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

Xinchen Kang, Kai Lyu, Lili Li, Jiangnan Li, Louis Kimberley, Bin Wang, Lifei Liu, Yongqiang Cheng, Mark D. Frogley, Svemir Rudić, Anibal J. Ramirez-Cuesta, Robert A. W. Dryfe, Buxing Han, Sihai Yang () and Martin Schröder ()
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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: Chinese Academy of Science
Yongqiang Cheng: Oak Ridge National Laboratory
Mark D. Frogley: Harwell Science Campus
Svemir Rudić: STFC Rutherford Appleton Laboratory
Anibal J. Ramirez-Cuesta: Oak Ridge National Laboratory
Robert A. W. Dryfe: University of Manchester
Buxing Han: Chinese Academy of Science
Sihai Yang: University of Manchester
Martin Schröder: University of Manchester

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-12268-5

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