Počet záznamů: 1

Mechanism of Framework Oxygen Exchange in Fe-Zeolites: A Combined DFT and Mass Spectrometry Study

SYSNO ASEP	0389992
Druh ASEP	J - Článek v odborném periodiku
Zařazení RIV	J - Článek v odborném periodiku
Poddruh J	Článek ve WOS
Název	Mechanism of Framework Oxygen Exchange in Fe-Zeolites: A Combined DFT and Mass Spectrometry Study
Tvůrce(i)	Andrikopoulos, Prokopis C. (UFCH-W)_{RID, ORCID} Sobalík, Zdeněk (UFCH-W)_RID Nováková, Jana (UFCH-W)_RID Sazama, Petr (UFCH-W)_{RID, ORCID} Sklenák, Štěpán (UFCH-W)_{RID, ORCID, SAI}
Zdroj.dok.	ChemPhysChem. - : Wiley - ISSN 1439-4235 Roč. 14, č. 3 (2013), s. 520-531
Poč.str.	11 s.
Jazyk dok.	eng - angličtina
Země vyd.	DE - Německo
Klíč. slova	density functional theory ; iron ; zeolites
Vědní obor RIV	CF - Fyzikální chemie a teoretická chemie
CEP	IAA400400812 GA AV ČR - Akademie věd
	GA203/09/1627 GA ČR - Grantová agentura ČR
Institucionální podpora	UFCH-W - RVO:61388955
UT WOS	000315142900009
EID SCOPUS	84874055020
DOI	10.1002/cphc.201200900
Anotace	The role of framework oxygen atoms in N2O decomposition [N2O(g)!N2(g) and 1=2O2(g)] over Fe-ferrierite is investigated employing a combined experimental (N2 18O decomposition in batch experiments followed by mass spectroscopy measurements) and theoretical (density functional theory calculations) approach. The occurrence of the isotope exchange indicates that framework oxygen atoms are involved in the N2O decomposition catalyzed by Fe-ferrierite. Our study, using an Fe-ferrierite sample with iron exclusively present as FeII cations accommodated in the cationic sites, shows that the mobility of framework oxygen atoms in the temperature range: 553 to 593 K is limited to the four framework oxygen atoms of the two AlO4- tetrahedra forming cationic sites that accomodate FeII. They exchange with the Fe extra-framework 18O atom originating from the decomposed N2 18O. We found, using DFT calculations, that O2 molecules facilitate the oxygen exchange. However, the corresponding calculated energy barrier of 87 kcalmol-1 is still very high and it is higher than the assumed experimental value based on the occurrence of the sluggish oxygen exchange at 553 K.
Pracoviště	Ústav fyzikální chemie J.Heyrovského
Kontakt	Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196
Rok sběru	2014

Počet záznamů: 1