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Instruments / Technical Area	Publication Details	Published	Actions
I15-Extreme Conditions	Pressure promoted low-temperature melting of metal–organic frameworks Remo N. Widmer , Giulio I. Lampronti , Simone Anzellini , Romain Gaillac , Stefan Farsang , Chao Zhou , Ana M. Belenguer , Craig Wilson , Hannah Palmer , Annette K. Kleppe , Michael T. Wharmby , Xiao Yu , Seth M. Cohen , Shane G. Telfer , Simon A. T. Redfern , François-Xavier Coudert , Simon Macleod , Thomas Bennett Nature Materials 18, 370 - 376 DOI: 10.1038/s41563-019-0317-4 Diamond Proposal Number(s): [16133, 19046] Show Abstract ▼ Abstract: Metal–organic frameworks (MOFs) are microporous materials with huge potential for chemical processes. Structural collapse at high pressure, and transitions to liquid states at high temperature, have recently been observed in the zeolitic imidazolate framework (ZIF) family of MOFs. Here, we show that simultaneous high-pressure and high-temperature conditions result in complex behaviour in ZIF-62 and ZIF-4, with distinct high- and low-density amorphous phases occurring over different regions of the pressure–temperature phase diagram. In situ powder X-ray diffraction, Raman spectroscopy and optical microscopy reveal that the stability of the liquid MOF state expands substantially towards lower temperatures at intermediate, industrially achievable pressures and first-principles molecular dynamics show that softening of the framework coordination with pressure makes melting thermodynamically easier. Furthermore, the MOF glass formed by melt quenching the high-temperature liquid possesses permanent, accessible porosity. Our results thus imply a route to the synthesis of functional MOF glasses at low temperatures, avoiding decomposition on heating at ambient pressure.	Mar 2019
I22-Small angle scattering & Diffraction	Flux melting of metal–organic frameworks Louis Longley , Sean M. Collins , Shichun Li , Glen J. Smales , Ilknur Erucar , Ang Qiao , Jingwei Hou , Cara M. Doherty , Aaron W. Thornton , Anita J. Hill , Xiao Yu , Nicholas J. Terrill , Andrew J. Smith , Seth M. Cohen , Paul A. Midgley , David A. Keen , Shane G. Telfer , Thomas Bennett Chemical Science 341 DOI: 10.1039/C8SC04044C Diamond Proposal Number(s): [18236] Open Access Show Abstract ▼ Abstract: Recent demonstrations of melting in the metal–organic framework (MOF) family have created interest in the interfacial domain between inorganic glasses and amorphous organic polymers. The chemical and physical behaviour of porous hybrid liquids and glasses is of particular interest, though opportunities are limited by the inaccessible melting temperatures of many MOFs. Here, we show that the processing technique of flux melting, ‘borrowed’ from the inorganic domain, may be applied in order to melt ZIF-8, a material which does not possess an accessible liquid state in the pure form. Effectively, we employ the high-temperature liquid state of one MOF as a solvent for a secondary, non-melting MOF component. Differential scanning calorimetry, small- and wide-angle X-ray scattering, electron microscopy and X-ray total scattering techniques are used to show the flux melting of the crystalline component within the liquid. Gas adsorption and positron annihilation lifetime spectroscopy measurements show that this results in enhanced, accessible porosity to a range of guest molecules in the resultant flux melted MOF glass.	Feb 2019

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