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Instruments / Technical Area	Publication Details	Published
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF)	Stepwise collapse of a giant pore metal–organic framework Adam F. Sapnik , Duncan N. Johnstone , Sean M. Collins , Giorgio Divitini , Alice M. Bumstead , Christopher W. Ashling , Philip A. Chater , Dean S. Keeble , Timothy Johnson , David A. Keen , Thomas D. Bennett Dalton Transactions 38 DOI: 10.1039/D1DT00881A Diamond Proposal Number(s): [20038, 20198] Open Access Show Abstract ▼ Abstract: Defect engineering is a powerful tool that can be used to tailor the properties of metal–organic frameworks (MOFs). Here, we incorporate defects through ball milling to systematically vary the porosity of the giant pore MOF, MIL-100 (Fe). We show that milling leads to the breaking of metal–linker bonds, generating additional coordinatively unsaturated metal sites, and ultimately causes amorphisation. Pair distribution function analysis shows the hierarchical local structure is partially retained, even in the amorphised material. We find that solvents can be used to stabilise the MIL-100 (Fe) framework against collapse, which leads to a substantial retention of porosity over the non-stabilised material.	Mar 2021
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF)	A new route to porous metal–organic framework crystal–glass composites Shichun Li , Shuwen Yu , Sean M. Collins , Duncan N. Johnstone , Christopher W. Ashling , Adam F. Sapnik , Philip A. Chater , Dean S. Keeble , Lauren N. Mchugh , Paul A. Midgley , David A. Keen , Thomas D. Bennett Chemical Science 11, 9910 - 9918 DOI: 10.1039/D0SC04008H Diamond Proposal Number(s): [20038, 22632, 21979] Open Access Show Abstract ▼ Abstract: Metal–organic framework crystal–glass composite (MOF CGC) materials consist of a crystalline MOF embedded within a MOF–glass matrix. In this work, a new synthetic route to these materials is demonstrated through the preparation of two ZIF-62 glass-based CGCs, one with crystalline ZIF-67 and the other with crystalline UiO-66. Previous attempts to form these CGCs failed due to the high processing temperatures involved in heating above the melting point of ZIF-62. Annealing of the ZIF-62 glass above the glass transition with each MOF however leads to stable CGC formation at lower temperatures. The reduction in processing temperatures will enable the formation of a greatly expanded range of MOF CGCs.	Sep 2020
I15-1-X-ray Pair Distribution Function (XPDF)	Tuning the morphological appearance of iron(III) fumarate: impact on material characteristics and biocompatibility Patrick Hirschle , Christian Hirschle , Konstantin Böll , Markus Döblinger , Miriam Höhn , Joshua M. Tuffnell , Christopher W. Ashling , David Keen , Thomas D. Bennett , Joachim O. Rädler , Ernst Wagner , Michael Peller , Ulrich Lächelt , Stefan Wuttke Chemistry Of Materials DOI: 10.1021/acs.chemmater.9b03662 Diamond Proposal Number(s): [21260] Show Abstract ▼ Abstract: Iron(III) fumarate materials are well suited for biomedical applications as they feature biocompatible building blocks, porosity, chemical functionalizability, and magnetic resonance imaging (MRI) activity. The synthesis of these materials however is difficult to control, and it has been challenging to produce monodisperse particle sizes and morphologies that are required in medical use. Here, we report the optimization of iron(III) fumarate nano- and microparticle synthesis by surfactant-free methods, including room temperature, solvothermal, microwave, and microfluidic conditions. Four variants of iron(III) fumarate with distinct morphologies were isolated and are characterized in detail. Structural characterization shows that all iron(III) fumarate variants exhibit the metal–organic framework (MOF) structure of MIL-88A. Nanoparticles with a diameter of 50 nm were produced, which contain crystalline areas not exceeding 5 nm. Solvent-dependent swelling of the crystalline particles was monitored using in situ X-ray diffraction. Cytotoxicity experiments showed that all iron(III) fumarate variants feature adequate biotolerability and no distinct interference with cellular metabolism at low concentrations. Magnetic resonance relaxivity studies using clinical MRI equipment, on the other hand, proved that the MRI contrast characteristics depend on particle size and morphology. All in all, this study demonstrates the possibility of tuning the morphological appearance of iron(III) fumarate particles and illustrates the importance of optimizing synthesis conditions for the development of new biomedical materials.	Mar 2020
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF)	Synthesis and properties of a compositional series of MIL-53(Al) metal-organic framework crystal-glass composites Christopher W. Ashling , Duncan N. Johnstone , Remo N. Widmer , Jingwei Hou , Sean M. Collins , Adam F. Sapnik , Alice M. Bumstead , Philip A. Chater , David A. Keen , Thomas Bennett Journal Of The American Chemical Society DOI: 10.1021/jacs.9b07557 Diamond Proposal Number(s): [20038, 20195] Open Access Show Abstract ▼ Abstract: Metal-organic framework crystal-glass composites (MOF-CGCs) are materials in which a crystalline MOF is dispersed within a MOF glass. In this work, we explore the room temperature stabilization of the open-pore form of MIL-53(Al), usually observed at high-temperature, which occurs upon encapsulation within a ZIF-62(Zn) MOF glass matrix. A series of MOF-CGCs containing different loadings of MIL-53(Al) were synthesized and characterized using X-ray diffraction and nuclear magnetic resonance spectroscopy. An upper limit of MIL-53(Al) that can be stabilized in the composite was determined for the first time. The nanostructure of the composites was probed using pair distribution function analysis and scanning transmission electron microscopy. Notably, the distribution and integrity of the crystalline compo-nent in a sample series was determined, and these findings related to the MOF-CGC gas adsorption capacity in order to identify the optimal loading necessary for maximum CO2 sorption capacity.	Sep 2019
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF)	Metal-organic framework crystal-glass composites Jingwei Hou , Christopher W. Ashling , Sean M. Collins , Andraž Krajnc , Chao Zhou , Louis Longley , Duncan N. Johnstone , Philip Chater , Shichun Li , Marie-Vanessa Coulet , Philip L. Llewellyn , François-Xavier Coudert , David Keen , Paul A. Midgley , Gregor Mali , Vicki Chen , Thomas D. Bennett Nature Communications 10, 2580 DOI: 10.1038/s41467-019-10470-z Diamond Proposal Number(s): [171151, 19130, 16983] Open Access Show Abstract ▼ Abstract: The majority of research into metal-organic frameworks (MOFs) focuses on their crystalline nature. Recent research has revealed solid-liquid transitions within the family, which we use here to create a class of functional, stable and porous composite materials. Described herein is the design, synthesis, and characterisation of MOF crystal-glass composites, formed by dispersing crystalline MOFs within a MOF-glass matrix. The coordinative bonding and chemical structure of a MIL-53 crystalline phase are preserved within the ZIF-62 glass matrix. Whilst separated phases, the interfacial interactions between the closely contacted microdomains improve the mechanical properties of the composite glass. More significantly, the high temperature open pore phase of MIL-53, which spontaneously transforms to a narrow pore upon cooling in the presence of water, is stabilised at room temperature in the crystal-glass composite. This leads to a significant improvement of CO2 adsorption capacity.	Jun 2019
I15-1-X-ray Pair Distribution Function (XPDF)	Structural evolution in a melt-quenched zeolitic imidazolate framework glass during heat-treatment Jiayang Zhang , Louis Longley , Hao Liu , Christopher W. Ashling , Philip A. Chater , Kevin A. Beyer , Karena W. Chapman , Haizheng Tao , David A. Keen , Thomas D. Bennett , Yuanzheng Yue Chemical Communications DOI: 10.1039/C8CC09574D Diamond Proposal Number(s): [171151] Show Abstract ▼ Abstract: A pronounced enthalpy release occurs around 1.38 Tg in the prototypical metal-organic framework glass formed from ZIF-4 [Zn(C3H3N2)2], but there is no sign for any crystallization (i.e., long-range ordering) taking place. This behavior is in strong contrast to that for other families of melt-quenched glasses.	Feb 2019
I15-1-X-ray Pair Distribution Function (XPDF) I22-Small angle scattering & Diffraction	Metal-organic framework glasses with permanent accessible porosity Chao Zhou , Louis Longley , Andraž Krajnc , Glen J. Smales , Ang Qiao , Ilknur Erucar , Cara M. Doherty , Aaron W. Thornton , Anita J. Hill , Christopher W. Ashling , Omid T. Qazvini , Seok J. Lee , Philip A. Chater , Nicholas J. Terrill , Andrew J. Smith , Yuanzheng Yue , Gregor Mali , David A. Keen , Shane G. Telfer , Thomas D. Bennett Nature Communications 9 DOI: 10.1038/s41467-018-07532-z Diamond Proposal Number(s): [18236] Open Access Show Abstract ▼ Abstract: To date, only several microporous, and even fewer nanoporous, glasses have been produced, always via post synthesis acid treatment of phase separated dense materials, e.g. Vycor glass. In contrast, high internal surface areas are readily achieved in crystalline materials, such as metal-organic frameworks (MOFs). It has recently been discovered that a new family of melt quenched glasses can be produced from MOFs, though they have thus far lacked the accessible and intrinsic porosity of their crystalline precursors. Here, we report the first glasses that are permanently and reversibly porous toward incoming gases, without post-synthetic treatment. We characterize the structure of these glasses using a range of experimental techniques, and demonstrate pores in the range of 4 – 8 Å. The discovery of MOF glasses with permanent accessible porosity reveals a new category of porous glass materials that are elevated beyond conventional inorganic and organic porous glasses by their diversity and tunability.	Nov 2018
I15-1-X-ray Pair Distribution Function (XPDF)	Thermodynamic features and enthalpy relaxation in a metal–organic framework glass Chao Zhou , Malwina Stepniewska , Louis Longley , Christopher W. Ashling , Philip A. Chater , David Keen , Thomas D. Bennett , Yuanzheng Yue Physical Chemistry Chemical Physics 423 DOI: 10.1039/C8CP02340A Diamond Proposal Number(s): [171151] Show Abstract ▼ Abstract: In this work, we explore the thermodynamic evolution in a melt-quenched metal–organic framework glass, formed from ZIF-62 upon heating to the melting point (Tm), and subsequent enthalpy relaxation. The temperature dependence of the difference in Gibbs free energy between the liquid and crystal states of ZIF-62 in the temperature range from the glass transition temperature (Tg) to Tm is found to be weaker than those of other types of glasses, e.g., metallic glasses. Additionally, we find that the stretched exponent of the enthalpy relaxation function in the glass varies significantly (β = 0.44–0.76) upon changing the extent of sub-Tg annealing, compared to metallic and oxide glasses with similar Tgs, suggesting a high degree of structural heterogeneity. Pair distribution function results suggest no significant structural changes during the sub-Tg relaxation in ZIF-62 glass.	Jun 2018
I15-1-X-ray Pair Distribution Function (XPDF) I22-Small angle scattering & Diffraction	Liquid phase blending of metal-organic frameworks Louis Longley , Sean Collins , Chao Zhou , Glen J. Smales , Sarah E. Norman , Nick J. Brownbill , Christopher W. Ashling , Philip A. Chater , Robert Tovey , Carola-Bibiane Schönlieb , Thomas F. Headen , Nicholas J. Terrill , Yuanzheng Yue , Andrew J. Smith , Frédéric Blanc , David Keen , Paul A. Midgley , Thomas Bennett Nature Communications 9 DOI: 10.1038/s41467-018-04553-6 Diamond Proposal Number(s): [171151, 18236] Open Access Show Abstract ▼ Abstract: The liquid and glass states of metal–organic frameworks (MOFs) have recently become of interest due to the potential for liquid-phase separations and ion transport, alongside the fundamental nature of the latter as a new, fourth category of melt-quenched glass. Here we show that the MOF liquid state can be blended with another MOF component, resulting in a domain structured MOF glass with a single, tailorable glass transition. Intra-domain connectivity and short range order is confirmed by nuclear magnetic resonance spectroscopy and pair distribution function measurements. The interfacial binding between MOF domains in the glass state is evidenced by electron tomography, and the relationship between domain size and Tg investigated. Nanoindentation experiments are also performed to place this new class of MOF materials into context with organic blends and inorganic alloys.	Jun 2018

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