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New Reaction of Anion Radicals O− with Water on the Surface of FeZSM-5 Научная публикация

Общее Язык: Английский, Жанр: Статья (Full article),
Статус опубликования: Опубликована, Оригинальность: Оригинальная
Журнал Journal of Catalysis
ISSN: 0021-9517 , E-ISSN: 1090-2694
Вых. Данные Год: 2008, Том: 254, Номер: 1, Страницы: 110-120 Страниц : 11 DOI: 10.1016/j.jcat.2007.12.001
Ключевые слова α-Oxygen, Anion radical O-, DRIFT spectroscopy, FeZSM-5, N2O, Photocatalytic oxidation
Авторы Panov Gennady I. 1 , Starokon Eugeny V. 1 , Pirutko Larisa V. 1 , Paukshtis Eugeny A. 1 , Parmon Valentin N. 1
Организации
1 Институт катализа им. Г.К. Борескова СО РАН

Информация о финансировании (2)

1 Российский фонд фундаментальных исследований 06-03-72551
2 Российский фонд фундаментальных исследований 06-03-33087

Реферат: Complexes of bivalent iron stabilized in the FeZSM-5 zeolite matrix (α-sites) are known to be able to decompose nitrous oxide stoichiometrically to form oxygen anion radicals, O−, bound to iron (α-oxygen), (FeII)α + N2O → (FeIIIsingle bondO−)α + N2. Similar to O− radicals on V and Mo oxides, α-oxygen is highly reactive in respect to CO, H2, methane and other hydrocarbons. It participates in catalytic oxidation of benzene to phenol by nitrous oxide, providing selectivity close to 100%. In this work, adsorption measurements, IR spectroscopy, TPD, and isotope methods were used to describe an earlier unknown reaction of O− species with water, which proceeds at 5–200 °C via the hydrogen abstraction mechanism according to the equation 2(FeIIIsingle bondO−)α + H2O → 2(FeIIIsingle bondOH−)α + (1/2)O2. The reaction leads to the hydroxyl groups formed on α-sites, and equivalent amount of O2 evolves into the gas phase from water. Desorption of the hydroxyl groups occurs at above 400 °C via their recombination into water and dioxygen, resulting in the reactivation of α-sites, 2(FeIIIsingle bondOH−)α → 2(FeII)α + H2O + (1/2)O2. High sensitivity of α-oxygen to water admixtures may be an important factor explaining some contradictory results reported in the literature on the behavior of α-oxygen. Because α-oxygen is a typical representative of anion radicals O−, this reaction may be relevant not only to the conventional oxidation catalysis over zeolites and metal oxides, but also to photocatalytic processes, where formation of O− is well documented.
Библиографическая ссылка: Panov G.I. , Starokon E.V. , Pirutko L.V. , Paukshtis E.A. , Parmon V.N.
New Reaction of Anion Radicals O− with Water on the Surface of FeZSM-5
Journal of Catalysis. 2008. V.254. N1. P.110-120. DOI: 10.1016/j.jcat.2007.12.001 WOS Scopus РИНЦ
Даты:
Поступила в редакцию: 17 сент. 2007 г.
Принята к публикации: 5 дек. 2007 г.
Опубликована online: 8 янв. 2008 г.
Опубликована в печати: 15 февр. 2008 г.
Идентификаторы:
Web of science WOS:000253646100012
Scopus 2-s2.0-38649087046
РИНЦ 13582348
Chemical Abstracts 2008:152527
Chemical Abstracts (print) 148:411737
Альметрики: