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Instruments / Technical Area	Publication Details	Published
I11-High Resolution Powder Diffraction I19-Small Molecule Single Crystal Diffraction	Exceptional packing density of ammonia in a dual-functionalized metal–organic framework Christopher Marsh , Xue Han , Jiangnan Li , Zhenzhong Lu , Stephen Argent , Ivan Da Silva , Yongqiang Cheng , Luke L. Daemen , Anibal J. Ramirez-Cuesta , Stephen P. Thompson , Alexander J. Blake , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society 361 DOI: 10.1021/jacs.1c01749 Diamond Proposal Number(s): [23483, 11622] Open Access Show Abstract ▼ Abstract: We report the reversible adsorption of ammonia (NH3) up to 9.9 mmol g–1 in a robust Al-based metal–organic framework, MFM-303(Al), which is functionalized with free carboxylic acid and hydroxyl groups. The unique pore environment decorated with these acidic sites results in an exceptional packing density of NH3 at 293 K (0.801 g cm–3) comparable to that of solid NH3 at 193 K (0.817 g cm–3). In situ synchrotron X-ray diffraction and inelastic neutron scattering reveal the critical role of free −COOH and −OH groups in immobilizing NH3 molecules. Breakthrough experiments confirm the excellent performance of MFM-303(Al) for the capture of NH3 at low concentrations under both dry and wet conditions.	Apr 2021
I11-High Resolution Powder Diffraction I19-Small Molecule Single Crystal Diffraction	Multi-stimulus linear negative expansion of a breathing M(O2CR)4-node MOF Daniel Watkins , Thomas M. Roseveare , Mark R. Warren , Stephen P. Thompson , Ashleigh J. Fletcher , Lee Brammer Faraday Discussions 49 DOI: 10.1039/D0FD00089B Open Access Show Abstract ▼ Abstract: The metal–organic framework (Me2NH2)2[Cd(NO2BDC)2] (SHF-81) comprises flattened tetrahedral Cd(O2CR)42− nodes, in which Cd(II) centres are linked via NO2BDC2− ligands (2-nitrobenzene-1,4-dicarboxylate) to give a doubly interpenetrated anionic network, with charge balanced by two Me2NH2+ cations per Cd centre resident in the pores. The study establishes that this is a twinned α-quartz-type structure (trigonal, space group P3x21, x = 1 or 2), although very close to the higher symmetry β-quartz arrangement (hexagonal, P6x22, x = 2 or 4) in its as-synthesised solvated form [Cd(NO2BDC)2]·2DMF·0.5H2O (SHF-81-DMF). The activated MOF exhibits very little N2 uptake at 77 K, but shows significant CO2 uptake at 273–298 K with an isosteric enthalpy of adsorption (ΔHads) at zero coverage of −27.4 kJ mol−1 determined for the MOF directly activated from SHF-81-DMF. A series of in situ diffraction experiments, both single-crystal X-ray diffraction (SCXRD) and powder X-ray diffraction (PXRD), reveal that the MOF is flexible and exhibits breathing behaviour with observed changes as large as 12% in the a- and b-axes (\|Δa\|, \|Δb\| < 1.8 Å) and 5.5% in the c-axis (\|Δc\| < 0.7 Å). Both the solvated SHF-81-DMF and activated/desolvated SHF-81 forms of the MOF exhibit linear negative thermal expansion (NTE), in which pores that run parallel to the c-axis expand in diameter (a- and b-axis) while contracting in length (c-axis) upon increasing temperature. Adsorption of CO2 gas at 298 K also results in linear negative expansion (Δa, Δb > 0; Δc < 0; ΔV > 0). The largest change in dimensions is observed during activation/desolvation from SHF-81-DMF to SHF-81 (Δa, Δb < 0; Δc > 0; ΔV < 0). Collectively the nine in situ diffraction experiments conducted suggest the breathing behaviour is continuous, although individual desolvation and adsorption experiments do not rule out the possibility of a gating or step at intermediate geometries that is coupled with continuous dynamic behaviour towards the extremities of the breathing amplitude.	Nov 2020
I11-High Resolution Powder Diffraction	Long-term stability of MFM-300(Al) towards toxic air pollutants Joseph H. Carter , Christopher Morris , Harry G. W. Godfrey , Sarah J. Day , Jonathan Potter , Stephen P. Thompson , Chiu C. Tang , Sihai Yang , Martin Schroeder Acs Applied Materials & Interfaces DOI: 10.1021/acsami.0c11134 Diamond Proposal Number(s): [14555] Open Access Show Abstract ▼ Abstract: Temperature or pressure-swing sorption in porous metal-organic framework (MOF) materials has been proposed for new gas separation technologies. The high tuneability of MOFs toward particular adsorbates and the relatively low energy penalty for system regeneration means that reversible physisorption in MOFs has the potential to create economic and environmental benefits compared with state-of-the-art chemisorption systems. However, for MOF-based sorbents to be commercialised they have to show long-term stability under the conditions imposed by the application. Here, we demonstrate the structural stability of MFM-300(Al) to the presence of a series of industrially-relevant toxic and corrosive gases, including SO2, NO2 and NH3, over four years using long duration synchrotron X-ray powder diffraction. Full structural analysis of gas-loaded MFM-300(Al) confirms the retention of these toxic gas molecules within the porous framework for up to 200 weeks, and cycling adsorption experiments verified the reusability of MFM-300(Al) for the capture of these toxic air pollutants.	Aug 2020
I11-High Resolution Powder Diffraction	The properties of methane clathrate in the presence of ammonium sulphate solutions with relevance to Titan Emmal Safi , Stephen P. Thompson , Aneurin Evans , Sarah J. Day , Claire A. Murray , Annabelle R. Baker , Joana M. Oliveira , Jaco Th. Van Loon EPSC-DPS Joint Meeting 2019 Show Abstract ▼ Abstract: The source of atmospheric methane on Saturn’s satellite Titan is currently unknown. However, one possibility is that it originates from clathrate hydrates formed below the surface. Titan’s sub-surface ocean is believed to be composed of saline, rather than pure, water and in situ experimental data on clathrate formation under these conditions are largely absent in literature. Here, synchrotron X-ray powder diﬀraction (SXRPD) is used to study the properties of methane clathrate hydrates formed in the presence of ammonium sulphate solutions under low temperature conditions with a pressure of 26 bar.	Sep 2019

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