Effect of the Nuclearity and Coordination of Cu and Fe Sites in beta Zeolites on the Oxidation of Hydrocarbons
The result's identifiers
Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388955%3A_____%2F20%3A00524176" target="_blank" >RIV/61388955:_____/20:00524176 - isvavai.cz</a>
Result on the web
<a href="http://hdl.handle.net/11104/0308541" target="_blank" >http://hdl.handle.net/11104/0308541</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acscatal.9b05431" target="_blank" >10.1021/acscatal.9b05431</a>
Alternative languages
Result language
angličtina
Original language name
Effect of the Nuclearity and Coordination of Cu and Fe Sites in beta Zeolites on the Oxidation of Hydrocarbons
Original language description
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.
Czech name
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10403 - Physical chemistry
Result continuities
Project
Result was created during the realization of more than one project. More information in the Projects tab.
Continuities
I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace
Others
Publication year
2020
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů
Data specific for result type
Name of the periodical
ACS Catalysis
ISSN
2155-5435
e-ISSN
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Volume of the periodical
10
Issue of the periodical within the volume
7
Country of publishing house
US - UNITED STATES
Number of pages
19
Pages from-to
3984-4002
UT code for WoS article
000526395000004
EID of the result in the Scopus database
2-s2.0-85084083134