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621 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
I09-Surface and Interface Structural Analysis I11-High Resolution Powder Diffraction	Boosting initial coulombic efficiency in Li-rich Mn-based cathodes by tuning orbital hybridization Tao Zeng , Ziqin Jiao , Xiaoyu Gao , Maolin Yang , Xiaohu Wang , Wenguang Zhao , Wei Tang , Mihai Chu , Ze He , Jinqi Li , Zhongyuan Huang , Guojie Chen , Ziwei Chen , Rui Wang , Liming Wang , Junrong Zhang , Lunhua He , Yuguang Pu , Yinguo Xiao Angewandte Chemie International Edition DOI: 10.1002/anie.202501777 Diamond Proposal Number(s): [36187, 34243] Show Abstract ▼ Abstract: Li-rich manganese-based oxides (LRMO) are promising cathode materials for next-generation lithium-ion batteries due to their high-capacity and low-cost merits. However, the low initial coulombic efficiency (ICE) and irreversible oxygen release of LRMO severely hinder their commercialization processes. Here, we employ glyoxal treatment to modulate the hybridization between transition metal (TM) 3d and oxygen (O) 2p orbitals in LRMO. This approach is found to reduce the Co/Mn t2g-O 2p hybridization in LRMO while simultaneously activating the Co2+/Co3+ redox below the Fermi level. Our findings demonstrate that tuning TM 3d-O 2p orbital hybridization can be a viable approach to improve the ICE of LMRO. Specifically, the ICE of LRMO can be elevated from 85.3 % to 102.5 %, and a high specific capacity of 291.2 mAh g−1 can be achieved at 0.1 C. Moreover, the treated LRMO cathodes exhibit significantly enhanced capacity retention.	May 2025
B18-Core EXAFS E02-JEM ARM 300CF	Catalytic ultrasound-driven synthesis of syngas from CO2 saturated water Lina Chen , Yi Qin , Claire T. Coulthard , Zoe R. Turner , Chunping Chen , James Kwan , Dermot O'Hare Energy & Environmental Science 458 DOI: 10.1039/D5EE01202C Diamond Proposal Number(s): [34632] Open Access Show Abstract ▼ Abstract: Conventional catalytic CO2 reduction into value-added products often encounters challenges such as high energy barriers and complex operational setups. Here, we introduce a sonocatalysis approach to CO2 reduction in water under ambient conditions. In an acoustic cavitation-induced high-energy local environment, the Cu nanoparticles incorporated on the ZnAl-layered double oxide create a favorable energy barrier for CO2 reduction in water, a CO production rate of 23.8 μmolCO g−1 h−1 with over 85% selectivity was achieved by ultrasonic irradiation of a CO2-saturated aqueous solution at room temperature. Furthermore, more acoustic cavitation was produced with 5% CO2 in argon dissolved in water, resulting in a higher CO productivity of 252.7 μmolCO g−1 h−1, 11 times larger than pure CO2. Hydrogen production also increased with acoustic cavitation, creating a syngas mixture with a CO to H2 ratio of 1.2 to 2.2. This approach produces a high sonochemical efficiency of 211.1 μmol kJ−1 g−1 L−1 for the ultrasound-driven fuel production from CO2 and water. These results highlight the use of cavitation to provide an alternative approach to CO2 conversion.	May 2025
B18-Core EXAFS	Enhanced dry reforming of methane over nickel catalysts supported on zirconia coated mesoporous silica Yi Zhong , Yuhao Peng , Hao Gu , Shan Zhang , Feng Ryan Wang , Wei Xiao , Hulei Yu , Dong Gu Iscience DOI: 10.1016/j.isci.2025.112582 Diamond Proposal Number(s): [36367] Open Access Show Abstract ▼ Abstract: Dry reforming of methane (DRM) offers a sustainable route to convert CH4 and CO2 into syngas, addressing both greenhouse gas emissions and energy demand. However, catalyst deactivation due to sintering and coking limits practical applications. In this work, we developed a mesoporous Ni-based catalyst (Ni/ZrSBA-15-OH) featuring abundant Ni-ZrO2 interfaces and small Ni nanoparticles (5.6 nm) confined within a stable silica framework. This catalyst showed excellent performance, achieving 80% CH4 and 87% CO2 conversions at 750 °C, with minimal coke formation (0.4 mg gcat-1 h-1) and high durability (1.3% CH4 conversion loss over 20 hours). Advanced characterizations (XAS, TEM, H2-TPR, and TPSR) revealed that the metal-oxide interface enhances the activation of reactants and stabilizes active sites. DFT calculations confirmed that the Ni-ZrO2 interface increases the energy barrier for CH* dehydrogenation, effectively suppressing carbon deposition. This study provides a rational strategy for designing structurally robust and coke-resistant Ni-based catalysts for efficient DRM.	May 2025
E02-JEM ARM 300CF	Low pressure amide hydrogenation enabled by magnetocatalysis Sheng-Hsiang Lin , Sihana Ahmedi , Aaron Kretschmer , Carlotta Campalani , Yves Kayser , Liqun Kang , Serena Debeer , Walter Leitner , Alexis Bordet Nature Communications 16 DOI: 10.1038/s41467-025-58713-6 Diamond Proposal Number(s): [35866] Open Access Show Abstract ▼ Abstract: The catalytic hydrogenation of amides with molecular hydrogen (H2) is an appealing route for the synthesis of valuable amines entering in the preparation of countless organic compounds. Running effective amide hydrogenation under mild H2 pressures is challenging although desirable to preclude the need for specialized high-pressure technologies in research and industry. Here we show that magnetocatalysis with standard supported catalysts enables unprecedented amide hydrogenation at mild conditions. Widely available and commercial platinum on alumina (Pt/Al2O3) was functionalized with iron carbide nanoparticles (ICNPs) to allow for localized and rapid magnetic induction heating resulting in the activation of neighboring Pt sites by thermal energy transfer. Exposure of the ICNPs@Pt/Al2O3 catalyst to an alternating current magnetic field enables highly active and selective hydrogenation of a range of amides at a reactor temperature of 150 °C under 3 bar or even ambient pressure of H2. ICNPs@Pt/Al2O3 reacts adaptively to fluctuations in electricity supply mimicking the use of intermittent renewable energy sources. This work may pave the way toward a greatly enhanced practicability of amide hydrogenation at the laboratory and production scales, and demonstrates more generally the broad potential of the emerging field of magnetocatalysis for synthetic chemistry.	Apr 2025
B18-Core EXAFS	Polysaccharide-derived sulfur-containing mesoporous carbon materials for platinum group metal recovery Nicholas Garland , Ross Gordon , Iain Hopkins , Ewan Ward , Con Robert Mcelroy , Duncan Macquarrie , Alison Parkin Carbon 10 DOI: 10.1016/j.carbon.2025.120309 Show Abstract ▼ Abstract: As cost effective and sustainable materials for the recovery of platinum and palladium we have investigated the potential of sulfur-containing porous carbon materials. Utilising the naturally abundant sulfur-containing κ-carrageenan, or by doping K2SO4 into alternative polysaccharides (i.e. alginic acid), the Starbon process provides a sustainable route to high surface area mesoporous materials without the need for templates or activating agents. X-ray diffraction, elemental analysis and X-ray photoelectron spectroscopy were used to elucidate the development of sulfur chemistry during pyrolysis so that conditions could be optimised to yield materials with significant quantities of reduced organic sulfur chemistry, considered most promising for platinum group metal adsorption. The resulting materials were found to exhibit large capacities for Pd(II) (156 mg.g-1) and Pt(II) (246 mg.g-1) as well as selectivity over the other platinum group metals and the common contaminant ions Cu(II), Ni(II) and Co(II) in large excess. Pd(II) and Pt(II) could be removed by elution in thiourea and the material reused, suggesting excellent potential for the application of these materials to the recovery of platinum and palladium from low grade feeds. Analysis of adsorbed palladium using X-ray photoelectron and X-ray absorption spectroscopies provides evidence for coordination to organic sulfur-containing groups on the Starbon surface.	Apr 2025
B18-Core EXAFS	Multimetallic layered double hydroxides as efficient and durable oxygen evolution catalysts for anion exchange membrane water electrolysis at high current densities Yaowen Xu , Kaiyang Xu , Hao Tan , Haoliang Huang , Fei Lin , Chenyue Zhang , Jingwei Wang , Run Ran , Zhipeng Yu , Sitaramanjaneya Mouli Thalluri , Lijian Meng , Dehua Xiong , Lifeng Liu Journal Of Materials Chemistry A DOI: 10.1039/D5TA01671A Diamond Proposal Number(s): [36104] Show Abstract ▼ Abstract: The development of efficient and durable electrocatalysts for the oxygen evolution reaction (OER) is critical to advancing anion exchange membrane water electrolysis (AEMWE) technology for sustainable hydrogen production. Herein, we report the synthesis of multimetallic NiCrFeMo layered double hydroxides (LDHs) via a facile microwave-assisted hydrothermal approach, engineered as high-performance OER catalysts for AEMWE operating at industrially relevant current densities. Advanced X-ray absorption spectroscopy (XAS) studies demonstrate that the interplay of Ni, Cr, Fe, and Mo tailors the electronic structure and coordination environment. Consequently, the NiCrFeMo LDHs exhibit remarkable OER performance, achieving overpotentials of 236 and 387 mV at 10 and 500 mA cm⁻², respectively, in 1.0 M KOH, as well as outstanding durability at 500 mA cm-2 for 1000 hours with negligible degradation. In-situ differential electrochemical mass spectroscopy (DEMS) and density functional theory (DFT) analyses reveal that the OER taking place on NiCrFeMo LDHs follows the adsorbate evolving mechanism, with minimal lattice oxygen involvement, contributing to the catalyst’s longevity. When integrated into a prototype AEM electrolyzer cell as the anode catalysts, the cell demonstrates a current density of 1 A cm⁻² at a relatively low voltage of 1.87 V and operates at 0.5 A cm-2 for 100 hours without decay, highlighting the potential of NiCrFeMo LDHs for practical applications. This work elucidates the synergistic effects of multimetallic compositions in LDHs, offering a strategy for designing cost-effective, high-efficiency OER catalysts to support green hydrogen production on scale.	Apr 2025
B18-Core EXAFS	Capping agent, solvent and nanoparticle interactions: driving selectivity for biomass transformations George F. Tierney , Daniel Banks , Marina Carravetta , Alice E. Oakley , Shahram Alijani , Ilaria Barlocco , Nikolaos Dimitratos , Alberto Villa , Peter P. P. Wells Chemcatchem DOI: 10.1002/cctc.202401892 Diamond Proposal Number(s): [19850] Show Abstract ▼ Abstract: It is well-established that tailoring the structural properties of nanoparticles, e.g., their size, shape, available active surface and interaction with metal oxide supports, imparts significant control on catalytic transformations. However, this often relies on the use of stabilizing (capping) agents. These capping agents, predominantly long chain or bulky polymers, are not benign and also influence the catalytic performance. In this study, we expand on the use of surfactant-controlled reaction pathways for the hydrogenation of furfural on Pd/TiO2. Furthermore, we demonstrate how solid-state NMR is able to study the surfactant-catalyst interaction and how these can be correlated to the selectivity profile for furfural hydrogenation.	Apr 2025
I11-High Resolution Powder Diffraction	Mixed anion closo-carbaborates as Na-superionic conductors Jakob B. Grinderslev , Therese S. S. Kjær , Lasse N. Skov , Torben R. Jensen Journal Of Materials Chemistry A 482 DOI: 10.1039/D4TA07853E Diamond Proposal Number(s): [29197] Show Abstract ▼ Abstract: Sodium closo-borates have recently received significant attention as solid electrolytes for all-solid-state sodium batteries. The closo-borate compounds exhibit high thermal and electrochemical stability, and the reorientational motion and weak coordination of the anion facilitate fast Na-ion conductivity. Here, we report a simple synthesis method to directly form a mixed anion sodium closo-(carba)borate, Na1.24[(CB8H9)0.26(CB9H10)0.50(B12H12)0.24]. The [B12H12]2− can readily be removed from the sample, but complete separation of [CB8H9]− and [CB9H10]− is challenging owing to their chemical similarities. Na[(CB8H9)1−x(CB9H10)x] and Nax+y+2z[(CB8H9)x(CB9H10)y(B12H12)z] form solid solutions that are isostructural with the high temperature polymorph of NaCB9H10 (P31c), which is also maintained upon cooling to low temperatures (T < −54 °C). A second high temperature polymorph (Im[3 with combining macron]m) is also observed in minor amounts in [CB8H9]−-rich samples. The highest sodium conductivity was observed for the composition Na[(CB8H9)0.38(CB9H10)0.62], demonstrating a conductivity of σ(Na+) = 5.5 × 10−3 S cm−1 at 20 °C. The initial synthesis product, Na1.24[(CB8H9)0.26(CB9H10)0.50(B12H12)0.24], has a high ionic transport number of tion > 0.9999 and a negligible electronic conductivity of σe = 2 × 10−11 S cm−1 at room temperature. The solid electrolyte shows excellent stability against Na-metal and demonstrates a stable stripping/plating behavior. An all-solid-state battery is demonstrated using Na-metal as the anode, Na[(CB8H9)0.04(CB9H10)0.96] as the electrolyte and NaTi2(PO4)3 as the cathode.	Apr 2025
B18-Core EXAFS	How non-aqueous media direct the reaction of Ca(OH)2 with CO2 to different forms of CaCO3 : operando mid-infrared and X-ray absorption spectroscopy studies Thokozile A. Kathyola , Sin-Yuen Chang , Elizabeth A. Willneff , Colin J. Willis , Giannantonio Cibin , Paul Wilson , Anna B. Kroner , Elizabeth J. Shotton , Peter J. Dowding , Sven L. M. Schroeder Physical Chemistry Chemical Physics 108 DOI: 10.1039/D4CP04774E Diamond Proposal Number(s): [14673, 21040] Open Access Show Abstract ▼ Abstract: Time-resolved structural changes taking place during the reaction of Ca(OH)2 and CO2 forming different CaCO3 polymorphs, in aqueous and non-aqueous environments, were recorded operando using mid-infrared (mid-IR) and X-ray absorption near-edge structure (XANES) spectroscopy. Results show that Ca(OH)2 directly transforms into calcite in a pure water dispersion. In methanolic media with low water content, calcium di-methylcarbonate (Ca(OCOOCH3)2) is formed, which is hydrolysed to amorphous calcium carbonate (ACC) and vaterite in the presence of sufficient water. The addition of toluene shifts the equilibrium composition further from Ca(OH)2 to ACC and the crystalline forms of CaCO3, probably by affecting the activity of the methoxide intermediate. It can facilitate the formation of aragonite. No Ca(OH)2 conversion was detected in pure ethanol, isopropanol and toluene dispersions, except for nanoscale Ca(OH)2 in ethanolic dispersion, which formed calcium di-ethylcarbonate (Ca(OCOOCH2CH3)2). Our findings underline that vaterite formation is driven by the solution and solid state chemistry related to the reaction via alkoxides and carbonic acid esters of the alcohols, rather than the nucleation process in solution. The alcohol in these systems does not just act as a solvent but as a reactant.	Apr 2025
I19-Small Molecule Single Crystal Diffraction	Proton-driven lithium separation using alkali-templated coordination cages Xiang Sun , Kai Wu , Paula C. P. Teeuwen , Philipp Pracht , David J. Wales , Jonathan R. Nitschke Chem 141 DOI: 10.1016/j.chempr.2025.102556 Diamond Proposal Number(s): [29890] Open Access Show Abstract ▼ Abstract: The extraction of lithium from natural deposits is energy intensive due to its coexistence with physiochemically similar alkali (Na+ and K+) and alkaline earth (Mg2+ and Ca2+) metal ions. Methods for the direct and specific extraction of lithium from salt mixtures are thus essential to ensure an adequate supply of this metal for the batteries needed to decarbonize the world economy. Here, we present the preparation of alkali-metal-templated coordination cages and their application to lithium extraction. Within the cage framework, protons alter the relative binding affinities of Li+ and similar metal ions: protons associate exclusively with Li+ in close proximity at the cage vertices, repelling other cations as a result of increased electrostatic repulsion, enhanced steric hindrance, and reduced availability of coordinating nitrogen atoms. We developed this proton-driven lithium recognition within coordination cages into a separation cycle capable of extracting Li+ from a mixture of salts that includes Na+, K+, Mg2+, and Ca2+.	Apr 2025

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