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Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy	Reversible coordinative binding and separation of sulfur dioxide in a robust metal–organic framework with open copper sites Gemma L. Smith , Jennifer E. Eyley , Xue Han , Xinran Zhang , Jiangnan Li , Nicholas M. Jacques , Harry G. W. Godfrey , Stephen P. Argent , Laura J. Mccormick Mcpherson , Simon J. Teat , Yongqiang Cheng , Mark D. Frogley , Gianfelice Cinque , Sarah Day , Chiu C. Tang , Timothy L. Easun , Svemir Rudic , Anibal J. Ramirez-cuesta , Sihai Yang , Martin Schroeder Nature Materials 29 DOI: 10.1038/s41563-019-0495-0 Show Abstract ▼ Abstract: Emissions of SO2 from flue gas and marine transport have detrimental impacts on the environment and human health, but SO2 is also an important industrial feedstock if it can be recovered, stored and transported efficiently. Here we report the exceptional adsorption and separation of SO2 in a porous material, [Cu2(L)] (H4L = 4′,4‴-(pyridine-3,5-diyl)bis([1,1′-biphenyl]-3,5-dicarboxylic acid)), MFM-170. MFM-170 exhibits fully reversible SO2 uptake of 17.5 mmol g−1 at 298 K and 1.0 bar, and the SO2 binding domains for trapped molecules within MFM-170 have been determined. We report the reversible coordination of SO2 to open Cu(ii) sites, which contributes to excellent adsorption thermodynamics and selectivities for SO2 binding and facile regeneration of MFM-170 after desorption. MFM-170 is stable to water, acid and base and shows great promise for the dynamic separation of SO2 from simulated flue gas mixtures, as confirmed by breakthrough experiments.	Oct 2019
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 I11-High Resolution Powder Diffraction	Post-synthetic modulation of the charge distribution in a metal-organic framework for optimal binding of carbon dioxide and sulfur dioxide Lei Li , Ivan Da Silva , Daniil I. Kolokolov , Xue Han , Jiangnan Li , Gemma Smith , Yongqiang Cheng , Luke L. Daemen , Christopher G. Morris , Harry G. W. Godfrey , Nicholas Jacques , Xinran Zhang , Pascal Manuel , Mark D. Frogley , Claire A. Murray , Anibal J. Ramirez-cuesta , Gianfelice Cinque , Chiu C. Tang , Alexander G. Stepanov , Sihai Yang , Martin Schroder Chemical Science DOI: 10.1039/C8SC01959B Diamond Proposal Number(s): [14564, 15970] Open Access Show Abstract ▼ Abstract: Modulation of pore environment is an effective strategy to optimize guest binding in porous materials. We report the post-synthetic modification of the charge distribution in a charged metal-organic framework, MFM-305-CH3, [Al(OH)(L)]Cl, [(H2L)Cl = 3,5-dicarboxy-1-methylpyridinium chloride] and its effect on guest binding. MFM-305-CH3 shows a distribution of cationic (methylpyridinium) and anionic (chloride) centers and can be modified to release free pyridyl N-centres by thermal demethylation of the 1-methylpyridinium moiety to give the neutral isostructural MFM-305. This leads simultaneously to enhanced adsorption capacities and selectivities (two parameters that often change in opposite directions) for CO2 and SO2 in MFM-305. The host-guest binding has been comprehensively investigated by in situ synchrotron X-ray and neutron powder diffraction, inelastic neutron scattering, synchrotron infrared and 2H NMR spectroscopy and theoretical modelling to reveal the binding domains of CO2 and SO2 in these materials. CO2 and SO2 binding in MFM-305-CH3 is shown to occur via hydrogen bonding to the methyl and aromatic-CH groups, with a long range interaction to chloride for CO2. In MFM-305 the hydroxyl, pyridyl and aromatic C-H groups bind CO2 and SO2 more effectively via hydrogen bonds and dipole interactions. Post-synthetic modification via dealkylation of the as-synthesised metal-organic framework is a powerful route to the synthesis of materials incorporating active polar groups that cannot be prepared directly.	Oct 2018

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