DOI: 10.1246/bcsj.73.29. Formation of an Iron-Oxo Species upon Decomposition of Dinitrogen Oxide on a Model of Fe-ZSM-5 Zeolite

Formation of an Iron-Oxo Species upon Decomposition of Dinitrogen Oxide on a Model of Fe-ZSM-5 Zeolite

10.1246/bcsj.73.29

Crossref journal-article

Oxford University Press (OUP)

Bulletin of the Chemical Society of Japan (286)

Abstract

Abstract The so-called ``α-oxygen" on Fe-ZSM-5 zeolite, a surface oxygen species responsible for high reactivity in oxidation of methane and of benzene, has been investigated. We present from density-functional-theory (DFT) calculations how such a reactive surface species is generated upon decomposition of dinitrogen oxide (N2O) and propose a possible form of ``α-oxygen" on Fe-ZSM-5 zeolite. In the initial stages of the reactions, a complex involving an Fe(ON2) moiety is formed, followed by dissociation into an iron-oxo species and N2. The activation energy for the decomposition of N2O on a possible iron active site model of Fe-ZSM-5 zeolite is predicted to be 2.4 kcal mol-1 at the B3LYP level of theory. Therefore the decomposition of N2O is expected to take place easily at a coordinatively unsaturated iron active center supported on zeolite. The iron-oxo species thus formed should play an essential role in the direct hydroxylation of methane, benzene, and other hydrocarbons if it involves a coordinatively unsaturated iron. The oxygen exchange on the iron-oxo complex was also investigated. The activation energy for the oxygen exchange on the ``α-oxygen" is predicted to be 26.8 kcal mol-1. We propose that the bare FeO+ complex and the so-called ``α-oxygen" on Fe-ZSM-5 zeolite involve similar catalytic active centers responsible for similar catalytic functions for methane and benzene.

Authors 4

Kazunari Yoshizawa (first)
Takashi Yumura (additional)
Yoshihito Shiota (additional)
Tokio Yamabe (additional)

References 70 Referenced 55

Dates

Type	When
Created	23 years ago (Sept. 6, 2002, 6:09 a.m.)
Deposited	1 year, 7 months ago (Jan. 20, 2024, 12:43 a.m.)
Indexed	3 weeks, 3 days ago (Aug. 12, 2025, 5:57 p.m.)
Issued	25 years, 8 months ago (Jan. 1, 2000)
Published	25 years, 8 months ago (Jan. 1, 2000)
Published Online	23 years, 10 months ago (Oct. 31, 2001)
Published Print	25 years, 8 months ago (Jan. 1, 2000)

Funders 0

None

BibTeX

@article{Yoshizawa_2000, title={Formation of an Iron-Oxo Species upon Decomposition of Dinitrogen Oxide on a Model of Fe-ZSM-5 Zeolite}, volume={73}, ISSN={1348-0634}, url={http://dx.doi.org/10.1246/bcsj.73.29}, DOI={10.1246/bcsj.73.29}, number={1}, journal={Bulletin of the Chemical Society of Japan}, publisher={Oxford University Press (OUP)}, author={Yoshizawa, Kazunari and Yumura, Takashi and Shiota, Yoshihito and Yamabe, Tokio}, year={2000}, month=jan, pages={29–36} }

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