Journal
CHEMICAL ENGINEERING SCIENCE
Volume 239, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ces.2021.116604
Keywords
CO2 methanation; Reverse water-gas shift; Ru-Ni alloy; DRIFTS; XANES; EXAFS
Categories
Funding
- Coordenacao de Aperfeicoamento de Pessoal de Ensino Superior (CAPES) [001]
- Conselho Nacional de Desenvolvimento Cientifico e Tecnologico [CNPQ - 302469/2020-6]
- CNPq [308200/2014-7, 303667/2018-4, 406516/2016-2, 302914/2015-3, 305023/2018-7]
- CAPES - COFECUB program [88881.142911/2017-01]
- Fundacao de Amparo a Pesquisa do Estado do Rio de Janeiro [FAPERJ - E26/202.840/2017, E-26/010.253/2016, FAPERJ - E26/010001861/2015]
- French government through the Programme Investissement d'Avenir (I-SITE) [I-SITE ULNE/ANR-16-IDEX-0004 ULNE]
- USDA National Institute of Food and Agriculture, Interdisciplinary Hands-on Research Traineeship and Extension Experiential Learning in Bioenergy/Natural Resources/Economics/Rural project, U-GREAT (Under Graduate Research, Education And Training) program [2016-67032-24984]
- Undergraduate NSF Research Program - National Science Foundation [1832388]
- UTSA
- State of Texas
- Direct For Education and Human Resources
- Division Of Undergraduate Education [1832388] Funding Source: National Science Foundation
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Zirconia was used to support Ru, Ni, and Ru-Ni bimetallic nanoparticles for CO2 methanation. The Ru/ZrO2 catalyst exhibited the highest CO2 reaction rate and CH4 selectivity. The performance improvement was attributed to the Ru-zirconia interface and Ru on-top atoms promoting reverse water gas shift and CO hydrogenation reactions.
Zirconia was used to support Ru, Ni, and Ru-Ni bimetallic nanoparticles for CO2 methanation. The formation of an alloy was detected in Ru K-edge spectra. The Ru/ZrO2 exhibited the highest CO2 reaction rate (1.35 mol/mol(metal).s) with a CH4 selectivity of 97.3%. The diffuse reflectance infrared fourier transform spectroscopy experiments suggest that formates serve as intermediates in converting CO2 to CO via reverse water-gas shift at the interface between Ru and defect-sites on zirconia, while Ru metal intercepts CO, further hydrogenating it to CH4. The better performance of Ru/ZrO2 could be related to the Ru-zirconia interface and Ru on-top atoms, which promote the reverse water gas shift and the CO hydrogenation reactions. Thus, this work provided important information about the effect of alloying Ru with Ni on the performance of the catalyst for the CO2 methanation, as well as the mechanism of this reaction for the best catalyst, Ru/ZrO2. (C) 2021 Elsevier Ltd. All rights reserved.
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