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A series of high entropy AB₂-type Ti_2-xZr_xMnCrFeNi alloys (x = 0.6, 0.7, 0.8, 0.9, 1.0, 1.1 and 1.2) were synthesized to investigate their potential for hydrogen storage and chemical compression. The influence of the Ti/Zr ratio was explored in terms of structural, microstructural and thermodynamic properties. The storage capacity together with the reaction enthalpy and entropy changes of the synthesized high entropy alloys were compared to predictions from Machine Learning (ML) to investigate changes in these properties across the explored composition space. The results revealed that a decreasing Zr content consistently lowered the hydride formation enthalpy and increased the plateau pressure from 8 to >90 bar H₂ at 25 °C, in good agreement with ML predictions. Selected compositions (x = 1.0 and 1.2) demonstrated reversible hydrogen storage capability over 150 cycles, with capacities of 1.34–1.40 wt % H₂ and remarkable reaction kinetics (<4 min) at ambient temperature. These experimental and computational findings highlight the potential of this Laves-HEA system as tuneable, stable, and cost-effective materials suitable for long-term operations in stationary hydrogen storage and compression applications.

Online acoustic emission (AE) sensing is a promising nondestructive technique for battery health monitoring. Herein, we report on the ability of AE sensing to differentiate among different chemomechanical degradation events in a TiS2-based model aqueous chemistry. Short and high-frequency AE signals primarily stem from fracture-related degradation of TiS2, such as layer delamination, exfoliation, and cracking. Long and lowfrequency signals originate from gas bubbles bursting when the cell is cycled outside the water stability window. The two processes demonstrate distinct AE features, allowing them to be semi-quantitatively distinguished from both time and frequency domains. Complementary physicochemical characterizations have been conducted to correlate with the AE observation, including online electrochemical mass spectrometry, operando synchrotron X-ray diffraction, and ex situ scanning electron microscopy. Our work indicates that online AE sensing holds the promise to identify complex chemomechanical degradation processes in batteries with liquid and potentially solid electrolytes.

High-quality crystals of CoTeO₄ were grown by application of chemical vapor transport reactions in closed silica ampoules, starting from polycrystalline material in a temperature gradient 640 °C → 580 °C with TeCl₄ as transport agent. Crystal structure analysis of CoTeO₄ from single crystal X-ray data revealed a dirutile-type structure with Co^II and Te^VI atoms at crystallographically distinct sites, each with point group symmetry . The statistical significance and accuracy of the previously reported structural model based on powder data with the ordered arrangement of Co and Te cations was noticeably improved. CoTeO₄ does not undergo a structural phase transition upon heating, but decomposes stepwise (Co₂Te₃O₈ as intermediate phase) to Co₃TeO₆ as the only crystalline phase stable above 770 °C. Temperature-dependent magnetic susceptibility and dielectric measurements suggest antiferromagnetic ordering at ∼50 K. Optical absorption spectroscopy and computational studies reveal wide-band semiconductive behavior for CoTeO₄. The experimentally determined band gap of ∼2.42 eV is also found for CdS, which is frequently used in photovoltaic systems but is hazardous to the environment. Hence, CoTeO₄ might be a possible candidate to replace CdS in this regard.

Four new compositionally complex perovskites with multiple (four or more) cations on the B site of the perovskites have been studied. The materials have the general formula La_0.5Sr_2.5(M)₂O_7−δ (M = Ti, Mn, Fe, Co, and Ni) and have been synthesized via conventional solid-state synthesis. The compounds are the first reported examples of compositionally complex n = 2 Ruddlesden–Popper perovskites. The structure and properties of the materials have been determined using powder X-ray diffraction, neutron diffraction, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and magnetometry. The materials are isostructural and adopt the archetypal I4/mmm space group with the following unit cell parameters: a ∼ 3.84 Å, and c ∼ 20.1 Å. The measured compositions from energy dispersive X-ray spectroscopy were La_0.51(2)Sr_2.57(7)Ti_0.41(2)Mn_0.41(2)Fe_0.39(2)Co_0.38(1)Ni_0.34(1)O_7−δ, La_0.59(4)Sr_2.29(23)Mn_0.58(5)Fe_0.56(6)Co_0.55(6)Ni_0.42(4)O_7−δ, La_0.54(2)Sr_2.49(13)Mn_0.41(2)Fe_0.81(5)Co_0.39(3)Ni_0.36(3)O_7−δ, and La_0.53(4)Sr_2.55(19)Mn_0.67(6)Fe_0.64(5)Co_0.31(2)Ni_0.30(3)O_7−δ. No magnetic contribution is observed in the neutron diffraction data, and magnetometry indicates a spin glass transition at low temperatures.

Temperature-dependent dc-magnetization and ac-susceptibility curves have been recorded for series of single and double layered Ruddlesden-Popper multicomponent perovskites with chemical formula A₂BO₄ and A₃B₂O₇, respectively, with (La, Sr) on A-sites and up to 7 different cations on the B-sites (Ti, Cr, Mn, Fe, Co, Ni, Cu). The phase purity and chemical homogeneity of the compounds were investigated by X-ray diffraction and energy dispersive X-ray spectroscopy. Independently of the composition, spin glassiness is observed in both systems. Scaling analyses suggest the materials undergo spin glass phase transitions at low temperatures. Yet, qualitative differences are observed between the single-layered and double-layered systems, which are discussed in the light of the spatial dimensionality and magnetic interaction in layered oxide perovskites.

Giant magnetocaloric (GMC) materials constitute a requirement for near room temperature magnetic refrigeration. (Fe,Mn)₂(P,Si) is a GMC compound with strong magnetoelastic coupling. The main hindrance towards application of this material is a comparably large temperature hysteresis, which can be reduced by metal site substitution with a nonmagnetic element. However, the (Fe,Mn)₂(P,Si) compound has two equally populated metal sites, the tetrahedrally coordinated 3f and the pyramidally coordinated 3g sites. The magnetic and magnetocaloric properties of such compounds are highly sensitive to the site specific occupancy of the magnetic atoms. Here we have attempted to study separately the effect of 3f and 3g site substitution with equal amounts of vanadium. Using formation energy calculations, the site preference of vanadium and its influence on the magnetic phase formation are described. A large difference in the isothermal entropy change (as high as 44\%) with substitution in the 3f and 3g sites is observed. The role of the lattice parameter change with temperature and the strength of the magnetoelastic coupling on the magnetic properties are highlighted.

Single crystals of three novel transition-metal oxalates, dirubidium diaquadioxalatocobalt(II) dihydrate or dirubidium cobalt(II) bis(oxalate) tetrahydrate, Rb-2[Co(C2O4) (2)(H2O)(2)]similar to 2H(2)O, (I), catena-poly[dirubidium [[ dichloridocobalt(II)]-similar to-oxalato]] or dirubidium cobalt(II) dichloride oxalate, {Rb-2[CoCl2(C2O4)]}(n), (II), and poly[dipotassium [tri-similar to-oxalato-copper(II)dilithium] dihydrate] or dipotassium dilithium copper(II) tris(oxalate) dihydrate, {K-2[Li2Cu(C2O4)(3)]similar to 2H(2)O}n, (III), have been grown under hydrothermal conditions and their crystal structures determined using single-crystal X-ray diffraction. The structure of (I) exhibits isolated octahedral [Co(C2O4)(2)(H2O) (2)] units, whereas (II) consists of trans chains of Co2+ ions bridged by bidentate oxalato ligands and (III) displays a novel tri-periodic network of Li+ and Cu2+ ions linked by oxalato bridging ligands.

The ability to rapidly screen material performance in the vast space of high entropy alloys is of critical importance to efficiently identify optimal hydride candidates for various use cases. Given the prohibitive complexity of first principles simulations and large-scale sampling required to rigorously predict hydrogen equilibrium in these systems, we turn to compositional machine learning models as the most feasible approach to screen on the order of tens of thousands of candidate equimolar high entropy alloys (HEAs). Critically, we show that machine learning models can predict hydride thermodynamics and capacities with reasonable accuracy (e.g. a mean absolute error in desorption enthalpy prediction of ∼5 kJ mol_H2⁻¹) and that explainability analyses capture the competing trade-offs that arise from feature interdependence. We can therefore elucidate the multi-dimensional Pareto optimal set of materials, i.e., where two or more competing objective properties can't be simultaneously improved by another material. This provides rapid and efficient down-selection of the highest priority candidates for more time-consuming density functional theory investigations and experimental validation. Various targets were selected from the predicted Pareto front (with saturation capacities approaching two hydrogen per metal and desorption enthalpy less than 60 kJ mol_H2⁻¹) and were experimentally synthesized, characterized, and tested amongst an international collaboration group to validate the proposed novel hydrides. Additional top-predicted candidates are suggested to the community for future synthesis efforts, and we conclude with an outlook on improving the current approach for the next generation of computational HEA hydride discovery efforts.

The fundamental understanding of electrochemical reaction kinetics for lithium/sodium-ion batteries (LIBs & NIBs) is a significant criterion for advancing new-generation electrode materials. Herein, we demonstrate a novel lithium-rich perovskite oxalate KLi3Fe(C2O4)(3) (KLFC) cathode with the combination of cation and anion redox delivering discharge capacities of 86 and 99 mA h g(-1) after 100 cycles for a LIB and NIB, respectively, with good cyclability. Experimental Raman spectroscopy analysis combined with DFT calculations of charged/discharged samples illustrate the oxalate anion redox activity. Further, first-principles calculations of the partial density of states and Bader charges analysis have also characterised the redox behaviour and charge transfer during the potassium extraction processes.

A series of compounds with compositions Fe5Si1-xGexB2 were synthesised and their structural and magnetic properties were investigated. The Mo5SiB2-type structure with tetragonal I4/mcm space group is maintained for all compounds with x < 0.15, which is estimated as the compositional limit of the system. The unit cell pa-rameters expand with Ge content before reaching a plateau of a = 5.5581(1) and c = 10.3545(1) angstrom at x = 0.15. The saturation magnetisation (MS) decreased slightly with increasing Ge content whilst the magnetocrystalline anisotropy energy (MAE) remains almost unaffected. The Curie temperature for all compounds studied is at 790 K whilst the spin-reorientation temperature shows suppression from 172 K to 101 K where x = 0.15. Ab Initio calculations reveal an increase in MAE for compositions up to x = 0.25 and a decreased magnitude of MAE of-0.14 MJ/m3 for the hypothetical compound Fe5GeB2 relative to the parent compound Fe5SiB2.