Fast Surface Restructuring within the Gap of Au Nanocube Dimer for the Enhancement of Catalytic Efficiency

查看全文 作　　者：Xiao [1]Wang;Zhongju [1]Ye;Jianhao [1]Hua;Lin [2]Wei;Shen [1]Lin;Lehui [1]Xiao 机构地区：[1]State Key Laboratory of Medicinal Chemical Biology,Tianjin Key Laboratory of Biosensing and Molecular Recognition,College of Chemistry,Nankai University,Tianjin 300071;[2]College of Chemistry and Chemical Engineering,Hunan Normal University,Changsha 410081 出　　处：《CCS Chemistry》索引2022年第4卷第3期,共13页 基　　金：This research was made possible by a generous grant from National Natural Science Foundation of China(NSFC,project no.21974073). 摘　　要：Identification of the catalytic dynamics and plasmonic effects plays a critical role in the design of heterogeneous catalysts.However,the knowledge of plasmonic effect on catalytic dynamics remains limited at the single-particle level.Using the non-fluorescent amplex red to fluorescent resorufin as a model reaction,significant enhancement in catalytic efficiency from the coupled Au nanocube dimer(AuCD)was clearly revealed with the single-molecule fluorescence microscopy.AuCD exhibits noticeably higher catalytic efficiency than the monomer,which is attributed to the spontaneous dynamic surface restructuring.Spatiotemporally resolved dynamics suggest that the active catalytic sites essentially originate from the plasmonic nanogap where an electromagnetic(EM)hot spot exists.The enhanced EM field accelerates the generation of hot carriers and promotes the spontaneous surface restructuring by enhancing the lattice vibrations,which ultimately improves the catalytic activity.These microscopic views provide new insights into the effect of EM fields on surface restructuring dynamics of nanocatalysts. 关 键 词：dark-field plasmonic nanoparticles Raman spectroscopy surface dynamic restructuring single-particle imaging