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Integration of mesopores and crystal defects in metal-organic frameworks via templated electrosynthesis

DOI: 10.1038/s41467-019-12268-5 DOI Help

Authors: Xinchen Kang (University of Manchester) , Kai Lyu (University of Manchester) , Lili Li (University of Manchester) , Jiangnan Li (University of Manchester) , Louis Kimberley (University of Manchester) , Bin Wang (University of Manchester) , Lifei Liu (Institute of Chemistry, Chinese Academy of Science) , Yongqiang Cheng (Oak Ridge National Laboratory) , Mark D. Frogley (Diamond Light Source) , Svemir Rudic (ISIS Facility) , Anibal J. Ramirez-cuesta (Oak Ridge National Laboratory) , Robert A. W. Dryfe (University of Manchester) , Buxing Han (Institute of Chemistry, Chinese Academy of Science) , Sihai Yang (University of Manchester) , Martin Schroder (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Communications , VOL 10

State: Published (Approved)
Published: October 2019
Diamond Proposal Number(s): 19171

Open Access Open Access

Abstract: Incorporation of mesopores and active sites into metal-organic framework (MOF) materials to uncover new efficient catalysts is a highly desirable but challenging task. We report the first example of a mesoporous MOF obtained by templated electrosynthesis using an ionic liquid as both electrolyte and template. The mesoporous Cu(II)-MOF MFM-100 has been synthesised in 100 seconds at room temperature, and this material incorporates crystal defects with uncoupled Cu(II) centres as evidenced by confocal fluorescence microscopy and electron paramagnetic resonance spectroscopy. MFM-100 prepared in this way shows exceptional catalytic activity for the aerobic oxidation of alcohols to produce aldehydes in near quantitative yield and selectivity under mild conditions, as well as having excellent stability and reusability over repeated cycles. The catalyst-substrate binding interactions have been probed by inelastic neutron scattering. This study offers a simple strategy to create mesopores and active sites simultaneously via electrochemical formation of crystal defects to promote efficient catalysis using MOFs.

Journal Keywords: Metal–organic frameworks; Chemical synthesis

Subject Areas: Chemistry, Materials


Instruments: B22-Multimode InfraRed imaging And Microspectroscopy

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s41467-019-12268-5.pdf