our understanding of the operando structural evolution of RuO2 and aids in designing durable catalysts for a-OER.