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Low-temperature selective oxidation of methane over distant binuclear cationic centers in zeolites

SYSNO ASEP	0505953
Document Type	J - Journal Article
R&D Document Type	Journal Article
Subsidiary J	Článek ve WOS
Title	Low-temperature selective oxidation of methane over distant binuclear cationic centers in zeolites
Author(s)	Tabor, Edyta (UFCH-W)_{RID, ORCID} Lemishka, Mariia (UFCH-W)_{RID, ORCID} Sobalík, Zdeněk (UFCH-W)_RID Mlekodaj, Kinga (UFCH-W)_{RID, ORCID} Andrikopoulos, Prokopis C. (UFCH-W)_{RID, ORCID} Dědeček, Jiří (UFCH-W)_{RID, ORCID} Sklenák, Štěpán (UFCH-W)_{RID, ORCID, SAI}
Article number	71
Source Title	Communications Chemistry. - : Nature Publishing Group - ISSN 2399-3669 Roč. 2, JAN 2019 (2019)
Number of pages	9 s.
Language	eng - English
Country	GB - United Kingdom
Keywords	initio molecular dynamics ; total energy calculation ; N2O decomposition
Subject RIV	CF - Physical ; Theoretical Chemistry
OECD category	Physical chemistry
R&D Projects	GA17-00742S GA ČR - Czech Science Foundation (CSF)
Method of publishing	Open access
Institutional support	UFCH-W - RVO:61388955
UT WOS	000472619600001
EID SCOPUS	85071158227
DOI	10.1038/s42004-019-0173-9
Annotation	Highly active oxygen capable to selectively oxidize methane to methanol at low temperature can be prepared in transition-metal cation exchanged zeolites. Here we show that the α-oxygen stabilized by the negative charges of two framework aluminum atoms can be prepared by the dissociation of nitrous oxide over distant binuclear cation structures (M(II)…M(II), M = cobalt, nickel, and iron) accommodated in two adjacent 6-rings forming cationic sites in the ferrierite zeolite. This α-oxygen species is analogous to that known only for iron exchanged zeolites. In contrast to divalent iron cations, only binuclear divalent cobalt cationic structures and not isolated divalent cobalt cations are active. Created methoxy moieties are easily protonated to yield methanol, formaldehyde, and formic acid which are desorbed to the gas phase without the aid of water vapor while previous studies showed that highly stable methoxy groups were formed on isolated iron cations in iron exchanged ZSM-5 zeolites.
Workplace	J. Heyrovsky Institute of Physical Chemistry
Contact	Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196
Year of Publishing	2020
Electronic address	http://hdl.handle.net/11104/0297274

Number of the records: 1