Liu, L;
Chen, Z;
Wang, J;
Zhang, D;
Zhu, Y;
Ling, S;
Huang, K-W;
... Han, Y; + view all
(2019)
Imaging defects and their evolution in a metal-organic framework at sub-unit-cell resolution.
Nature Chemistry
, 11
(7)
pp. 622-628.
10.1038/s41557-019-0263-4.
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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.
| Type: | Article |
|---|---|
| Title: | Imaging defects and their evolution in a metal-organic framework at sub-unit-cell resolution |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41557-019-0263-4 |
| Publisher version: | https://doi.org/10.1038/s41557-019-0263-4 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10085205 |
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