4.7 Article

Redox property switching in MOFs with open metal sites for improved catalytic hydrogenation performance

Journal

JOURNAL OF ALLOYS AND COMPOUNDS
Volume 888, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.jallcom.2021.161494

Keywords

Metal-organic frameworks; Open metal sites; Catalysis; Hydrogenation; 4-nitrophenol

Funding

  1. National Natural Science Foundation of China [21902022, 21601028]
  2. Shandong Provincial Natural Science Foundation [ZR2018LB018, ZR2019QB026, ZR2020QB082]
  3. Dezhou Graduate School, North University of China [2020010JJ]
  4. Dezhou University Scientific Research Foundation [2019xgrc07, 30101409, 30101905, 2020xjpy07, 2020xjpy08]

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In this study, a decompression-thermalization strategy was used to tune the redox and catalytic hydrogenation properties of a Cu-containing metal-organic framework (MOF). The generation of open metal sites (OMSs) significantly improved the catalytic performance in hydrogenation reactions, with experimental and theoretical results showing that OMSs endow Cu species with unique electronic properties.
In this study, a decompression-thermalization strategy was utilized for a Cu-containing metal-organic framework (MOF) to tune its redox and catalytic hydrogenation properties. Remarkably, at just 120 degrees C, open metal sites (OMSs) were successfully constructed by removing coordinated solvent molecules to generate the daughter MOF-120. The tailored redox property of MOF-120 is correlated with the presence of OMSs. Compared with the pristine MOF where copper cations were capped by DMF, MOF-120 exhibited improved kinetics, showed a reduction of activation energy and outstanding recyclability in the hydrogenation of 4nitrophenol under mild conditions (25 degrees C, 1 atm). Both experimental studies and theoretical calculation results reveal that the generation of OMSs endows the Cu species with unique electronic properties, which assist the adsorption and electron transfer between substrate molecules and is responsible for the enhanced performance in the hydrogenation process. (c) 2021 Elsevier B.V. All rights reserved.

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