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76 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5, 6, 7, 8 [Next/Last]

Instruments / Technical Area	Publication Details	Published
I15-1-X-ray Pair Distribution Function (XPDF) I15-Extreme Conditions	Multiple local symmetries result in a common average polar axis in high-strain BiFeO3-based ceramics Ge Wang , Tengfei Hu , Wenxuan Zhu , Zhilun Lu , Annette Kleppe , Maria Diaz Lopez , Antonio Feteira , Derek C. Sinclair , Zhengqian Fu , Houbing Huang , Dawei Wang , Ian M. Reaney Physical Review Letters 130 DOI: 10.1103/PhysRevLett.130.076801 Diamond Proposal Number(s): [21714, 27500] Show Abstract ▼ Abstract: For the first time, the origin of large electrostrain in pseudocubic BiFeO 3 -based ceramics is verified with direct structural evidence backed by appropriate simulations. We employ advanced structural and microstructural characterizations of BiFeO 3 -based ceramics that exhibit large electrostrain ( > 0.4 % ) to reveal the existence of multiple, nanoscale local symmetries, dominantly tetragonal or orthorhombic, which have a common, averaged direction of polarization over larger, meso- or microscale regions. Phase-field simulations confirm the existence of local nanoscale symmetries, thereby providing a new vision for designing high-performance lead-free ceramics for high-strain actuators.	Feb 2023
I15-1-X-ray Pair Distribution Function (XPDF)	Study of a local structure at the interface between corrosion films and carbon steel surface in undersaturated CO2 environments Adriana Matamoros-Veloza , Tomasz M. Stawski , Silvia Vargas , Anne Neville Acs Omega DOI: 10.1021/acsomega.2c07631 Diamond Proposal Number(s): [20339] Open Access Show Abstract ▼ Abstract: Industries transporting CO2 gas-saturated fluids have infrastructures made of carbon steel. This is a good material with great mechanical properties but prone to corrosion and potential failure. Corrosion in sweet environments involves the formation of FeCO3 as a corrosion film, which is recognized to play a protective role under certain conditions. This work on the dissolution of corrosion films in sweet environments, under acidic and undersaturated conditions, demonstrates that the effects on the integrity of steel are far more significant than the damage observed on the surface of the corrosion film. Our results prove that dissolution of FeCO3 involved the presence of an amorphous phase, the intermediate formation of FeCl2 or FeCl+, and the presence of a phase with short distance atom–atom correlations. The amorphous phase was identified as a mixture of retained γ-Fe and Fe3C. Partially broken α-Fe and Fe3C structures were identified to prove the damage on the material, confirming the interface zone without evident damage on the corrosion film. Dissolution affected both the α-Fe and FeCO3, with the lattice [102̅] from the FeCO3 crystalline structure being the fastest to dissolve. The damage of steel at the molecular scale was evident at the macroscale with pit depths of up to 250 μm. The impact on the integrity of steel can be, therefore, more drastic than frequently reported in industrial operations of CO2 transport industries that use cleaning procedures (e.g., acid treatment, pigging) as part of their operational activities.	Feb 2023
I11-High Resolution Powder Diffraction I15-1-X-ray Pair Distribution Function (XPDF)	On the local structure in ordered and disordered closo-hydroborate solid electrolytes Paul Till , Ryo Asakura , Arndt Remhof , Wolfgang G. Zeier The Journal Of Physical Chemistry C 1413 DOI: 10.1021/acs.jpcc.2c07835 Diamond Proposal Number(s): [26379] Show Abstract ▼ Abstract: Na+closo-hydroborates are a heavily researched solid electrolyte class for applications in all-solid-state Na batteries. The structural characterization of these materials is notoriously challenging due to the elements involved and the fast rotational motion of hydroborate cages. The average structures obtained by Bragg diffraction have numerous atomic positions with low occupancies, complicating the determination of actual atom–atom distances. Total average scattering and derived pair distribution functions display atom–atom distances in real space, providing additional structure information to the average crystal structure. In this work, we present the pair distribution functions of the five different Na+closo-hydroborates: Na2B10H10, Na2B12H12, NaCB11H12, and the mixtures of 1:1 Na2B12H12/Na2B10H10 and 2:1 NaCB11H12/Na2B12H12. All pair distribution functions show a fast decay of peak height with increasing atom–atom distance on the local scale, suggesting a low correlation of atom motions between hydroborate cages, as observed in various other molecular crystals. The combination of Bragg diffraction, showing the average ordering of closo-hydroborate cages, and pair distribution function analysis, providing local atom–atom distances, is a useful tool to develop a deeper understanding of the closo-hydroborates and also of other plastic crystals.	Jan 2023
I15-1-X-ray Pair Distribution Function (XPDF)	Noncovalent bonding assessment by Pair Distribution Function Lucy K. Saunders , Daniel J. M. Irving , Philip A. Chater , Maria Diaz-Lopez Faraday Discussions DOI: 10.1039/D2FD00159D Open Access Show Abstract ▼ Abstract: Noncovalent interactions are essential in the formation and properties of a diverse range of materials. However, reliably identifying the noncovalent interactions remains challenging using conventional methods such as X-ray diffraction, especially in nanocrystalline, poorly crystalline or amorphous materials which lack long-range lattice periodicity. Here, we demonstrate the accurate determinations of deviations in the local structure and tilting of aromatic rings during the temperature-induced first order structural transition in the 1:1 adduct of 4,4’-bipyridinium squarate from low temperature form HAZFAP01 to high temperature HAZFAP07. This work demonstrates how Pair Distribution Function (PDF) analyses can improve our understanding of local structural deviations resulting from noncovalent bonds and guide the development of novel functional materials.	Jan 2023
I12-JEEP: Joint Engineering, Environmental and Processing	Revealing atomic structure evolution of an Al-1.5Fe alloy in the liquid state using X-ray total scattering and empirical potential structure refinement S. Huang , L. Qin , J. Zhao , K. Xiang , S. Luo , St. Michalik , J. Mi 6th International Conference on Advances in Solidification Processes (ICASP-6) DOI: 10.1088/1757-899X/1274/1/012007 Diamond Proposal Number(s): [27571] Open Access Show Abstract ▼ Abstract: We used in-situ real-time synchrotron X-ray total scattering and empirical potential structure refinement method to study the evolution of atomic structure of an Al-1.5Fe alloy melt from 750°C to 630 °C. Detailed data normalization and analyses for the total scattering data were presented in order to achieve sensible atomic structure simulation using the empirical potential structure refinement (EPSR) method with constraints of R-factor is <10-3. Reliable construction of 3D atomic structure of Al-Fe melt in the temperature range reveals that more Al atoms coordinate Fe atoms and the Fe-centered clusters get more compact with the temperature decreases. More systematic work linking the liquid structure to the nucleation structure is under way.	Jan 2023
I15-1-X-ray Pair Distribution Function (XPDF)	The influence of phase purity on the stability of Pt/LaAlO3 catalysts in the aqueous phase reforming of glycerol D. R. Inns , X. Pei , Z. Zhou , D. J. M. Irving , S. A. Kondrat Materials Today Chemistry 26 DOI: 10.1016/j.mtchem.2022.101230 Diamond Proposal Number(s): [29757] Open Access Show Abstract ▼ Abstract: Aqueous phase reforming (APR) of waste oxygenates offers the potential for sustainable hydrogen production. However, catalyst stability remains elusive, due to the aggressive hydrothermal conditions employed. Herein, we show that the catalytic performance and stability of Pt supported on LaAlO3 catalysts for glycerol APR is strongly influenced by the phase purity of LaAlO3. Calcination of the support at 700 °C produces the LaAlO3 perovskite phase and an amorphous lanthanum carbonate phase, which can be removed by calcination at higher temperature. Catalysts comprised of phase pure LaAlO3 were notably more active, with a support calcination temperature of 1100 °C resulting in 20.4% glycerol conversion (TOF 686 h−1) in a 2 h batch reaction. Interestingly, all the catalysts, regardless of LaAlO3 phase purity, eventually transform into Pt/LaCO3OH-AlO(OH) during reaction, but only in the presence of evolved carbon dioxide, itself produced from glycerol reforming. Studies using simulated reaction products showed that organic acid products (lactic acid), in the absence of CO2, facilitated La leaching and loss of crystallinity. A carbonate source (CO2) is essential to limit La leaching and form stable Pt/LaCO3OH. Pt supported on LaCO3OH and AlO(OH) are stable and active catalysts during APR reactions. Yet, the rate of perovskite phase decomposition strongly influences the final catalyst performance, with the initially phase impure LaAlO3 decomposing too quickly to facilitate Pt redistribution. LaAlO3 calcined at higher temperatures evolved more slowly and consequently produced more active catalysts.	Dec 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Local structure in α-BIMEVOXes (ME = Ge, Sn) Yajun Yue , Aleksandra Dzięgielewska , Man Zhang , Stephen Hull , Franciszek Krok , Richard M. Whiteley , Harold Toms , Marcin Malys , Xuankai Huang , Marcin Krynski , Ping Miao , Haixue Yan , Isaac Abrahams Chemistry Of Materials 12 DOI: 10.1021/acs.chemmater.2c03001 Diamond Proposal Number(s): [24348] Open Access Show Abstract ▼ Abstract: The BIMEVOXes are among the best oxide ion conductors at low and intermediate temperatures. Their high conductivity is associated with local defect structure. In this work, the local structures of two BIMEVOX compositions, Bi2V0.9Ge0.1O5.45 and Bi2V0.95Sn0.05O5.475, are examined using total neutron and X-ray scattering methods, with both compositions exhibiting the ordered α-phase at 25 °C and the disordered γ-phase at 700 °C. While the diffraction data for the α-phase do not allow for the polar (C2) and nonpolar (C2/m) structures to be readily distinguished, measurements of dielectric permittivity suggest the α-phase is weakly ferroelectric in character, consistent with calculations of spontaneous polarization based on a combination of density functional calculations and machine learning methodology. Reverse Monte Carlo (RMC) analysis of total scattering data reveals Ge preferentially adopts tetrahedral geometry at both temperatures, while Sn is found to predominantly adopt octahedral coordination in the α-phase and tetrahedral coordination in the γ-phase. In all cases, V polyhedra are found to consist of tetrahedral, pentacoordinate, and octahedral geometries, as also predicted by the crystallographic analysis and confirmed by 51V solid state NMR spectroscopy. Although similar long-range structures are observed at room temperature, the oxide ion vacancy distributions were found to be quite different between the two studied compositions, with a nonrandom deficiency in vacancy pairs in the second-nearest shell along the ⟨100⟩ tetragonal direction for BIGEVOX10, compared with a long-distance (>8.0 Å) ordering of equatorial vacancies for BISNVOX05. This is attributed to the differences in the preferred coordination geometries of the substituent cations in the two systems. Impedance spectroscopy measurements reveal both compositions show high conductivity in the order of 10–1 S cm–1 at 600 °C.	Dec 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Formation of a meltable purinate metal–organic framework and its glass analogue Alice M. Bumstead , Celia Castillo-Blas , Ignas Pakamore , Michael F. Thorne , Adam F. Sapnik , Ashleigh M. Chester , Georgina Robertson , Daniel J. M. Irving , Philip A. Chater , David A. Keen , Ross S. Forgan , Thomas D. Bennett Chemical Communications DOI: 10.1039/D2CC05314D Diamond Proposal Number(s): [20038] Open Access Show Abstract ▼ Abstract: The chemistries that can be incorporated within melt-quenched zeolitic imidazolate framework (ZIF) glasses are currently limited. Here we describe the preparation of a previously unknown purine-containing ZIF which we name ZIF-UC-7. We find that it melts and forms a glass at one of the lowest temperatures reported for 3D hybrid frameworks.	Dec 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Quantification of gas-accessible microporosity in metal-organic framework glasses Louis Frentzel-Beyme , Pascal Kolodzeiski , Jan-Benedikt Weiß , Andreas Schneemann , Sebastian Henke Nature Communications 13 DOI: 10.1038/s41467-022-35372-5 Diamond Proposal Number(s): [21604] Open Access Show Abstract ▼ Abstract: Metal-organic framework (MOF) glasses are a new class of glass materials with immense potential for applications ranging from gas separation to optics and solid electrolytes. Due to the inherent difficulty to determine the atomistic structure of amorphous glasses, the intrinsic structural porosity of MOF glasses is only poorly understood. Here, we investigate the porosity features (pore size and pore limiting diameter) of a series of prototypical MOF glass formers from the family of zeolitic imidazolate frameworks (ZIFs) and their corresponding glasses. CO2 sorption at 195 K allows quantifying the microporosity of these materials in their crystalline and glassy states, also providing excess to the micropore volume and the apparent density of the ZIF glasses. Additional hydrocarbon sorption data together with X-ray total scattering experiments prove that the porosity features of the ZIF glasses depend on the types of organic linkers. This allows formulating design principles for a targeted tuning of the intrinsic microporosity of MOF glasses. These principles are counterintuitive and contrary to those established for crystalline MOFs but show similarities to strategies previously developed for porous polymers.	Dec 2022
I15-1-X-ray Pair Distribution Function (XPDF)	Structure dependence of fracture toughness and ionic conductivity in lithium borophosphate glassy electrolytes for all-solid-state batteries Zhimin Chen , Tao Du , Søren S. Sørensen , Rasmus Christensen , Qi Zhang , Lars R. Jensen , Oxana Magdysyuk , Maria Diaz-Lopez , Mathieu Bauchy , Yuanzheng Yue , Morten M. Smedskjaer Journal Of Power Sources 553 DOI: 10.1016/j.jpowsour.2022.232302 Diamond Proposal Number(s): [30401] Open Access Show Abstract ▼ Abstract: Glass materials are potential candidates as solid electrolytes for batteries, but the atomistic origins of the variations in their properties and functionalities with composition are not well understood. Here, based on combined experimental and simulation techniques, we investigate the structural origin of the variation in fracture toughness and ionic conductivity of lithium borophosphate glass electrolytes with varying compositions. We focus on these properties since they are critically important for mechanical stability and electrochemical performances of glassy electrolytes. To this end, we have performed molecular dynamics simulations combined with X-ray total scattering experiments to provide the atomic picture of the disordered structure of borophosphate glass. The mechanical properties have been characterized through single-edge precracked beam measurements and axial tensile simulations. We find that the deformation and fracture behaviors of the electrolytes are governed by bond switching events of boron, which dissipate the strain energy during fracture. The migration of lithium ions in the electrolyte network is facilitated by hopping between superstructural rings, which reflects the important role of medium-range order structure in determining the lithium-ion diffusion. These findings have important implications for the design of future glassy electrolytes.	Nov 2022

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