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Revealing catalyst restructuring and composition during nitrate electroreduction through correlated operando microscopy and spectroscopy.
Nat Mater
January 2025
Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, Berlin, Germany.
Electrocatalysts alter their structure and composition during reaction, which can in turn create new active/selective phases. Identifying these changes is crucial for determining how morphology controls catalytic properties but the mechanisms by which operating conditions shape the catalyst's working state are not yet fully understood. In this study, we show using correlated operando microscopy and spectroscopy that as well-defined CuO cubes evolve under electrochemical nitrate reduction reaction conditions, distinct catalyst motifs are formed depending on the applied potential and the chemical environment.
View Article and Find Full Text PDFSelf-absorption effect in soft X-ray emission spectra utilized for bandgap evaluation of semiconductors.
Microscopy (Oxf)
January 2025
Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Miyagi 980-8577, Japan.
The self-absorption effects observed in the background intensity just above the Si L-emission spectra of Si and β-Si3N4, and the C K-emission spectra of diamond and graphite were examined. Based on comparisons with reported results, the energy positions of absorption edges-representing the bottom of conduction bands (CB)-were assigned. The self-absorption profiles in the background intensities were consistent with previously reported data.
View Article and Find Full Text PDFHow amino acids intercalate in CaFe layered double hydroxides: A combined RIXS and NEXAFS study.
Chemphyschem
January 2025
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, PS-ISRR, GERMANY.
Two-dimensional layered double hydroxides (LDHs) are ideal candidates for a large number of (bio)catalytic applications due to their flexible composition and easy to tailor properties. Functionality can be achieved by intercalation of amino acids (as the basic units of peptides and proteins). To gain insight on the functionality, we apply resonant inelastic soft x-ray scattering and near edge x-ray absorption fine structure spectroscopy to CaFe LDH in its pristine form as well as intercalated with the amino acids proline and cysteine to probe the electronic structure and its changes upon intercalation.
View Article and Find Full Text PDFMagnetotactic bacteria from diverse Pseudomonadota families biomineralize intracellular Ca-carbonate.
ISME J
January 2025
Université Aix-Marseille, CNRS, CEA, UMR7265 Institut de Biosciences and Biotechnologies d'Aix-Marseille, CEA Cadarache, F-13108 Saint-Paul-lez-Durance, France.
Intracellular calcium carbonate formation has long been associated with a single genus of giant Gammaproteobacteria, Achromatium. However, this biomineralization has recently received increasing attention after being observed in photosynthetic Cyanobacteriota and in two families of magnetotactic bacteria affiliated with the Alphaproteobacteria. In the latter group, bacteria form not only intracellular amorphous calcium carbonates into large inclusions that are refringent under the light microscope, but also intracellular ferrimagnetic crystals into organelles called magnetosomes.
View Article and Find Full Text PDFStructures of Gas-Phase Hydrated Phosphotyrosine Revealed by Soft X-ray Action Spectroscopy.
Chemistry
January 2025
Deutsches Elektronen-Synchrotron DESY, 22603, Hamburg, Germany.
Gas-phase near-edge X-ray absorption mass spectrometry (NEXAMS) was employed at the carbon and oxygen K-edges to probe the influence of a single water molecule on the protonated phosphotyrosine molecule. The results of the photodissociation experiments revealed that the water molecule forms two bonds, with the phosphate group and another chemical group. By comparing the NEXAMS spectra at the carbon and oxygen K-edges with density functional theory calculations, we attributed the electronic transitions responsible for the observed resonances, especially the transitions due to the presence of the water molecule.
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