Journal
APPLIED CATALYSIS A-GENERAL
Volume 626, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcata.2021.118357
Keywords
CeO2; Methane oxidation; In-situ; XANES; Oxygen vacancies
Categories
Funding
- Brazilian Synchrotron Light Laboratory (LNLS, Brazil) [XAFS1 13662, XAFS1 15360, 20170441]
- Agencia Nacional de Promocion Cientifica y Tecnologica (Argentina) [3411, 1921, 3021]
- CAPES-MinCyT bilateral cooperation
- University of Sao Paulo, Brazil
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This study focuses on the analysis of SDC nanopowders and NiO/SDC nanocomposites in terms of their reducibility and catalytic activity for partial oxidation of methane. The results show that the crystallite size and surface area play a crucial role in methane activation by modifying the sample's redox behavior, with the oxidation of the metallic phase being the main cause of sample deactivation. A complex relationship between oxygen vacancy concentration and catalytic activity was observed during the experiments.
In this work, we analyze Sm2O3-doped CeO2 (SDC) nanopowders and NiO/SDC nanocomposites in terms of sample reducibility and catalytic activity for partial oxidation of methane. We assess the role of the average crystallite size and specific surface area in Ni and Ce reduction kinetics by in-situ X-ray absorption spectroscopy experiments in diluted H2 and CH4/O2 mixtures. Our results indicate that crystallite size and surface area play a key role in CH4 activation through modification of the sample redox behavior. The oxidation of the metallic phase is the main cause of sample deactivation. A clear relationship is established between the temperature of maximum Ni oxidation rate and grain size. An interplay between Ce atoms from the support and Ni from the active phase was observed during the experiments, evidencing a complex relationship between oxygen vacancy concentration and catalytic activity. A high Ce3+ content in catalyst support was detrimental to catalytic activity
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