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Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction I12-JEEP: Joint Engineering, Environmental and Processing	Analysis by synchrotron X-ray scattering of the kinetics of formation of an Fe-based metal-organic framework with high CO 2 adsorption Harry G. W. Godfrey , Lydia Briggs , Xue Han , William J. F. Trenholme , Christopher Morris , Mathew Savage , Louis Kimberley , Oxana Magdysyuk , Michael Drakopoulos , Claire A. Murray , Chiu C. Tang , Mark D. Frogley , Gianfelice Cinque , Sihai Yang , Martin Schroeder Apl Materials 7 DOI: 10.1063/1.5121644 Diamond Proposal Number(s): [11278] Open Access Show Abstract ▼ Abstract: Understanding the mechanism of assembly and function of metal-organic frameworks (MOFs) is important for the development of practical materials. Herein, we report a time-resolved diffraction analysis of the kinetics of formation of a robust MOF, MFM-300(Fe), which shows high adsorption capacity for CO2 (9.55 mmol g−1 at 293 K and 20 bar). Applying the Avrami-Erofe’ev and the two-step kinetic Finke-Watzky models to in situ high-energy synchrotron X-ray powder diffraction data obtained during the synthesis of MFM-300(Fe) enables determination of the overall activation energy of formation (50.9 kJ mol−1), the average energy of nucleation (56.7 kJ mol−1), and the average energy of autocatalytic growth (50.7 kJ mol−1). The synthesis of MFM-300(Fe) has been scaled up 1000-fold, enabling the successful breakthrough separations of the CO2/N2 mixture in a packed-bed with a selectivity for CO2/N2 of 21.6. This study gives an overall understanding for the intrinsic behaviors of this MOF system, and we have determined directly the binding domains and dynamics for adsorbed CO2 molecules within the pores of MFM-300(Fe).	Nov 2019
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
I11-High Resolution Powder Diffraction	Iodine adsorption in a redox-active metal–organic framework: electrical conductivity induced by host−guest charge-transfer Xinran Zhang , Ivan Da Silva , Rodrigo Fazzi , Alena M. Sheveleva , Xue Han , Ben F. Spencer , Sergey A. Sapchenko , Floriana Tuna , Eric J. L. Mcinnes , Ming Li , Sihai Yang , Martin Schroder Inorganic Chemistry DOI: 10.1021/acs.inorgchem.9b02176 Diamond Proposal Number(s): [21079] Show Abstract ▼ Abstract: We report a comparative study of the binding of I2 (iodine) in a pair of redox-active metal–organic framework (MOF) materials, MFM-300(VIII) and its oxidized, deprotonated analogue, MFM-300(VIV). Adsorption of I2 in MFM-300(VIII) triggers a host-to-guest charge-transfer, accompanied by a partial (∼30%) oxidation of the VIII centers in the host framework and formation of I3– species residing in the MOF channels. Importantly, this charge-transfer induces a significant enhancement in the electrical conductivity (Δσ = 700000) of I2@MFM-300(VIII/IV) in comparison to MFM-300(VIII). In contrast, no host–guest charge-transfer or apparent change in the conductivity was observed upon adsorption of I2 in MFM-300(VIV). High-resolution synchrotron X-ray diffraction of I2@MFM-300(VIII/IV) confirms the first example of self-aggregation of adsorbed iodine species (I2 and I3–) into infinite helical chains within a MOF.	Sep 2019
I11-High Resolution Powder Diffraction	Exceptional adsorption and binding of sulfur dioxide in a robust zirconium-based metal–organic framework Joseph H. Carter , Xue Han , Florian Y. Moreau , Ivan Da Silva , Adam Nevin , Harry G. W. Godfrey , Chiu C. Tang , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society DOI: 10.1021/jacs.8b08433 Diamond Proposal Number(s): [14341] Show Abstract ▼ Abstract: We report a record-high SO2 adsorption capacity of 12.3 mmol g–1 in a robust porous material, MFM-601, at 298 K and 1.0 bar. SO2 adsorption in MFM-601 is fully reversible and highly selective over CO2 and N2. The binding domains for adsorbed SO2 and CO2 molecules in MFM-601 have been determined by in situ synchrotron X-ray diffraction experiments, giving insights at the molecular level to the basis of the observed high selectivity.	Nov 2018
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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