Catalytically Active Atomically Thin Cuprate with Periodic Cu Single Sites
Koh, Ming Joo
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Chemical Science Program
Physical Science and Engineering (PSE) Division
Permanent link to this recordhttp://hdl.handle.net/10754/678271
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AbstractRational design and synthesis of catalytically active two-dimensional (2D) materials with an abundance of atomically precise active sites in their basal planes remains a grand challenge. Here, we report a ligand exchange strategy to exfoliate bulk [Cu4(OH)6][O3S(CH2)4SO3] cuprate crystals into atomically thin 2D cuprate layers ([Cu2(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 mechanistic studies reveal that the reactions proceed via coordinatively unsaturated CuO4(II) 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 an attractive catalyst candidate for broad utility in fine chemical synthesis.
CitationYang, H., Xi, S., Guo, N., Wang, M., Liu, L., Lyu, P., Yu, X., Li, J., Xu, H., Hai, X., Li, Z., Li, X., Sun, T., Zhao, X., Han, Y., Yu, W., Wu, J., Zhang, C., Fei, H., … Lu, J. (2022). Catalytically Active Atomically Thin Cuprate with Periodic Cu Single Sites. National Science Review. https://doi.org/10.1093/nsr/nwac100
SponsorsJ.L. acknowledges the support from Ministry of Education of Singapore Grant (R-143-000-B47-114). J.L. and J.W. thank the support from National University of Singapore Flagship Green Energy Program (R-143-000-A55-646) and Agency for Science, Technology and Research (A*STAR) under its Advanced Manufacturing and Engineering Individual Research Grants Grant (A20E5c0096). C.Z. thanks the support of Ministry of Education of Singapore Grant (R-723-000-029-112), National University of Singapore Green Energy Program (R-143-000-A63-114) and National University of Singapore Graphene Center Computer Clusters. M.J.K. acknowledges the support form Ministry of Education of Singapore Academic Research Funds Tier 1 (R-143-000-B57-114). S.-B.X. acknowledges the support from the X-ray Absorption Fine Structure for Catalysis Beamline of Singapore Synchrotron Light Source and the National Supercomputing Centre, Singapore. X.-X.Z. thanks the support from the Presidential Postdoctoral Fellowship, Nanyang Technological University, Singapore (03INS000973C150).
PublisherOxford University Press (OUP)
JournalNational Science Review
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