Ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes  

作　　者：Jumei Zhang Ziheng Zhang Gang Li Hongjin Qiao Hua Xie Ling Jiang 

机构地区：[1]School of Life Science,Ludong University,Yantai 264025,China [2]State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China

出　　处：《Chinese Chemical Letters》2025年第2期151-155,共5页中国化学快报(英文版)

基　　金：supported by the Natural Science Foundation of Shandong Province(No.ZR2021QB215);the National Natural Science Foundation of China(Nos.22273101,22125303,92061203,21327901,and 22288201);Dalian Institute of Chemical Physics(No.DICP I202437);the Talent Induction Program for Youth Innovation Teams in Colleges and Universities of Shandong Province(No.2022-2024);the Talent Introduction Research Start-up Funds of Ludong University(No.20212026)。

摘　　要：A series of heteronuclear yttrium-nickel monoxide carbonyl complexes YNiO(CO)_(n)^(-)(n=1-5)were generated in a pulsed-laser vaporization source and characterized by mass-selected photoelectron velocity-map spectroscopy combined with theoretical calculations.CO ligand-mediated reactivity in CO oxidation of yttrium-nickel monoxide carbonyl complexes was experimentally and theoretically identified.During the consecutive CO adsorption,aμ^(2)-O linear structure was most favorable for YNiO(CO)_(n)^(-)(n=1,2),then a structure in which the terminal O was bonded to the Y atom became favored for YNiO(CO)_(3)^(-),and finally a structure bearing a CO_(2)moiety was most favorable for YNiO(CO)_(n)^(-)(n=4,5).Theoretical calculations indicated that the Ni atom acted as an electron acceptor and accumulated electron density at n≤3,and then served as an electron donor along with the Y atom to contribute electron density in the rearrangement that accompanied CO oxidation at n>3.

关 键 词：Heteronuclear cluster CO oxidation Electron donor Quantum chemical calculation Photoelectron velocity-map imaging spectroscopy 

分 类 号：O641.4[理学—物理化学] O621.254.1[理学—化学]