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作 者:Xuhui Fan Fan Wang Mengjiao Li Faiza Meharban Yaying Li Yuanyuan Cui Xiaopeng Li Jingsan Xu Qi Xiao Wei Luo
机构地区:[1]State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,College of Materials Science and Engineering,Donghua University,Shanghai 201620,China [2]Beijing Key Laboratory of Ionic Liquids Clean Process,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China [3]School of Chemical Sciences,University of Chinese Academy of Sciences,Beijing 100049,China [4]National Energy R&D Center for Coal to Liquid Fuels,Synfuels China Technology Co.,Ltd.,Beijing 101407,China [5]Shimadzu(China)Co.,Ltd.,Shanghai 200233,China [6]School of Chemistry and Physics&Centre for Materials Science,Queensland University of Technology,Brisbane,QLD 4001,Australia
出 处:《Chinese Chemical Letters》2025年第1期362-368,共7页中国化学快报(英文版)
基 金:supported by Shanghai Pujiang Program(No.21PJ1400400);the Research Start-up Fund at Donghua University;the Foundation of State Key Laboratory of Coal Combustion(No.FSKLCCA2309);the National Natural Science Foundation of China(No.22302109);the Australian Research Council(No.DP230102740)。
摘 要:In this work,we developed plasmonic photocatalyst composed of Cu Pd alloy nanoparticles supported on Ti N,the optimized Cu_(3)Pd_(2)/Ti N catalyst shows excellent conversion(>96%)and selectivity(>99%)for Heck reaction at 50℃ under visible light irradiation.By in-situ spectroscopic investigations,we find that visible light excitation could achieve stable metallic Cu species on the surface of Cu Pd alloy nanoparticles,thereby eliminating the inevitable surface oxides of Cu based catalyst.The in-situ formed metallic Cu species under irradiation take advantage of the strong interactions of Cu with visible light,and manifest in the localized surface plasmon resonances(LSPR)photoexcitation.Visible light excitation could further promote the charge transfer between catalytic Pd component and the support Ti N,resulting in electron-rich Pd sites on Cu Pd/Ti N.Moreover,light excitation on Cu Pd/Ti N generates strong chemisorption of iodobenzene and styrene,favoring the activation of reactants for Heck reaction.DFT calculations suggest that electron-rich Cu Pd sites ideally lower the activation energy barrier for the coupling reaction.This work provides valuable insights for mechanistic understanding of plasmonic photocatalysis.
关 键 词:PHOTOCATALYSIS CuPd alloy CHEMISORPTION Photocatalytic mechanism LSPR
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