文献类型：期刊文献

英文题名：Modulating Ru-O bond covalency via Ga-doping for enhanced oxygen evolution reaction in acid

作者：Liu, Zhongliang[1];Liu, Heng[3];Zhou, Kai[1];Liu, Miaomiao[4];Xue, Tianrui[1];Shen, Yongjun[1];Li, Hao[3];Li, Huihui[1];Li, Chunzhong[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China;[3]Tohoku Univ, Adv Inst Mat Res WPI AIMR, Sendai 9808577, Japan;[4]Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China

年份：2025

卷号：68

期号：11

起止页码：5606

外文期刊名：SCIENCE CHINA-CHEMISTRY

收录：;EI(收录号：20252218530548);WOS:【SCI-EXPANDED(收录号:WOS:001499183000001)】；

基金：This work was supported by the National Natural Science Foundation of China (U22B20143, U24A20546, 22478121), the Shanghai Municipal Science and Technology Major Project, the Science and Technology Commission of Shanghai Municipality (22dz1205900), the Fundamental Research Funds for the Central Universities (JKD01241702), the Japan Society for the Promotion of Science (JSPS) KAKENHI (JP23K13703, JP24K23069), and the Ensemble Grants for Early Career Researchers 2024, Strategic Priority Research Program of the Chinese Academy of Sciences (XDA 0400000). We acknowledge the Center for Computational Materials Science, Institute for Materials Research, Tohoku University for the use of MASAMUNE-IMR (202212-SCKXX-0204) and the Institute for Solid State Physics (ISSP) at the University of Tokyo for the use of their supercomputers. We thank the Shanghai Synchrotron Radiation Facility (SSRF) for supporting the XAS experiments at the BL14W1 beamline.

语种：英文

外文关键词：oxygen evolution reaction; metal-oxygen covalency; proton exchange membrane water electrolysis; water oxidation

摘要：The increasing demand for green hydrogen production requires the development of advanced ruthenium (Ru)-based oxide catalysts for the anodic oxygen evolution reaction (OER). Here, we report the development of a Ga-doped RuO2 catalyst (Ga-RuO2) that demonstrates enhanced OER performance attributed to modulated Ru-O bond covalency. The fully occupied 3d orbital of Ga stabilizes its oxidation state during OER, while its atomic radius, similar to Ru, helps maintain the initial crystal lattice structure upon doping. In-situ characterization, kinetic analysis and theoretical calculations reveal that the weakened Ru-O bond covalency lowers the energy barriers for *OH and *OOH formation, thus contributing to an enhanced OER performance. The resultant Ga-RuO2 achieves a current density of 10 mA cm-2 at a low overpotential of 203 mV and demonstrates durable operation for 500 h in acid. This work provides valuable insights into the electronic structure engineering of Ru-based catalysts for practical water electrolysis applications.