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Effect of the Nuclearity and Coordination of Cu and Fe Sites in beta Zeolites on the Oxidation of Hydrocarbons
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SYSNO ASEP 0524176 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Effect of the Nuclearity and Coordination of Cu and Fe Sites in beta Zeolites on the Oxidation of Hydrocarbons Author(s) Sazama, Petr (UFCH-W) RID, ORCID
Morávková, Jaroslava (UFCH-W) RID, ORCID
Sklenák, Štěpán (UFCH-W) RID, ORCID, SAI
Vondrová, Alena (UFCH-W) RID
Tabor, Edyta (UFCH-W) RID, ORCID
Sádovská, Galina (UFCH-W) RID, ORCID
Pilař, Radim (UFCH-W) RID, ORCIDSource Title ACS Catalysis. - : American Chemical Society - ISSN 2155-5435
Roč. 10, č. 7 (2020), s. 3984-4002Number of pages 19 s. Language eng - English Country US - United States Keywords selective catalytic-reduction ; volatile organic-compounds ; initio molecular-dynamics ; total-energy calculations ; copper active-sites ; low-temperature ; n2o decomposition ; methane oxidation ; zsm-5 zeolite ; bea zeolite ; Cu zeolite ; Fe zeolite ; methane oxidation Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry R&D Projects GA18-20303S GA ČR - Czech Science Foundation (CSF) LM2015073 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) EF16_013/0001821 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) Method of publishing Limited access Institutional support UFCH-W - RVO:61388955 UT WOS 000526395000004 EID SCOPUS 85084083134 DOI 10.1021/acscatal.9b05431 Annotation Cu and Fe zeolites can activate oxygen for oxidative reactions of methane and stable hydrocarbon molecules. Here, we analyzed the activity of Cu and Fe sites with various nuclearities and coordinations in *BEA zeolites toward complete oxidation of methane, toluene, and ethanol by molecular oxygen. Spectral analysis of the interaction of methane with the individual Cu and Fe sites and a kinetic study show that the oxidation of methane is catalyzed by different active sites with different activation energies. In the low-temperature region (225-325 degrees C), the activity is primarily caused by reactive bridging oxygen atoms in dimeric Cu and Fe clusters. Isolated Fe3+-oxo ions in the octahedral coordination and Cu2+ partially charge-balanced by the framework with less rigid redox states contribute to the activity at higher temperatures of >= 350 degrees C. The isolated Fe3+-oxo ions tetrahedrally coordinated to the framework oxygen and the bare Cu2+ ions charge-balanced exclusively by the framework are strongly stabilized and cannot act as active sites. Oxidation of the hydrocarbons over both the dimeric and isolated Cu and Fe active sites is nonspecific with practically barrierless consecutive reactions of already activated molecules and therefore fully CO2-selective for all of the hydrocarbons in an excess of oxygen. Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2021 Electronic address http://hdl.handle.net/11104/0308541
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