文献类型：期刊文献

英文题名：Understanding the Position Effects of Monoatom Doping in Silver Nanoclusters on Oxygen Reduction by Single Entity Electrochemistry

作者：Sun, Zehui[1,2];Chen, Cheng[3,4];Wei, Mengdan[1,2];Wang, Haifeng[3,4];Chen, Jianfu[3,4];Ma, Wei[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, Feringa Nobel PrizeScientist Joint Res Ctr,Frontie, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Joint Int Res Lab Precis Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2025

卷号：64

期号：27

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20251918398695);WOS:【SCI-EXPANDED(收录号:WOS:001483177900001)】；

基金：This research was supported by the National Natural Science Foundation of China (22272052 and 22473043), the Major Research Project (92061108), the National Key R&D Program of China (2021YFA1500700), and the Science and Technology Commission of Shanghai Municipality (24DX1400200). The authors thank the Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterization.

语种：英文

外文关键词：Alloy nanoclusters; Intracluster migration; Monoatom doping; Position effects; Single entity electrochemistry

摘要：Alloying nanoclusters (NCs) with monoatom doping represents an effective strategy to enhance catalytic performances due to the synergistic interactions between the dopant and host atoms. However, in-depth understanding the position effects of monoatom doping within alloying NCs, particularly at the atomic level, remains elusive. Here, we employed single entity collision electrochemistry method to investigate the electrocatalytic behaviors of individual monoatom-doped bimetallic M1Ag24 (M = Ag, Au, Pt, and Cu) NCs toward oxygen reduction reaction (ORR). By relying on high-resolution and high-throughput electrochemical measurements, we successfully discriminated the effects of monoatom variation in M1Ag24 NCs on ORR activity at the single atom resolution and identified different M1Ag24 NCs across characteristic populations. Our experimental findings and theoretical calculations reveal the electrocatalytic reaction dynamics associated with intracluster migration of Au monoatom during the dynamic alloying process of Au1Ag24 NCs. This work demonstrates a novel approach for in situ identifying the position effects of foreign doping atoms on the electrocatalytic activity of alloy NCs at the single atom level.