文献类型：期刊文献

英文题名：Uncovering Dynamic Edge-Sites in Atomic Co-N-C Electrocatalyst for Selective Hydrogen Peroxide Production

作者：Hu, Jinwen[1];Shang, Wenzhe[1];Xin, Cuncun[1];Guo, Jingya[1];Cheng, Xusheng[1];Zhang, Songlin[1];Song, Suchan[1];Liu, Wei[1,3];Ju, Feng[2,3];Hou, Jungang[1];Shi, Yantao[1]

机构：[1]Dalian Univ Technol, Frontier Sci Ctr Smart Mat, Sch Chem Engn, Dept Chem,State Key Lab Fine Chem, Dalian 116024, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai, Peoples R China;[3]Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis, Utrecht, Netherlands

年份：2023

卷号：62

期号：27

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20232114126187);WOS:【SCI-EXPANDED(收录号:WOS:000991476800001)】；

基金：This work was supported by the National Natural Science Foundation of China (22002013 and 52272193), the Fundamental Research Funds for the Central Universities (DUT22LAB602, DUT20RC(3)021), Liao Ning Revitalization Talents Program (XLYC2008032). The authors would like to thank NSRL, BSRF, and SSRF for the synchrotron radiation beam time. The authors would like to thank the Instrumental Analysis Center of Dalian University of Technology.

语种：英文

外文关键词：Edge-Site; Oxygen Reduction; X-Ray Absorption Spectroscopy; In Situ

摘要：Understanding the nature of single-atom catalytic sites and identifying their spectroscopic fingerprints are essential prerequisites for the rational design of target catalysts. Here, we apply correlated in situ X-ray absorption and infrared spectroscopy to probe the edge-site-specific chemistry of Co-N-C electrocatalyst during the oxygen reduction reaction (ORR) operation. The unique edge-hosted architecture affords single-atom Co site remarkable structural flexibility with adapted dynamic oxo adsorption and valence state shuttling between Co(2-delta)+ and Co2+, in contrast to the rigid in-plane embedded Co-1-N-x counterpart. Theoretical calculations demonstrate that the synergistic interplay of in situ reconstructed Co-1-N-2-oxo with peripheral oxygen groups gives a rise to the near-optimal adsorption of *OOH intermediate and substantially increases the activation barrier for its dissociation, accounting for a robust acidic ORR activity and 2e(-) selectivity for H2O2 production.