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Synthesis of a Cu/ZnO Nanocomposite by Electroless Plating for the Catalytic Conversion of CO2 to Methanol
Maja Pori, Iztok Arčon, Marjan Marinšek, Goran Dražić, Blaž Likozar, Zorica Crnjak Orel, Damjan Lašič Jurković, 2019, original scientific article

Abstract: The process of methanol synthesis based on the hydrogenation of CO2 was investigated over binary Cu/ZnO catalyst materials, prepared by applying a novel electroless plating fabrication method. The activity of the produced catalytic samples was determined at temperature range between 200 and 300 °C and the feedstock conversion data were supplemented with a detailed microstructure analysis using high-resolution transmission electron microscopy (HRTEM), X-ray powder diffraction (XRD) and Cu and Zn K-edge, X-ray absorption near-edge structure (XANES) measurements and extended X-ray absorption fine-structure (EXAFS) measurements. It was confirmed that the disorder in the Cu crystallites created unique geometrical situations, which acted as the additional reactive centres for the adsorption of the reactant molecule species. Copper and zinc structural synergy (spill-over) was also demonstrated as being crucial for the carbon dioxide’s activation. EXAFS and XANES results provide strong evidence for surface alloying between copper and zinc and thus the present results demonstrate new approach applicable for explaining metal–support interactions.
Found in: osebi
Keywords: EXAFS, CuZn alloy, Spillover mechanism, CO2 valorization, Electroless deposition method, Heterogeneous catalysis
Published: 12.04.2019; Views: 1402; Downloads: 0
.pdf Fulltext (1,92 MB)

Photo-Chemically-Deposited and Industrial Cu/ZnO/Al2O3 Catalyst Material Surface Structures During CO2 Hydrogenation to Methanol: EXAFS, XANES and XPS Analyses of Phases After Oxidation, Reduction, and Reaction
Blaž Likozar, Iztok Arčon, Venkata Dasireddy, Maja Pori, 2021, original scientific article

Abstract: Industrial Cu/ZnO/Al2O3 or novel rate catalysts, prepared with a photochemical deposition method, were studied under functional CH3OH synthesis conditions at the set temperature (T) range of 240–350 °C, 20 bar pressure, and stoichiometric carbon dioxide/hydrogen composition. Analytical scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), X-ray adsorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) methods were systematically utilized to investigate the interfaces, measured local geometry, and chemical state electronics around the structured active sites of commercially available Cu/ZnO/Al2O3 material or synthesized Cu/ZnO. Processed Cu K-edge EXAFS analysis suggested that various Cu atom species, clusters, metallic fcc Cu, Cu oxides (Cu2O or CuO) and the Cu0.7Zn2 alloy with hexagonal crystalline particles are contained after testing. It was proposed that in addition to the model’s Cu surface area, the amount, ratio and dispersion of the mentioned bonded Cu compounds significantly influenced activity. Additionally, XPS revealed that carbon may be deposited on the commercial Cu/ZnO/Al2O3, forming the inactive carbide coating with Cu or/and Zn, which may be the cause of basicity’s severe deactivation during reactions. The selectivity to methanol decreased with increasing T, whereas more Cu0.7Zn2 inhibited the CO formation through reverse water–gas shift (RWGS) CO2 reduction.
Found in: osebi
Keywords: CH3OH synthesis, Cu/ZnO-based catalyst, XPS, XANES, EXAFS analyses, Catalyst selectivity and activity
Published: 03.06.2021; Views: 72; Downloads: 0
.pdf Fulltext (3,98 MB)

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