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.
Highlights
The electrolysis was continued for a further 400 s, and the precipitate collected via filtration and washed with DMF and acetone, each for five times, and the material dried at 60 °C
The electronic structure calculations were performed on the Γ-point only for the MOF due to its large unit cell, and on a 5 × 7 × 3 Monkhorst–Pack mesh for benzyl alcohol
The supercell used for the phonon calculation was 1 × 1 × 1 of the unit cell for the MOF, and 2 × 3 × 1 of the unit cell for benzyl alcohol
Summary
The as-synthesised material was collected via filtration and washed with hot DMF and acetone, each for five times, and dried at 60 °C. The electrolysis was continued for a further 400 s, and the precipitate collected via filtration and washed with DMF and acetone, each for five times, and the material dried at 60 °C. FTIR data were collected on a Bruker Vertex spectrometer on Beamline B22 at Diamond Light Source, while TGA measurements were performed under N2 at a heating rate of 10 °C/min.
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