Spectroscopic characterization of chain-to-ring structural evolution in platinum carbide clusters  

作　　者：Yu Zhang Shihu Du Zhi Zhao Haiyan Han Gang Li Jinghan Zou Hua Xie Ling Jiang 

机构地区：[1]State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]College of Chemistry and Chemical Engineering,Xinyang Normal University,Xinyang 464000,Henan,China [3]School of Mathematics and Physics,Hebei University of Engineering,Handan 056038,Hebei,China

出　　处：《Journal of Energy Chemistry》2023年第2期529-534,I0014,共7页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(22273101,22103082,22125303,92061203,and 22288201);the Youth Innovation Promotion Association of the Chinese Academy of Sciences(CAS)(2020187);the Innovation Program for Quantum Science and Technology(2021ZD0303304);Chinese Academy of Sciences(GJJSTD20220001);Dalian Institute of Chemical Physics(DICP DCLS201702);K.C.Wong Education Foundation(GJTD-201806)。

摘　　要：Metal carbides play an important role in catalysis and functional materials.However,the structural characterization of metal carbide clusters has been proven to be a challenging experimental target due to the difficulty in size selection.Here we use the size-specific photoelectron velocity-map imaging spectroscopy to study the structures and properties of platinum carbide clusters.Quantum chemical calculations are carried out to identify the structures and to assign the experimental spectra.The results indicate that the cluster size of the chain-to-ring structural evolution for the PtC_(n)^(-)anions occurs at n=14,whereas that for the PtC_(n) neutrals at n=10,revealing a significant effect of charge on the structures of metal carbides.The greatest importance of these building blocks is the strong preference of the Pt atom to expose in the outer side of the chain or ring,exhibiting the active sites for catalyzing potential reactions.These findings provide unique spectroscopic snapshots for the formation and growth of platinum carbide clusters and have important implications in the development of related single-atom catalysts with isolated metal atoms dispersed on supports.

关 键 词：CATALYSIS Functional material Metal carbide Photoelectron velocity-map imaging spectroscopy Quantum chemical calculation 

分 类 号：O643.36[理学—物理化学]