Size hierarchy of gold clusters in nanogold-catalyzed acetylene hydrochlorination

作     者：Yifei Zhang Xinrui Gu Fatimah Kehinde Busari Sami Barkaoui Zhong-Kang Han Alfons Baiker Zhen Zhao Gao Li 

作者机构：Institute of Catalysis for Energy and Environment College of Chemistry and Chemical Engineering Shenyang Normal University Shenyang 110034 China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China School of Materials Science and Engineering Zhejiang University Hangzhou 310000 China Department of Chemistry and Applied Biosciences ETH Hönggerberg HCI CH-8093 Zurich Switzerland University of Chinese Academy of Sciences Beijing 100049 China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2024年第17卷第11期

页      面：9594-9600页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：financial support by the National Natural Science Foundation of China(No.22172167) 

主　　题：gold clusters size hierarchy AunSm acetylene hydrochlorination scaling relationship 

摘      要：Size hierarchy is a distinct feature of nanogold-catalysts as it can strongly affect their performance in various reactions. We developed a simple method to generate Au n S m nanoclusters of different sizes by thermal treatment of an Au144(PET)60 (PET: phenylethanethiol) parent cluster. These clusters, deposited on activated carbon, exhibit excellent catalytic performance in the hydrochlorination of acetylene. In-situ ultraviolet laser dissociation high-resolution mass spectrometry of the parent cluster in the presence of acetylene revealed a remarkable cluster size-dependence of acetylene adsorption, which is a crucial step in the hydrochlorination. Systematic density functional theory calculations of the reaction pathways on the differently-sized clusters provide deeper insight into the cluster size dependence of the adsorption energies of the reactants and afforded a scaling relationship between the adsorption energy of acetylene and the co-adsorption energies of the reactants (C_(2)H_(2) and HCl), which could enable a qualitative prediction of the optimal Au n S m cluster for the hydrochlorination of acetylene.