文献类型：期刊文献

英文题名：Dynamic Evolution and Reversibility of a Single Au25 Nanocluster for the Oxygen Reduction Reaction

作者：Sun, Zehui[1,2];Wang, Jia[3,4];Su, Lei[1,2];Gu, Zhihao[1,2];Wu, Xin-Ping[3,4];Chen, Wei[5];Ma, Wei[1,2]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Sch Chem,Joint Int Res Lab Precis Chem & Mol Engn, 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, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[5]Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Electroanalyt Chem, Changchun 130022, Peoples R China

年份：2024

卷号：146

期号：29

起止页码：20059

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20242916711352);WOS:【SCI-EXPANDED(收录号:WOS:001276301600001)】；

基金：This research was supported by the National Natural Science Foundation of China (22272052), the Major Research Project (92061108), the Shanghai Municipal Science and Technology Major Project (grant no. 2018SHZDZX03), and the Fundamental Research Funds for the Central Universities. W.M. is sponsored by the National Ten Thousand Talent Program for young top-notch talent.

语种：英文

外文关键词：Catalyst activity - Electrolytic reduction - Gold compounds - Ligands - Oxygen

摘要：Ultrasmall metallic nanoclusters (NCs) protected by surface ligands represent the most promising catalytic materials; yet understanding the structure and catalytic activity of these NCs remains a challenge due to dynamic evolution of their active sites under reaction conditions. Herein, we employed a single-nanoparticle collision electrochemistry method for real-time monitoring of the dynamic electrocatalytic activity of a single fully ligand-protected Au-25(PPh3)(10)(SC2H4Ph)(5)Cl-2(2+) nanocluster (Au-25(2+) NC) at a cavity carbon nanoelectrode toward the oxygen reduction reaction (ORR). Our experimental results and computational simulations indicated that the reversible depassivation and passivation of ligands on the surface of the Au-25(2+) NC, combined with the dynamic conformation evolution of the Au-25(9+) core, led to a characteristic current signal that involves "ON-OFF" switches and "ON" fluctuations during the ORR process of a single Au-25(2+) NC. Our findings reinvent the new perception and comprehension of the structure-activity correlation of NCs at the atomic level.