文献类型：期刊文献

英文题名：Enriched Oxygen Coverage Localized within Ir Atomic Grids for Enhanced Oxygen Evolution Electrocatalysis

作者：Lin, Hao Yang[1];Yang, Qian Qian[1];Lin, Miao Yu[1];Xu, Hao Guan[1];Tang, Xuan[2,3];Fu, Huai Qin[4];Wu, Haoran[5];Zhu, Minghui[5];Zhou, Lihui[2,3];Yuan, Hai Yang[1];Dai, Sheng[2,3];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Adv Mat, Sch Chem & Mol Engn, Inst Fine Chem, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[5]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China

年份：2024

卷号：36

期号：40

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20243416927151);WOS:【SCI-EXPANDED(收录号:WOS:001296158400001)】；

基金：H.Y.L. and Q.Q.Y. contributed equally to this work. This work was financially supported by the National Key Research and Development Program of China (No:2023YFA1507102), the National Natural Science Foundation of China (22239001, 51920105003, 22376062, and 22379043), the Shanghai Pilot Program for Basic Research (22TQ1400100-12), the Science and Technology Commission of Shanghai Municipality (23520710700, 21DZ1207101, 22ZR1415700, and 22ZR1416400), Shanghai Rising-star Program (20QA1402400), and the Fundamental Research Funds for the Central Universities. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry, the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF), and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses. The authors also thank the Jiaxing Puxiang Technology Co. Ltd. for the helpful test and discussion of in situ ATR-SEIRAS results.

语种：英文

外文关键词：Ir atomic grids; oxygen coverage; oxygen evolution reaction; reactive support

摘要：Inefficient active site utilization of oxygen evolution reaction (OER) catalysts have limited the energy efficiency of proton exchange membrane (PEM) water electrolysis. Here, an atomic grid structure is demonstrated composed of high-density Ir sites (approximate to 10 atoms per nm2) on reactive MnO2-x support which mediates oxygen coverage-enhanced OER process. Experimental characterizations verify the low-valent Mn species with decreased oxygen coordination in MnO2-x exert a pivotal impact in the enriched oxygen coverage on the surface during OER process, and the distributed Ir atomic grids, where highly electrophilic Ir & horbar;O(II-delta)- bonds proceed rapidly, render intense nucleophilic attack of oxygen radicals. Thereby, this metal-support cooperation achieves ultra-low overpotentials of 166 mV at 10 mA cm-2 and 283 mV at 500 mA cm-2, together with a striking mass activity which is 380 times higher than commercial IrO2 at 1.53 V. Moreover, its high OER performance also markedly surpasses the commercial Ir black catalyst in PEM electrolyzers with long-term stability. Atomic grid structure with high-density Ir sites (approximate to 10 atoms per nm2) on MnO2-x support realizes co-catalytic Ir-Mn interaction in water oxidation process, involving enriched oxygen coverage driven by Mn-Ov coordination defects to cooperate with highly electrophilic Ir-O(II-delta)- species, which facilitates intensive O-O radical direct coupling within the grids for performance enhancement. image