Article
Chemistry, Multidisciplinary
Ida Gjerlevsen Nielsen, Sanna Sommer, Ann-Christin Dippel, Jorgen Skibsted, Bo Brummerstedt Iversen
Summary: The study directly determined the atomic structures of Ga3+ ion complexes in aqueous solutions across a wide range of pH, counter anions and concentrations using X-ray pair distribution function analysis and Ga-71 NMR. Different coordination structures of gallium ions were observed at different pH levels, with octahedral coordination dominating at low pH and polyoxogallate structures forming at slightly higher pH. The study provides valuable insights into the aqueous chemistry of Ga3+ ions with atomic resolution, relevant for semiconductor fabrication and medical applications.
Editorial Material
Multidisciplinary Sciences
Hui Chen, Hong-Jun Gao
Summary: Periodic waves of changing electron density are found to be more prevalent in different materials than previously thought, contributing to their ability to conduct electricity without resistance, according to four studies.
Article
Chemistry, Physical
V Cascos, L. Troncoso, A. Larralde, C. Alvarez-Galvan, M. T. Fernandez-Diaz, J. A. Alonso
Summary: In this research, two perovskite materials were prepared and tested as cathode materials for solid-oxide fuel cells, showing high power densities at 850 degrees C. The introduction of highly charged cations like Ir4+ and Ta5+ at the Co sites improved essential properties such as electrical conductivity and polarization resistances.
ACS APPLIED ENERGY MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Maxwell W. Terban, Simon J. L. Billinge
Summary: This article reviews the application of atomic pair distribution function (PDF) analysis in the study of molecular materials. The PDF method is a powerful tool for investigating short- and intermediate-range order in nanoscale materials. It can provide structural details that are obscured in reciprocal space by defects, disorder, or structural ambiguities. While its use in inorganic and nanomaterials research has been highlighted, significant progress has also been made in applying PDF analysis to molecular materials such as carbon, pharmaceuticals, polymers, liquids, coordination compounds, and composites. The article provides an overview of applications in a wide variety of molecular compounds and systems, and offers pedagogical descriptions and tips for implementation.
News Item
Multidisciplinary Sciences
Kelsey B. Hatzell, Maha Yusuf
Summary: The development of a promising type of battery is hindered by the growth of lithium filaments in the electrolyte, causing device failures. Investigating this failure mechanism may provide a solution. See p.287.
Review
Chemistry, Multidisciplinary
He Zhu, Yalan Huang, Jincan Ren, Binghao Zhang, Yubin Ke, Alex K. -Y. Jen, Qiang Zhang, Xun-Li Wang, Qi Liu
Summary: The correlation between structure and function is crucial in materials science and engineering. Modern functional materials often exhibit inhomogeneities at the atomic level, giving them unique properties related to electrons, phonons, and magnetic moments. The pair distribution function (PDF) technique has emerged as a powerful tool for detecting local structure away from average in functional materials, with the advancements in crystallographic techniques and the availability of synchrotron X-rays, spallation neutrons, and advanced computing power.
Article
Chemistry, Inorganic & Nuclear
Hector C. Mandujano, Melaku Sisay Tafere, Naveen Kumar Chogondahalli Muniraju, Tielyr D. Creason, Timothy M. McWhorter, Krzysztof Gofryk, Thomas W. Heitmann, Qiang Zhang, Bayram Saparov, Harikrishnan S. Nair
Summary: In this work, the Mn2SiX4 olivines (X=S, Se) were studied using magnetic susceptibility, X-ray and neutron diffraction. The crystal structures of Mn2SiS4 and Mn2SiSe4 were determined using synchrotron X-ray, neutron diffraction, and X-ray total scattering data. It was found that the Mn triangle forming the sawtooth lattice is isosceles in both compounds. The temperature evolution of magnetic susceptibility showed anomalies below 83 K and 70 K for Mn2SiS4 and Mn2SiSe4, respectively, indicating the presence of magnetic ordering. Neutron diffraction measurements revealed that the magnetic space groups of Mn2SiS4 and Mn2SiSe4 are Pnma and Pnm ' a ', respectively.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Seyed Sepehr Mohajerani, Francesco Ricci, Fredrik L. Nordstrom
Summary: The binary T-X phase diagram of salicylic acid and benzoic acid was experimentally determined, showing two crystalline solid solutions with solid-state miscibility limits of 10.9 mol% and 82.5 mol% benzoic acid in salicylic acid at 25 degrees Celsius. The eutectic composition of 60.0 mol% benzoic acid in salicylic acid at a eutectic temperature of 112.69 degrees Celsius was also determined. Non-linearity in the Tammann plot was observed due to the temperature dependence of the solvus and compositional non-uniformity in the material.
Article
Chemistry, Physical
Tiffany Kinnibrugh, Tim Fister
Summary: This study used total scattering approach to elucidate the evolving solvation structure of sulfuric acid solutions from 0-18M concentrations. A transition from octahedrally hydrated sulfates up to 6-7 M concentrations, followed by gradual dehydration was observed, reaching a solution structure similar to high acid concentrations water-in-salt electrolyte systems.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Multidisciplinary
Magnus Klove, Rasmus Stubkjaer Christensen, Ida Gjerlevsen Nielsen, Sanna Sommer, Mads Ry Vogel Jorgensen, Ann-Christin Dippel, Bo Brummerstedt Iversen
Summary: The structures of Zr4+ ions in solution were studied using X-ray pair distribution function (PDF) analysis. It was found that [Zr-4(OH)8(OH2)16]8+ tetramers are predominant in water, while monomeric complexes exist in non-aqueous solvents. The PDF analysis also revealed second sphere coordination of chloride counter ions to the aqueous tetramers.
Article
Chemistry, Multidisciplinary
Sandra Helen Skjaervo, Martin A. Karlsen, Riccardo Comin, Simon J. L. Billinge
Summary: This paper discusses the development of constraints for modelling pure octahedral tilts in perovskites, which helps disentangle the tilts from other structural distortions and provides stable refinements of the tilt components in real materials. The model in the program allows features in the PDF to be separated based on rigid tilts and non-rigid relaxations, giving researchers an intuitive picture of the tilting.
Article
Chemistry, Physical
Andreas Donni, Vladimir Y. Pomjakushin, Lei Zhang, Kazunari Yamaura, Alexei A. Belik
Summary: High-pressure synthesis was used to prepare (Ho1-xMnx)MnO3 solid solutions with x = 0.2 and 0.3, showing unique magnetic and structural properties with magnetization reversal behavior below the compensation temperature.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Review
Chemistry, Inorganic & Nuclear
Lei Gao, Jiangyang Pan, Longbang Di, Jinlong Zhu, Liping Wang, Song Gao, Ruqiang Zou, Le Kang, Songbai Han, Yusheng Zhao
Summary: This review article summarizes the progress of neutron diffraction in analyzing the structure and revealing the ionic transport mechanisms of antiperovskite solid-state electrolytes (SSEs). It introduces the structure-function relationships involved in ionic transport pathways, defect chemistry, anion disorder, and lattice dynamics. Additionally, possible future directions for the application of neutron diffraction in antiperovskite SSEs are suggested.
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Anita Zeidler, Philip S. Salmon, Takeshi Usuki, Shinji Kohara, Henry E. Fischer, Mark Wilson
Summary: The structure of molten NaCl was investigated using neutron and x-ray diffraction along with molecular dynamics simulations. The results showed that the rigid-ion approach matched the simple theory qualitatively, while the polarizable ion approach provided a good account of the diffraction results and agreed with experimental data.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Physics, Applied
Benjamin A. Frandsen, Raju Baral, Barry Winn, V. Ovidiu Garlea
Summary: This study reports the first example of obtaining magnetic pair distribution function (mPDF) data through neutron polarization analysis, showcasing high-quality mPDF data collected on an antiferromagnetic semiconductor. By applying ad hoc corrections to the data, significant improvement in data quality was demonstrated, providing insights into the potential for routine collection of high-quality mPDF data.
JOURNAL OF APPLIED PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Robert A. House, Helen Y. Playford, Ronald Smith, Jennifer Holter, Ian Griffiths, Ke-Jin Zhou, Peter G. Bruce
Summary: By presenting neutron PDF data, it was demonstrated that the charged O-redox cathode material contains molecular O-2, which could potentially increase the energy density of Li-ion batteries.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Shurong Yuan, Bernet E. Meijer, Guanqun Cai, Richard J. C. Dixey, Franz Demmel, Martin T. Dove, Jiaxun Liu, Helen Y. Playford, Helen C. Walker, Anthony E. Phillips
Summary: This study resolves the long-standing controversy on the origin of entropy change in ammonium sulfate, a simple inorganic salt. It shows that the entropy arises from low-frequency librations of ammonium ions, suggesting that vibrational entropy is equally important as configurational entropy in the search for molecular materials with large entropy changes.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Victor Krayzman, Alexei Bosak, Helen Y. Playford, Bruce Ravel, Igor Levin
Summary: The nanoscale structure of Sr0.61Ba0.39Nb2O6 with incommensurate modulation is determined using atomistic refinements. The modulation arises from the intergrowth of structural slabs with distinct types of octahedral rotations. The polar displacements of Nb are not affected by this modulation. Competing polar and antipolar modes are observed above the ferroelectric transition temperature, but suppressed below it. The coupling between the polar off-centering of Nb controls the ferroelectric-to-relaxor crossover in TTBs.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Reza J. J. Kashtiban, Christopher E. E. Patrick, Quentin Ramasse, Richard I. I. Walton, Jeremy Sloan
Summary: Halide perovskite structures formed at the quantum scale are revolutionizing optoelectronic materials design, such as solar cells and light-emitting diodes. Four sub-nanometer halide perovskite structures were successfully created inside single-walled carbon nanotubes, demonstrating unique properties and bandgap widening compared to bulk forms. These structures show promise in the development of advanced optoelectronic devices.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Satarupa Das, Jinfang Zhang, Thomas W. Chamberlain, Guy J. Clarkson, Richard I. Walton
Summary: CO2 epoxidation to cyclic carbonates under mild, solvent-free conditions is a promising pathway for sustainable CO2 utilization. However, previous metal-organic frameworks (MOFs) used for this purpose are not suitable for commercial utilization due to the nonrenewable ligands used. This study presents new yttrium MOFs based on renewable 2,5-furandicarboxylate (FDC) ligands, which exhibit high catalytic activity and conversion efficiency for CO2 epoxidation reactions.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Yongzhao Zhang, Baiwen Zhao, Satarupa Das, Volkan Degirmenci, Richard L. I. Walton
Summary: This study focuses on the synthesis of metal-organic frameworks with the UiO-66 structure and their use as catalysts for optimizing HMF yield. The materials exhibit high catalytic performance in DMSO solvent and can achieve high conversion and yield under optimized reaction conditions.
Article
Chemistry, Inorganic & Nuclear
Lu Jia, Matthew D. Lloyd, Martin R. Lees, Limin Huang, Richard I. Walton
Summary: In this study, the crystallization of a new series of A-site substituted lanthanum ferrite materials (La1-xREx)FeO3 was explored using hydrothermal method. The effect of elemental substitution on the morphological, structural, and magnetic properties of the materials was studied. It was found that homogeneous solid solutions are formed when La3+ and substituent ions have similar radii, while crystallization in separate phases is found when there is a large radius difference. A-site replacement induces an evolution in the crystallite shape, providing evidence for a phase-separation-driven evolution of morphology.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
S. C. H. Llewelyn, L. R. Owen, H. Y. Playford, N. G. Jones, D. Dye, M. C. Hardy, H. J. Stone
Summary: This study examined the effects of Ni:Co ratio variation on the lattice misfit of NiCo-5Al-5Ti-15Cr alloys over a wide temperature range. Different alloy compositions were prepared and aged at 800 degrees C, and neutron diffraction was used to determine the lattice parameters. The results showed that the lattice misfit decreased with increasing temperature for alloys with Co content of 0-47 at%, and the misfit increased systematically with increasing Co content up to 38 at%. The alloy with 47Co exhibited lower misfit values than the 38Co alloy at temperatures up to 700 degrees C.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Nanoscience & Nanotechnology
Aron Summer, Helen Y. Playford, Lewis R. Owen, Janet M. Fisher, Amy Kolpin, David Thompsett, Richard I. Walton
Summary: Reverse Monte Carlo analysis was performed on neutron and x-ray total scattering data from two ceria-zirconia samples to analyze the distribution of cations and examine oxide-ion disorder. The first sample heated in air at moderate conditions showed a single-phase solid-solution structure with statistical distribution of cations, but a local tetragonal symmetry was observed. The second sample heated under H-2 followed by reoxidation exhibited considerable disorder and a non-statistical distribution of cations, indicating the presence of cation-rich nano-domains.
Article
Chemistry, Physical
Yulia M. T. A. Putri, Thomas W. Chamberlain, Volkan Degirmenci, Jarnuzi Gunlazuardi, Yuni K. Krisnandi, Richard I. Walton, Tribidasari A. Ivandini
Summary: This study proposes NiCo-MOF-74 synthesized directly on the surface of porous NiO film as an efficient electrocatalyst for the anode in direct urea fuel cells. The nickel-to-cobalt ratio of 4:1 exhibits the best catalytic activity towards urea oxidation, resulting in significant current enhancement compared to other electrodes. At optimized conditions, a current density of approximately 110 mA cm-2 and a maximum power density of 4131 mu W cm-2 can be achieved in an electrolyte solution of 3.0 M KOH and 1.0 M urea. The increased active surface area of the nickel-based anodes contributes to an abundance of active sites for urea oxidation, leading to excellent stability and reproducibility over 15 hours of application in a direct urea fuel cell.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Electrochemistry
Evangeline C. Wheeler-Jones, Melanie J. Loveridge, Richard I. Walton
Summary: A composite of Nb2O5 and MoO2 was synthesized and demonstrated as a high-capacity, high-rate anode for lithium-ion batteries. The composite showed an intimate mix of individual oxide particles, and a ratio of Nb : Mo of 45: 55. It exhibited notable rate capability and achieved a stable reversible capacity of 514 mAh g(-1), realizing its theoretical capacity.
BATTERIES & SUPERCAPS
(2023)
Article
Chemistry, Physical
Rita Mendes Da Silva, Anita Zeidler, Hesameddin Mohammadi, Lawrence V. D. Gammond, Esther Giron Lange, Randall E. Youngman, Bruce G. Aitken, Alex C. Hannon, Chris J. Benmore, Gavin B. M. Vaughan, Philip S. Salmon
Summary: The structure of zinc aluminosilicate glasses with a wide composition range was investigated using neutron and high-energy x-ray diffraction and Al-27 magic angle spinning nuclear magnetic resonance spectroscopy. The results revealed a composition-dependent structure, where four-coordinated aluminum atoms were dominant and zinc played a role as both a network modifier and charge compensator. The coordination environment of zinc varied systematically with the glass composition, influencing the coordination number and bond distance.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Fayan Zhu, Daniel. T. T. Bowron, Sabrina Gartner, Chunhui Fang, Yongquan Zhou, Hongyan Liu, Alex. C. C. Hannon
Summary: H/D isotopic substitution neutron diffraction was used in combination with EPSR and DFT-based quantum calculations to investigate the interactions in borate solutions. The solute ions and molecules were found to significantly affect the structure of water molecules, leading to a deviation from tetrahedral structure. Potassium ions formed various ion pairs with B(OH)3, and the composition of these ion pairs changed with solution concentration. Boric acid molecules showed different hydration preferences, with direct hydration being the most energetically favorable.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Review
Chemistry, Physical
Gabriel E. Perez, Jake M. Brittain, Innes McClelland, Stephen Hull, Martin O. Jones, Helen Y. Playford, Serena A. Cussen, Peter J. Baker, Emily M. Reynolds
Summary: Neutron and muon characterisation techniques have unique capabilities for studying the complex structure and dynamics of rechargeable battery systems. The neutron's interaction with atomic nuclei enables it to detect light elements and its weak interaction allows it to penetrate deep into the sample, while the non-invasive nature of the implanted positive muon makes it a probe for studying ionic diffusion phenomena at different depths. This review discusses the application of these techniques in ion battery research and provides an accessible overview of their working principles.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)