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Mechanisms of CO oxidation on high entropy spinels.
Phys Chem Chem Phys
January 2025
CNR-Istituto Officina dei Materiali, TASC, Trieste, Italy.
The CO oxidation reaction on (Co,Mg,Mn,Ni,Zn)(Al,Co,Cr,Fe,Mn)O and (Cr,Mn,Fe,Co,Ni)O high entropy spinel oxides was studied for what concerns its mechanism by means of soft X-ray absorption spectroscopy. In the (Cr,Mn,Fe,Co,Ni)O high entropy spinel, CO oxidation starts at 150 °C, and complete conversion to CO is obtained at 300 °C. For the (Co,Mg,Mn,Ni,Zn)(Al,Co,Cr,Fe,Mn)O spinel oxides, in contrast, the reaction starts at 200 °C, and complete conversion needs temperatures of the order of 350 °C.
View Article and Find Full Text PDFRevealing 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 PDFEffective Utilization of Nanoporosity and Surface Area Guides Electrosynthesis over Soft-Landed Copper Oxide Catalyst Layers.
Nano Lett
January 2025
Applied Electrochemistry and Catalysis (ELCAT), University of Antwerp, 2610 Wilrijk, Belgium.
Porous nanomaterials find wide-ranging applications in modern medicine, optoelectronics, and catalysis, playing a key role in today's effort to build an electrified, sustainable future. Accurate in situ quantification of their structural and surface properties is required to model their performance and improve their design. In this article, we demonstrate how to assess the porosity, surface area and utilization of a model nanoporous soft-landed copper oxide catalyst layer/carbon interface, which is otherwise difficult to resolve using physisorption or capacitance-based methods.
View Article and Find Full Text PDFSolar-driven production of renewable chemicals via biomass hydrogenation with green methanol.
Nat Commun
January 2025
School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, National Synchrotron Radiation Laboratory, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, PR China.
Solar-driven, selective biomass hydrogenation is recognized as a promising route to renewable chemicals production, but remains challenging. Here, we report a TiO supported Cu single-atom catalyst with a four-coordinated Cu-O structure, which can be universally applied for solar-driven production of various renewable chemicals from lignocellulosic biomass-derived platform molecules with good yields using green methanol as a hydrogen donor, to address this challenge. It is significant that the biomass upgrading driven by natural sunlight on a gram scale demonstrates the great practical potential.
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