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Improvement of Ni/Al2O3 Catalysts for Low-Temperature CO2 Methanation by Vanadium and Calcium Oxide Addition

CO₂ methanation is a very promising technology for the production of alternative fuels with the simultaneous use of greenhouse gases. Therefore, intensive research is carried out on the optimization of catalysts with excellent properties for operation in the area of low temperatures. Here, we present research on a catalyst composed of 19 wt % NiO supported on alumina/calcium aluminate. The catalyst was modified with V₂O₅ in order to be suited for extrusion and scale-up in the frame of power to gas technology. Samples with various vanadium contents (Ni–xV, where x represents the amount of vanadium) were prepared in the form of ground granules obtained from 0.5 mm diameter spherical grains. X-ray diffraction (XRD), transmission electron microscopy (TEM), skeletal infrared (IR), diffuse reflectance ultraviolet–visible-near-infrared (DR-UV–vis-NIR), and X-ray photoelectron (XPS) spectroscopies, as well as H₂ temperature-programmed reduction (H₂-TPR), were used to characterize the samples. Catalytic performances of the catalyst samples were tested in CO₂ hydrogenation at 1 atm. Among the many supported Ni catalysts tested in our laboratories, the catalysts of 0.5 and 1 wt % V showed very high activity, with the highest CH₄ yield of 97% at 623 K. These catalysts exhibited 100% CH₄ selectivity up to 673 K. The excellent performances of the studied catalysts are attributed to the possible formation of Ni–V solid solution alloy nanoparticles.

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This research was supported by receiving funding from the Foundation for Polish Science Reintegration/2016-1/5 Project “Waste to fuel—Catalyst and process development for waste biomass valorization”, cofinanced by the European Regional Development Fund under the Intelligent Development Operational Program 2014–2020 (POIR), Axis IV: Increasing the scientific and research potential, Measure 4.4: Increasing the human potential in the R&D sector, awarded to I.S.P., with connected subcontracting agreement 1414/2018 given to G.G. for the Task “CO₂ valorization over V-modified Ni catalyst supported on various supports”. I.S.P. gratefully acknowledges support from the French Government for collaboration with Sorbonne University Project “Catalytic conversion of CO₂ to hydrocarbons: The Ni–V catalyst selectivity and durability in in plasma assisted hydrogenation of CO₂ to methane”