Existence of a Heterogeneous Pathway in Palladium-Catalyzed Carbon–Carbon Coupling Reaction:Evidence from Ag@Pd_(3)Cu Intermetallic Nanoplates  

作　　者：Rui Liu Cuihong Xu Yanan Chen Huachao Zhao Jiefang Sun Zuoliang He Wanyu Shan Gang Li Qiantao Shi Liping Fang Jingfu Liu Guibin Jiang 

机构地区：[1]State Key Laboratory of Environmental Chemistry and Ecotoxicology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing 100085 [2]School of Environment,Hangzhou Institute of Advanced Study,University of Chinese Academy of Sciences,Hangzhou 310024 [3]Guangdong Key Laboratory of Integrated Agro-Environmental Pollution Control and Management,Institute of Eco-Environmental and Soil Sciences,Guangdong Academy of Sciences,Guangzhou 510650 [4]College of Resources and Environment,University of Chinese Academy of Sciences,Beijing 100049 [5]Beijing Center for Disease Prevention and Control,Beijing 100013 [6]Center for Environmental Systems,Stevens Institute of Technology,Hoboken,NJ 07030

出　　处：《CCS Chemistry》2022年第2期671-682,共12页中国化学会会刊（英文）

基　　金：the National Key R&D Program of China(no.2016YFA0203102);the National Natural Science Foundation of China(nos.21577157,21777177,and 21822608)。

摘　　要：Palladium(Pd)-catalyzed cross-coupling reaction is a widely studied process with significant economic interest and represents one of the most successful nanocatalytic examples.Owing to the observed leaching of Pd ions from both monometallic and short-range-ordered Pd bimetallic nanocatalysts,there is ambiguity regarding whether the coupling reaction has a heterogeneous component.Herein,facilitated by theoretical calculations,we discovered that the Pd ion leaching-free Pd_(3)Cu intermetallic compound was able to catalyze the cross-coupling reaction heterogeneously with activity comparable with that of Pd ions leached from monometallic Pd.The observation that Pd_(3)Cu acted as a heterogeneous catalyst was further confirmed by the reaction-promoting effect of hot electrons generated by the Ag core in Ag@Pd_(3)Cu nanoplates upon photon adsorption and could only participate in the reaction on the surface of the nanocatalyst.Additionally,it demonstrated experimentally the effectiveness of the heterogeneous route in the coupling reaction.This study shows that the combination of plasmonic catalysis and intermetallic compounds is a promising strategy for designing robust nanocatalysts to synthesize value-added chemicals.

关 键 词：plasmonic catalysis intermetallics carbon-carbon coupling reaction mechanism heterogeneous pathway 

分 类 号：O64[理学—物理化学]