Selective oxidation of aromatic compounds on zeolites using N2O as a mild oxidant

Kustov, L. М.; Тарасов, А. Л.; Богдан, В. И.; Tyrlov, A.A.; Fulmer, James

doi:10.1016/s0920-5861(00)00354-0

Cited by 68 publications

(33 citation statements)

References 6 publications

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“…ZSM-5 zeolites have been reported to be efficient catalysts for the hydroxylation of benzene to phenol by nitrous oxide with selectivity to phenol close to 100% at about 50% conversion of benzene [1][2][3][4]. The catalytic performance is due to iron in the zeolites [5][6][7][8][9].…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Benzene hydroxylation over FeZSM-5 catalysts: which Fe sites are active?

Yuranov

Bulushev

Renken

et al. 2004

Journal of Catalysis

111

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FeZSM-5 with a wide range of Fe content (0.015-2.1 wt%) were studied in the benzene hydroxylation to phenol with nitrous oxide (C 6 H 6 :N 2 O = 1:5) at low temperatures (< 550 K). Catalysts were activated before the reaction by steaming and/or calcinations in He (1323 K). High selectivity of benzene-to-phenol transformation (> 98%) was obtained within 3 h without any deactivation of the catalyst. Three types of Fe(II) sites were formed in the zeolites extraframework due to activation and are attributed to: (1) Fe(II) sites in mononuclear species, (2) oligonuclear species with at least two oxygen-bridged Fe(II) sites, and (3)

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Section: Introductionmentioning

confidence: 99%

“…This α-oxygen is responsible for the benzene hydroxylation and low-temperature oxidation of CO and CH 4 [18]. Each Fe atom in the binuclear complex is capable of generating one α-oxygen atom.…”

Section: Introductionmentioning

confidence: 99%

Benzene hydroxylation over FeZSM-5 catalysts: which Fe sites are active?

Yuranov

Bulushev

Renken

et al. 2004

Journal of Catalysis

111

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“…However, the nature of active sites responsible for the α-oxygen species formation (hereafter "α-sites") remains unclear. Some authors claim that Lewis acid sites of the extraframework aluminum [9,10] or gallium [11] are responsible for the ben-Scheme 1. Formation of α-sites and active α-oxygen [3].…”

Section: Introductionmentioning

confidence: 99%

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Kiwi‐Minsker

2003

Journal of Catalysis

131

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Surface-active centers were detected in HZSM-5 with a low content of iron (< 1000 ppm) activated by steaming and high-temperature calcination in inert atmospheres (up to 1323 K). These centers lead to the formation of surface oxygen (O) ad species from N 2 O and were characterized quantitatively by the transient response method. The total amount of active centers was proportional to the content of iron in the zeolites. Only a part of (O) ad deposited by decomposing N 2 O was active in CO oxidation at 523 K and appeared as sharp O 2 peaks at 666 K during the TPD measurements. A binuclear Fe center is suggested featuring a "diamond core" structure, similar to that of the monooxygenase enzyme, as an active center. The active O atoms were assigned to the paired terminal oxygen atoms each bonded to one Fe site (ferryl groups) in the diferric [Fe 2 O 2 H] + cluster. Oxygen pretreatment at 823 K decreases somewhat the total amount of active sites but does not affect the ratio of active/inactive oxygen. Zeolite presaturated by water vapor at 473-523 K generates (O) ad species from N 2 O completely inactive in the CO oxidation. Part of it appears as a broad peak at 940 K in the TPD profile. The total amount of the deposited oxygen corresponds to half of the stoichiometric amount of the surface Fe atoms and suggests that water blocks a half of the binuclear [Fe 2 O 2 H] + center, the remaining acting as a single Fe site.

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“…A one-step oxidation of benzene by nitrous oxide is an attractive way of phenol production and various catalysts based on metal oxides have been used for this process [4][5][6][7][8][9][10][11][12][13]. The MFI type zeolites have been reported as the most efficient catalyst with selectivity as high as 95% towards phenol formation at appreciable conversion [6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

“…The MFI type zeolites have been reported as the most efficient catalyst with selectivity as high as 95% towards phenol formation at appreciable conversion [6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

Synthesis of ZSM-5 coatings on stainless steel grids and their catalytic performance for partial oxidation of benzene by N2O

Louis

Reuse

Kiwi‐Minsker

et al. 2001

Applied Catalysis A: General

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The one step hydroxylation of benzene has been performed over structured catalytic bed made of ZSM-5 coatings grown by hydrothermal synthesis on stainless steel grids. The catalysts demonstrated a 97% selectivity towards phenol formation at benzene conversion of 11%. In addition of achieving the same reactivity as over the traditional zeolitic fixed beds, these new catalytic packings present several advantages gained from the special arrangement of the catalytic bed like low pressure drop, improved heat and mass transfer, and controlled hydrodynamics.

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Selective oxidation of aromatic compounds on zeolites using N2O as a mild oxidant

Cited by 68 publications

References 6 publications

Benzene hydroxylation over FeZSM-5 catalysts: which Fe sites are active?

Benzene hydroxylation over FeZSM-5 catalysts: which Fe sites are active?

Active sites in HZSM-5 with low Fe content for the formation of surface oxygen by decomposing N2O: is every deposited oxygen active?

Synthesis of ZSM-5 coatings on stainless steel grids and their catalytic performance for partial oxidation of benzene by N2O

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