On the involvement of radical oxygen species O− in catalytic oxidation of benzene to phenol by nitrous oxide

Chernyavsky, V.S.; Pirutko, Larisa V.; Uriarte, A.; Харитонов, А. С.; Panov, G. I.

doi:10.1016/j.jcat.2006.10.023

Cited by 63 publications

(37 citation statements)

References 25 publications

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“…The direct oxidation of benzene to phenol is one of the most challenging reactions in the field of catalytic chemistry. [1][2][3][4][5] It was found that a special Fe-oxo species, which was formed after high temperature pretreatment of Fe/ZSM-5 followed by reaction with N 2 O, could selectively oxidize methane and benzene even at 243 K, which mimics the biocatalysis of soluble methane monooxygenase (sMMO). 4 It was found that the active oxygen species generated on Fe/ZSM-5 can oxide benzene to phenol in a one-step method at high temperature.…”

Section: Introductionmentioning

confidence: 99%

“…4 It was found that the active oxygen species generated on Fe/ZSM-5 can oxide benzene to phenol in a one-step method at high temperature. [1][2][3][4][5][6][7] These findings have received much attention in studying the active oxygen species as well as the reaction intermediate for the selective oxidation of benzene, particularly the reaction intermediate involved in the mechanism.…”

Section: Introductionmentioning

confidence: 99%

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Direct Spectroscopic Observation of Fe(III)−Phenolate Complex Formed From the Reaction of Benzene With Peroxide Species on Fe/ZSM-5 At Room Temperature

Xia

Sun

et al. 2008

J. Phys. Chem. C

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The reaction of benzene with the active oxygen species was studied by UV−visible diffuse reflectance and Raman spectroscopies. For the first time, the intermediate Fe(III)−phenolate complex was evidenced by a UV−visible absorption band at 690 nm and the Raman bands at 643, 896, 990, 1149, 1228, 1475, 1580, and 1607 cm−1. The Raman bands of the Fe(III)−phenolate complex were also confirmed by density functional theory calculations.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Direct Spectroscopic Observation of Fe(III)−Phenolate Complex Formed From the Reaction of Benzene With Peroxide Species on Fe/ZSM-5 At Room Temperature

Xia

Sun

et al. 2008

J. Phys. Chem. C

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“…Different suggestions have been made in the literature: atomic oxygen [4,9,10], oxygen anion radicals [15,16] and/or Fe 4+ =O groups [14], have been proposed as active species of N 2 O decomposition and/ or hydroxylation of benzene with N 2 O. It is well established that a-oxygen is produced by interaction of reduced samples with N 2 O [17].…”

Section: Introductionmentioning

confidence: 99%

FTIR Characterization of Fe3+–OH Groups in Fe–H–BEA Zeolite: Interaction with CO and NO

et al. 2008

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Fe 3+ -OH groups of a Fe-H-BEA sample prepared by conventional ion-exchange method are characterized by an IR band at 3686-3684 cm -1 . They exhibit a weak acidity: upon low-temperature CO adsorption the O-H stretching modes are blue shifted by 100 cm -1 and the respective carbonyl adducts are observed at 2158 cm -1 . The Fe 3+ -OH groups are reduced at room temperature by NO to form Fe 2+ -NO species and NO + groups in cationic positions. Desorption of pre-adsorbed NO at temperatures above 373 K regenerates the Fe 3+ -OH groups. The relation of the Fe 3+ -OH species to the socalled a-oxygen is discussed.

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“…9,12−17 It has been found that only a fraction of these “α-oxygen” are able to oxidize benzene to phenol. 5,15 Steaming of isomorphously substituted Fe/ZSM-5 zeolite is crucial to enhance the number of extraframework Fe ions. 9,18 During steaming, Fe–O–Si bonds in Fe/ZSM-5 crystals are broken, resulting in the migration of Fe from the zeolite framework to extraframework locations.…”

Section: Introductionmentioning

confidence: 99%

Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol

2017

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Fe/ZSM-5 nanosheet zeolites of varying thickness were synthesized with di- and tetraquaternary ammonium structure directing agents and extensively characterized for their textural, structural, and catalytic properties. Introduction of Fe3+ ions in the framework of nanosheet zeolites was slightly less effective than in bulk ZSM-5 zeolite. Steaming was necessary to activate all catalysts for N2O decomposition and benzene oxidation. The higher the Fe content, the higher the degree of Fe aggregation was after catalyst activation. The degree of Fe aggregation was lower when the crystal domain size of the zeolite or the Fe content was decreased. These two parameters had a substantial influence on the catalytic performance. Decreasing the number of Fe sites along the b-direction strongly suppressed secondary reactions of phenol and, accordingly, catalyst deactivation. This together with the absence of diffusional limitations in nanosheet zeolites explains the much higher phenol productivity obtainable with nanostructured Fe/ZSM-5. Steamed Fe/ZSM-5 zeolite nanosheet synthesized using C22-6-3·Br2 (domain size in b-direction ∼3 nm) and containing 0.24 wt % Fe exhibited the highest catalytic performance. During the first 24 h on stream, this catalyst produced 185 mmolphenol g–1. Calcination to remove the coke deposits completely restored the initial activity.

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On the involvement of radical oxygen species O− in catalytic oxidation of benzene to phenol by nitrous oxide

Cited by 63 publications

References 25 publications

Direct Spectroscopic Observation of Fe(III)−Phenolate Complex Formed From the Reaction of Benzene With Peroxide Species on Fe/ZSM-5 At Room Temperature

Direct Spectroscopic Observation of Fe(III)−Phenolate Complex Formed From the Reaction of Benzene With Peroxide Species on Fe/ZSM-5 At Room Temperature

FTIR Characterization of Fe3+–OH Groups in Fe–H–BEA Zeolite: Interaction with CO and NO

Stable Fe/ZSM-5 Nanosheet Zeolite Catalysts for the Oxidation of Benzene to Phenol

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