Pd1/CeO2 single-atom catalyst for alkoxycarbonylation of aryl iodides  

单原子Pd1/CeO2催化剂催化芳香族碘化物烷氧基羰基化反应

作　　者：Fang Chen Tianbo Li Xiaoli Pan Yalin Guo Bing H an Fei Liu Botao Qiao Aiqin W ang Tao Zhang 陈芳;李天泊;潘晓丽;郭亚琳;韩冰;刘菲;乔波涛;王爱琴;张涛(CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China;University of Chinese Academy of Sciences,Beijing 100049,China;Dalian National Laboratory for Clean Energy,Dalian 116023,China)

机构地区：[1]CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]Dalian National Laboratory for Clean Energy,Dalian 116023,China

出　　处：《Science China Materials》2020年第6期959-964,共6页中国科学（材料科学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (21776270);the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100);China Postdoctoral Science Foundation(2017M621170);DICP Outstanding Postdoctoral Foundation(2017YB02);Liaoning Revitalization Talents Program;dedicated funds for methanol conversion from DICP

摘　　要：Heterogenization of the homogeneous catalysis has been studied for almost 50 years.Single-atom catalysis has the advantages of both homo-and heterogeneous catalysis.It has been proposed,and subsequently experimentally verified that single-atom catalysis is able to bridge homo-and heterogeneous catalysis,thus providing a new avenue to realize the heterogenization of homogeneous catalysis.Alkoxycarbonylation of aryl halides is an effective method for the direct synthesis of carboxylic acid derivatives,and is commonly catalyzed by Pd-based homogeneous complexes with N/P-containing ligands and organic/inorganic base.Herein,we firstly reported that Pd1/CeO2 single-atom catalyst showed good performance in the alkoxycarbonylation of aryl iodides reaction.Under base-free and ligand-free conditions,Pd1/CeO2 single-atom catalyst can transfer different aryl iodides to corresponding products.The catalyst can be easily recovered and reused four times without significant loss of reactivity.均相反应多相化是一个由来已久的研究课题.作为多相催化研究的新前沿,单原子催化剂兼具均相催化剂孤立活性位点和多相催化剂简单易分离的优势,自提出以来便被认为有望成为联系均相催化与多相催化的桥梁,而且近几年来已从实验上得到了证实.因此单原子催化剂为均相催化反应多相化提供了新途径.卤代芳烃烷氧基羰基化反应被广泛用于合成芳香族醛、酮、酸及其衍生物,但该反应目前主要采用均相Pd基催化剂,而且还需添加配体或有机/无机碱.本文中,我们首次报道了将单原子催化剂Pd1/CeO2用于芳香族碘化物烷氧基羰基化反应中,在无配体和无外加碱辅助下,催化剂表现出优异的活性、良好的循环稳定性以及底物普适性.

关 键 词：single-atom catalyst ALKOXYCARBONYLATION Pd1/CeO2 heterogenization base-free 

分 类 号：O643.36[理学—物理化学]