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Splitting Dioxygen over Distant Binuclear Fe Sites in Zeolites. Effect of the Local Arrangement and Framework Topology
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SYSNO ASEP 0539845 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Splitting Dioxygen over Distant Binuclear Fe Sites in Zeolites. Effect of the Local Arrangement and Framework Topology Author(s) Tabor, Edyta (UFCH-W) RID, ORCID
Lemishka, Mariia (UFCH-W) RID, ORCID
Olszówka, Joanna Elżbieta (UFCH-W) ORCID
Mlekodaj, Kinga (UFCH-W) RID, ORCID
Dědeček, Jiří (UFCH-W) RID, ORCID
Andrikopoulos, Prokopis C. (UFCH-W) RID, ORCID
Sklenák, Štěpán (UFCH-W) RID, ORCID, SAISource Title ACS Catalysis. - : American Chemical Society - ISSN 2155-5435
Roč. 11, č. 4 (2021), s. 2340-2355Number of pages 16 s. Language eng - English Country US - United States Keywords alpha oxygen ; oxidation of methane ; utilization of methane Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry R&D Projects GA17-00742S GA ČR - Czech Science Foundation (CSF) Method of publishing Limited access Institutional support UFCH-W - RVO:61388955 UT WOS 000621598700035 EID SCOPUS 85101027291 DOI 10.1021/acscatal.0c04459 Annotation Activation of dioxygen is of extreme importance due to its potential for transformation of methane to valuable products and applications in other selective oxidation reactions. Distant binuclear cationic Fe(II) centers in Fe-ferrierite were shown to split dioxygen at room temperature to form a pair of very active oxygen species (i.e., α-oxygens) and subsequently oxidize methane to methanol at room temperature as well. Our study reveals that the activity in splitting dioxygen represents a general property of the distant binuclear cationic Fe(II) centers stabilized in the aluminosilicate matrix. Computational models of the ferrierite, beta, A, and mordenite zeolites with various Al sitings in the rings forming the cationic sites were investigated by periodic DFT calculations including molecular dynamics simulations. The results reveal that the Fe(II) sites stabilized in various zeolite matrices can split dioxygen if the two cationic sites forming the distant binuclear Fe(II) centers (i) face each other, (ii) are parallel, and (iii) are axial, and (iv) the Fe···Fe distance lies in a narrow range from ca. 7 to ca. 8 Å (ca. 7–ca. 10 Å for the distance between the two rings (forming the corresponding cationic sites) in empty zeolites since this distance is equal to or larger than the Fe···Fe distances). Our study opens the possibility of developing Fe-zeolite-based systems for the dioxygen activation employed for direct oxidations using various zeolite matrices. Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2022 Electronic address http://hdl.handle.net/11104/0317547
Number of the records: 1