Highly Active and Stable Ni/La-Doped Ceria Material for Catalytic CO2Reduction by Reverse Water-Gas Shift Reaction
| Autor: | Consuelo Alvarez-Galvan, Pablo G. Lustemberg, Freddy E. Oropeza, Belén Bachiller-Baeza, Martin Dapena Ospina, María Herranz, Jesús Cebollada, Laura Collado, José M. Campos-Martin, Víctor A. de la Peña-O’Shea, José A. Alonso, M. Verónica Ganduglia-Pirovano |
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| Přispěvatelé: | Ministerio de Ciencia e Innovación (España), Consejo Superior de Investigaciones Científicas (España), Agencia Estatal de Investigación (España), Comunidad de Madrid, European Commission |
| Rok vydání: | 2022 |
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| Popis: | [EN] The design of an active, effective, and economically viable catalyst for CO2 conversion into value-added products is crucial in the fight against global warming and energy demand. We have developed very efficient catalysts for reverse water-gas shift (rWGS) reaction. Specific conditions of the synthesis by combustion allow the obtention of macroporous materials based on nanosized Ni particles supported on a mixed oxide of high purity and crystallinity. Here, we show that Ni/La-doped CeO2 catalysts─with the "right"Ni and La proportions─have an unprecedented catalytic performance per unit mass of catalyst for the rWGS reaction as the first step toward CO2 valorization. Correlations between physicochemical properties and catalytic activity, obtained using a combination of different techniques such as X-ray and neutron powder diffraction, Raman spectroscopy, in situ near ambient pressure X-ray photoelectron spectroscopy, electron microscopy, and catalytic testing, point out to optimum values for the Ni loading and the La proportion. Density functional theory calculations of elementary steps of the reaction on model Ni/ceria catalysts aid toward the microscopic understanding of the nature of the active sites. This finding offers a fundamental basis for developing economical catalysts that can be effectively used for CO2 reduction with hydrogen. A catalyst based on Ni0.07/(Ce0.9La0.1Ox)0.93 shows a CO production of 58 × 10-5 molCO·gcat-1·s-1 (700 °C, H2/CO2 = 2; selectivity to CO > 99.5), being stable for 100 h under continuous reaction. We acknowledge the financial support of the Spanish Ministry of Science and Innovation (PID2021-123287OB-I00, PID2021-122477-OB-I00, PID2021-128915NB-I00, and RTI2018-101604-B-I00) and of the CSIC through the i-LINK 2021 program (LINKA20408). Financial support has also been received from AEI-MINECO/FEDER (Nympha Project, PID2019-106315RB-I00), “Comunidad de Madrid” regional government, and the European Structural Funds (FotoArt-CM project, S2018/NMT-4367). Authors also acknowledge financial support from the grant PLEC2021-007906 funded by MCIN/AEI/10.13039/501100011033 and the “European Union NextGenerationEU/PRTR”. We are grateful to ILL (France) for making all facilities available. This project also received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement no. 832121. Computer time provided by the RES (Red Española de Supercomputación) resources at the MareNostrum 4 (BSC, Barcelona) node and the DECI resources at the BEM cluster of the WCSS based in Poland with the support from PRACE aislb is acknowledged. |
| Databáze: | OpenAIRE |
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