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Instruments / Technical Area	Publication Details	Published	Actions
B22-Multimode InfraRed imaging And Microspectroscopy	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 Rudic , Anibal J. Ramirez-Cuesta , Robert A. W. Dryfe , Buxing Han , Sihai Yang , Martin Schroder Nature Communications 10 DOI: 10.1038/s41467-019-12268-5 Diamond Proposal Number(s): [19171] Open Access Show 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.	Oct 2019
B22-Multimode InfraRed imaging And Microspectroscopy	Quantitative electro-reduction of CO2 to liquid fuel over electro-synthesized metal–organic frameworks Xinchen Kang , Bin Wang , Kui Hu , Kai Lyu , Xue Han , Ben F. Spencer , Mark D. Frogley , Floriana Tuna , Eric J. L. Mcinnes , Robert A. W. Dryfe , Buxing Han , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society DOI: 10.1021/jacs.0c05913 Diamond Proposal Number(s): [19171] Open Access Show Abstract ▼ Abstract: Efficient electro-reduction of CO2 over metal–organic framework (MOF) materials is hindered by the poor contact between thermally synthesized MOF particles and the electrode surface, which leads to low Faradaic efficiency for a given product and poor electrochemical stability of the catalyst. We report a MOF-based electrode prepared via electro-synthesis of MFM-300(In) on an indium foil, and its activity for the electrochemical reduction of CO2 is assessed. The resultant MFM-300(In)-e/In electrode shows a 1 order of magnitude improvement in conductivity compared with that for MFM-300(In)/carbon-paper electrodes. MFM-300(In)-e/In exhibits a current density of 46.1 mA cm–2 at an applied potential of −2.15 V vs Ag/Ag+ for the electro-reduction of CO2 in organic electrolyte, achieving an exceptional Faradaic efficiency of 99.1% for the formation of formic acid. The facile preparation of the MFM-300(In)-e/In electrode, coupled with its excellent electrochemical stability, provides a new pathway to develop efficient electro-catalysts for CO2 reduction.	Sep 2020

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