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28 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I15-1-X-ray Pair Distribution Function (XPDF)	Glassy behaviour of mechanically amorphised ZIF-62 isomorphs Michael F. Thorne , Adam F. Sapnik , Lauren N. Mchugh , Alice M. Bumstead , Celia Castillo-Blas , Dean S. Keeble , Maria Diaz-Lopez , Philip A. Chater , David A. Keen , Thomas D. Bennett Chemical Communications DOI: 10.1039/D1CC03469C Diamond Proposal Number(s): [20038] Open Access Show Abstract ▼ Abstract: Zeolitic imidazolate frameworks (ZIFs) can be melt-quenched to form glasses. Here, we present an alternative route to glassy ZIFs via mechanically induced amorphisation. This approach allows various glassy ZIFs to be produced in under 30 minutes at room temperature, without the need for melt-quenching.	Aug 2021
I15-Extreme Conditions	The correlation between X-ray scattering structure factor and shear bands density of a metallic glass and a composite C. Zhang , T.-L. Lee , J. C. Khong , J.c. Qiao , D. Daisenberger , Y. Yao , J. Mi Materials Letters 304 DOI: 10.1016/j.matlet.2021.130727 Diamond Proposal Number(s): [9902, 8858] Show Abstract ▼ Abstract: The tensile fractured surfaces of ZrTi-based bulk metallic glass and composite samples were studied using synchrotron X-ray total scattering. The scanned areas contain different shear bands densities. The shear bands create localized atomic strains, which in turn cause more ordered atomic structures. Such structural changes were reflected in the scattering structure factor, i.e. the higher the density of the shear bands, the higher the scattering structure factor. Similar phenomenon was also found in the metallic glass composite.	Aug 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Polymethylaluminoxane organic frameworks (sMAOF) – highly active supports for slurry phase ethylene polymerisation Alexander F. R. Kilpatrick , Harry S. Geddes , Zoe R. Turner , Jean-Charles Buffet , Andrew L. Goodwin , Dermot O'Hare Catalysis Science & Technology 15 DOI: 10.1039/D1CY00767J Diamond Proposal Number(s): [16072, 19128] Open Access Show Abstract ▼ Abstract: A series of modified solid polymethylaluminoxane (sMAO) catalyst supports have been developed for slurry phase ethylene polymerisation, using aryl di-ol modifier groups. Characterisation using ICP-MS analysis, X-ray total scattering, SEM–EDX, diffuse FT-IR and solid state NMR spectroscopy shows that the organic linker groups are uniformly distributed in a proposed organic framework stucture we call a “sMAOF”. When used as a support for rac-ethylene{bis(1-indenyl)} zirconium dichloride, (EBI)ZrCl2, these linker modified sMAOF materials provide a 40% enhancement in polymerisation activity with respect to unmodified sMAO: activities of 163 × 103 and 116 × 103 kgPE molZr−1 h−1 at 80 °C for (EBI)ZrCl2 supported on sMAOF(1,4-HO(C6F4)OH) and sMAO, respectively. The observed activity increase is correlated with the higher BET surface area and increased porosity in the linker modified sMAOF activating support.	Jul 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Frustrated flexibility in metal-organic frameworks Roman Pallach , Julian Keupp , Kai Terlinden , Louis Frentzel-Beyme , Marvin Kloß , Andrea Machalica , Julia Kotschy , Suresh K. Vasa , Philip A. Chater , Christian Sternemann , Michael T. Wharmby , Rasmus Linser , Rochus Schmid , Sebastian Henke Nature Communications 12 DOI: 10.1038/s41467-021-24188-4 Diamond Proposal Number(s): [15895, 21262, 21604] Open Access Show Abstract ▼ Abstract: Stimuli-responsive flexible metal-organic frameworks (MOFs) remain at the forefront of porous materials research due to their enormous potential for various technological applications. Here, we introduce the concept of frustrated flexibility in MOFs, which arises from an incompatibility of intra-framework dispersion forces with the geometrical constraints of the inorganic building units. Controlled by appropriate linker functionalization with dispersion energy donating alkoxy groups, this approach results in a series of MOFs exhibiting a new type of guest- and temperature-responsive structural flexibility characterized by reversible loss and recovery of crystalline order under full retention of framework connectivity and topology. The stimuli-dependent phase change of the frustrated MOFs involves non-correlated deformations of their inorganic building unit, as probed by a combination of global and local structure techniques together with computer simulations. Frustrated flexibility may be a common phenomenon in MOF structures, which are commonly regarded as rigid, and thus may be of crucial importance for the performance of these materials in various applications.	Jul 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Liquid structure and dynamics in the choline acetate:urea 1:2 deep eutectic solvent Alessandro Triolo , Maria Enrica Di Pietro , Andrea Mele , Fabrizio Lo Celso , Martin Brehm , Valerio Di Lisio , Andrea Martinelli , Philip Chater , Olga Russina The Journal Of Chemical Physics 154 DOI: 10.1063/5.0054048 Diamond Proposal Number(s): [27222] Open Access Show Abstract ▼ Abstract: We report on the thermodynamic, structural, and dynamic properties of a recently proposed deep eutectic solvent, formed by choline acetate (ChAc) and urea (U) at the stoichiometric ratio 1:2, hereinafter indicated as ChAc:U. Although the crystalline phase melts at 36–38 °C depending on the heating rate, ChAc:U can be easily supercooled at sub-ambient conditions, thus maintaining at the liquid state, with a glass–liquid transition at about −50 °C. Synchrotron high energy x-ray scattering experiments provide the experimental data for supporting a reverse Monte Carlo analysis to extract structural information at the atomistic level. This exploration of the liquid structure of ChAc:U reveals the major role played by hydrogen bonding in determining interspecies correlations: both acetate and urea are strong hydrogen bond acceptor sites, while both choline hydroxyl and urea act as HB donors. All ChAc:U moieties are involved in mutual interactions, with acetate and urea strongly interacting through hydrogen bonding, while choline being mostly involved in van der Waals mediated interactions. Such a structural situation is mirrored by the dynamic evidences obtained by means of 1H nuclear magnetic resonance techniques, which show how urea and acetate species experience higher translational activation energy than choline, fingerprinting their stronger commitments into the extended hydrogen bonding network established in ChAc:U.	Jun 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Evolution of the local structure in the sol–gel synthesis of Fe3C nanostructures Matthew S. Chambers , Dean S. Keeble , Dean Fletcher , Joseph A. Hriljac , Zoe Schnepp Inorganic Chemistry 52 DOI: 10.1021/acs.inorgchem.0c03692 Diamond Proposal Number(s): [15959] Open Access Show Abstract ▼ Abstract: The sol–gel synthesis of iron carbide (Fe3C) nanoparticles proceeds through multiple intermediate crystalline phases, including iron oxide (FeOx) and iron nitride (Fe3N). The control of particle size is challenging, and most methods produce polydisperse Fe3C nanoparticles of 20–100 nm in diameter. Given the wide range of applications of Fe3C nanoparticles, it is essential that we understand the evolution of the system during the synthesis. Here, we report an in situ synchrotron total scattering study of the formation of Fe3C from gelatin and iron nitrate sol–gel precursors. A pair distribution function analysis reveals a dramatic increase in local ordering between 300 and 350 °C, indicating rapid nucleation and growth of iron oxide nanoparticles. The oxide intermediate remains stable until the emergence of Fe3N at 600 °C. Structural refinement of the high-temperature data revealed local distortion of the NFe6 octahedra, resulting in a change in the twist angle suggestive of a carbonitride intermediate. This work demonstrates the importance of intermediate phases in controlling the particle size of a sol–gel product. It is also, to the best of our knowledge, the first example of in situ total scattering analysis of a sol–gel system.	May 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Melting of hybrid organic–inorganic perovskites Bikash Kumar Shaw , Ashlea R. Hughes , Maxime Ducamp , Stephen Moss , Anup Debnath , Adam F. Sapnik , Michael F. Thorne , Lauren N. Mchugh , Andrea Pugliese , Dean S. Keeble , Philip Chater , Juan M. Bermudez-Garcia , Xavier Moya , Shyamal K. Saha , David A. Keen , François-Xavier Coudert , Frédéric Blanc , Thomas Bennett Nature Chemistry 119 DOI: 10.1038/s41557-021-00681-7 Diamond Proposal Number(s): [20038] Show Abstract ▼ Abstract: Several organic–inorganic hybrid materials from the metal–organic framework (MOF) family have been shown to form stable liquids at high temperatures. Quenching then results in the formation of melt-quenched MOF glasses that retain the three-dimensional coordination bonding of the crystalline phase. These hybrid glasses have intriguing properties and could find practical applications, yet the melt-quench phenomenon has so far remained limited to a few MOF structures. Here we turn to hybrid organic–inorganic perovskites—which occupy a prominent position within materials chemistry owing to their functional properties such as ion transport, photoconductivity, ferroelectricity and multiferroicity—and show that a series of dicyanamide-based hybrid organic–inorganic perovskites undergo melting. Our combined experimental–computational approach demonstrates that, on quenching, they form glasses that largely retain their solid-state inorganic–organic connectivity. The resulting materials show very low thermal conductivities (~0.2 W m−1 K−1), moderate electrical conductivities (10−3–10−5 S m−1) and polymer-like thermomechanical properties.	May 2021
E02-JEM ARM 300CF I15-1-X-ray Pair Distribution Function (XPDF) I22-Small angle scattering & Diffraction	Mixed hierarchical local structure in a disordered metal–organic framework Adam F. Sapnik , Irene Bechis , Sean M. Collins , Duncan N. Johnstone , Giorgio Divitini , Andrew J. Smith , Philip A. Chater , Matthew A. Addicoat , Timothy Johnson , David A. Keen , Kim E. Jelfs , Thomas D. Bennett Nature Communications 12 DOI: 10.1038/s41467-021-22218-9 Diamond Proposal Number(s): [20038, 24563] Open Access Show Abstract ▼ Abstract: Amorphous metal–organic frameworks (MOFs) are an emerging class of materials. However, their structural characterisation represents a significant challenge. Fe-BTC, and the commercial equivalent Basolite® F300, are MOFs with incredibly diverse catalytic ability, yet their disordered structures remain poorly understood. Here, we use advanced electron microscopy to identify a nanocomposite structure of Fe-BTC where nanocrystalline domains are embedded within an amorphous matrix, whilst synchrotron total scattering measurements reveal the extent of local atomic order within Fe-BTC. We use a polymerisation-based algorithm to generate an atomistic structure for Fe-BTC, the first example of this methodology applied to the amorphous MOF field outside the well-studied zeolitic imidazolate framework family. This demonstrates the applicability of this computational approach towards the modelling of other amorphous MOF systems with potential generality towards all MOF chemistries and connectivities. We find that the structures of Fe-BTC and Basolite® F300 can be represented by models containing a mixture of short- and medium-range order with a greater proportion of medium-range order in Basolite® F300 than in Fe-BTC. We conclude by discussing how our approach may allow for high-throughput computational discovery of functional, amorphous MOFs.	Apr 2021
I15-Extreme Conditions	The mediation of bond strain by vacancies and displacive disorder in A-site-deficient perovskites I. Levin , V. Krayzman , H. Y. Playford , J. C. Woicik , R. Maier , Z. Lu , A. Bruma , M. Eremenko , M. G. Tucker Acta Materialia 7 DOI: 10.1016/j.actamat.2021.116678 Diamond Proposal Number(s): [16168] Show Abstract ▼ Abstract: Local distortions in perovskite-like A-site-deficient (Sr,La)TiO3 solid solutions have been determined by refining large-scale atomic configurations against neutron/X-ray total-scattering and extended-X-ray-absorption-fine-structure data. Structural relaxations in this system are driven by the competing bonding requirements of Sr, La, and the undercoordinated oxygen atoms that surround vacant A-sites, which form upon substitution of La for Sr. La cations exhibit significant, disordered off-center displacements within their oversized oxygen cages required by the larger Sr cations. The resulting split-site probability density distributions of La vary with the Sr/La ratio and the state of the A-site ordering, which together modify the structure's ability to relieve the tensile bond strain around La through octahedral rotation and displacements of oxygens surrounding the vacancies. The displacive disorder of La can provide a hitherto overlooked mechanism for reducing the thermal conductivity, which is relevant to thermoelectric properties of this system. A comparison of the local structural behaviors in (Sr,La)TiO3 and the previously studied (Na,Bi)NbO3 solid solutions permits generalizations about A-site deficient perovskites. We find that A-site vacancies provide the nearest-neighbor oxygens with a degree of freedom to mediate the strain in the system, and their effects on local structural relaxations are determined by cation chemistry and stoichiometry.	Jan 2021
I15-1-X-ray Pair Distribution Function (XPDF)	Metal-organic framework and inorganic glass composites Louis Longley , Courtney Calahoo , René Limbach , Yang Xia , Joshua M. Tuffnell , Adam F. Sapnik , Michael F. Thorne , Dean S. Keeble , David A. Keen , Lothar Wondraczek , Thomas D. Bennett Nature Communications 11 DOI: 10.1038/s41467-020-19598-9 Diamond Proposal Number(s): [20038] Open Access Show Abstract ▼ Abstract: Metal-organic framework (MOF) glasses have become a subject of interest as a distinct category of melt quenched glass, and have potential applications in areas such as ion transport and sensing. In this paper we show how MOF glasses can be combined with inorganic glasses in order to fabricate a new family of materials composed of both MOF and inorganic glass domains. We use an array of experimental techniques to propose the bonding between inorganic and MOF domains, and show that the composites produced are more mechanically pliant than the inorganic glass itself.	Nov 2020

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