Catalytically active atomically thin cuprate with periodic Cu single sites  

作　　者：Huimin Yang Shibo Xi Na Guo Mu Wang Lingmei Liu Pin Lyu Xiaolong Yu Jing Li Haomin Xu Xiao Hai Zejun Li Xinzhe Li Tao Sun Xiaoxu Zhao Yu Han Wei Yu Jie Wu Chun Zhang Honghan Fei Ming Joo Koh Jiong Lu 

机构地区：[1]Department of Chemistry,National University of Singapore,Singapore 117543,Singapore [2]Institute of Chemical and Engineering Sciences,Singapore 627833,Singapore [3]Department of Physics,National University of Singapore,Singapore 117542,Singapore [4]Advanced Membranes and Porous Materials Center,King Abdullah University of Science and Technology,Thuwal 23955-6900,Kingdom of Saudi Arabia [5]SDU-ANU Joint Science College,Shandong University,Weihai 264209,China [6]School of Materials Science and Engineering,Peking University,Beijing 100871,China [7]Centre for Advanced 2D Materials and Graphene Research Centre,National University of Singapore,Singapore 117546,Singapore [8]Department of Chemistry,Tongji University,Shanghai 200092,China

出　　处：《National Science Review》2023年第1期221-230,共10页国家科学评论（英文版）

基　　金：J.L.acknowledges the support of the Ministry of Education of Singapore Grant(R-143-000-B47-114);J.L.and J.W.are grateful for the support from the National University of Singapore Flagship Green Energy Program(R-143-000-A55-646);the Agency for Science,Technology and Research(A*STAR)under its Advanced Manufacturing and Engineering Individual Research Grants(A20E5c0096);C.Z.is grateful for the support of the Ministry of Education of Singapore Grant(MOE2019-T2-2-030);the National University of Singapore Green Energy Program(R-143-000-A63-114);National University of Singapore Graphene Center Computer Clusters and National Supercomputing Center computer resources;M.J.K.acknowledges the support of the Ministry of Education of Singapore Academic Research Funds Tier 1(R-143-000-B57-114);S.-B.X.acknowledges the support of the X-ray Absorption Fine Structure for Catalysis Beamline of Singapore Synchrotron Light Source and the National Supercomputing Centre,Singapore;X.-X.Z.is thankful for the support of the Presidential Postdoctoral Fellowship,Nanyang Technological University,Singapore(03INS000973C150)。

摘　　要：Rational design and synthesis of catalytically active two-dimensional(2D)materials with an abundance of atomically precise active sites in their basal planes remains a great challenge.Here,we report a ligand exchange strategy to exfoliate bulk[Cu_(4)(OH)_(6)][O_(3)S(CH_(2))_4SO_(3)]cuprate crystals into atomically thin 2D cuprate layers([Cu_(2)(OH)_(3)]^(+)).The basal plane of 2D cuprate layers contains periodic arrays of accessible unsaturated Cu(Ⅱ)single sites(2D-CuSSs),which are found to promote efficient oxidative Chan-Lam coupling.Our me chanistic studies reveal that the reactions proceed via coordinatively unsaturated CuO_4(Ⅰ)single sites with the formation of Cu(Ⅰ)species in the rate-limiting step,as corroborated by both operando experimental and theoretical studies.The robust stability of 2D-CuSSs in both batch and continuous flow reactions,coupled with their recyclability and good performance in complex molecule derivatization,render 2D-CuSSs attractive catalyst candidates for broad utility in fine chemical synthesis.

关 键 词：EXFOLIATION NANOSHEET heterogeneous catalysis 

分 类 号：O643.36[理学—物理化学]