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    Imaging defects and their evolution in a metal–organic framework at sub-unit-cell resolution

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    Type
    Article
    Authors
    Liu, Lingmei
    Chen, Zhijie cc
    Wang, Jianjian cc
    Zhang, Daliang cc
    Zhu, Yihan
    Ling, Sanliang cc
    Huang, Kuo-Wei cc
    Belmabkhout, Youssef cc
    Adil, Karim cc
    Zhang, Yuxin
    Slater, Ben cc
    Eddaoudi, Mohamed cc
    Han, Yu cc
    KAUST Department
    Advanced Membranes and Porous Materials Research Center
    Chemical Science Program
    Electron Microscopy
    Functional Materials Design, Discovery and Development (FMD3)
    Homogeneous Catalysis Laboratory (HCL)
    KAUST Catalysis Center (KCC)
    Nanostructured Functional Materials (NFM) laboratory
    Physical Science and Engineering (PSE) Division
    KAUST Grant Number
    FCC/1/1972-19
    Date
    2019-05-13
    Embargo End Date
    2019-11-13
    Submitted Date
    2018-06-04
    Permanent link to this record
    http://hdl.handle.net/10754/655981
    
    Metadata
    Show full item record
    Abstract
    Defect engineering of metal–organic frameworks (MOFs) offers promising opportunities for tailoring their properties to specific functions and applications. However, determining the structures of defects in MOFs—either point defects or extended ones—has proved challenging owing to the difficulty of directly probing local structures in these typically fragile crystals. Here we report the real-space observation, with sub-unit-cell resolution, of structural defects in the catalytic MOF UiO-66 using a combination of low-dose transmission electron microscopy and electron crystallography. Ordered ‘missing linker’ and ‘missing cluster’ defects were found to coexist. The missing-linker defects, reconstructed three-dimensionally with high precision, were attributed to terminating formate groups. The crystallization of the MOF was found to undergo an Ostwald ripening process, during which the defects also evolve: on prolonged crystallization, only the missing-linker defects remained. These observations were rationalized through density functional theory calculations. Finally, the missing-cluster defects were shown to be more catalytically active than their missing-linker counterparts for the isomerization of glucose to fructose.
    Citation
    Liu, L., Chen, Z., Wang, J., Zhang, D., Zhu, Y., Ling, S., … Han, Y. (2019). Imaging defects and their evolution in a metal–organic framework at sub-unit-cell resolution. Nature Chemistry, 11(7), 622–628. doi:10.1038/s41557-019-0263-4
    Sponsors
    This research was supported by Competitive Center Funds (FCC/1/1972-19) to Y.H. and M.E. from King Abdullah University of Science and Technology. This research used resources of the Core Labs of King Abdullah University of Science and Technology. Yi.Z. acknowledges financial support from the National Natural Science Foundation of China (21771161) and the Thousand Talents Program for Distinguished Young Scholars. S.L. and B.S. are thankful to the Materials Chemistry Consortium (EPSRC: EP/L000202) for provision of computer time on ARCHER UK National Supercomputing Service. B.S. acknowledges the Royal Society for financial support through an industry fellowship (F160062). The authors acknowledge helpful discussions with A. Goodwin, M. Cliffe and G. Shearer.
    Publisher
    Springer Nature
    Journal
    Nature Chemistry
    DOI
    10.1038/s41557-019-0263-4
    PubMed ID
    31086300
    Additional Links
    http://www.nature.com/articles/s41557-019-0263-4
    ae974a485f413a2113503eed53cd6c53
    10.1038/s41557-019-0263-4
    Scopus Count
    Collections
    Articles; Advanced Membranes and Porous Materials Research Center; Physical Science and Engineering (PSE) Division; Functional Materials Design, Discovery and Development (FMD3); Chemical Science Program; KAUST Catalysis Center (KCC)

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