Hydrocarbon Oxidation over Fe- and Cr-Containing Metal-Organic Frameworks MIL-100 and MIL-101– A Comparative Study | Sciact - CRIS-система Института катализа

Hydrocarbon Oxidation over Fe- and Cr-Containing Metal-Organic Frameworks MIL-100 and MIL-101– A Comparative Study Научная публикация

Конференция

7th World Congress on Oxidation Catalysis
09-12 июн. 2013 , Saint Louis

Журнал

Catalysis Today
ISSN: 0920-5861 , E-ISSN: 1873-4308

Вых. Данные

Год: 2014, Том: 238, Страницы: 54-61 Страниц : 8 DOI: 10.1016/j.cattod.2014.01.010

Ключевые слова

Alkenes, Anthracene, Heterogeneous catalysis, MIL-100, MIL-101, Selective oxidation

Авторы

Kholdeeva Oxana A. ^1,2 , Skobelev Igor Y. ¹ , Ivanchikova Irina D. ¹ , Kovalenko Konstantin A. ^2,3 , Fedin Vladimir P. ^2,3 , Sorokin Alexander B. ⁴

Организации

1	Boreskov Institute of Catalysis, Lavrentiev ave. 5, Novosibirsk 630090, Russia
2	Novosibirsk State University, Pirogova st. 2, Novosibirsk 630090, Russia
3	Nikolaev Institute of Inorganic Chemistry, Lavrentiev ave. 3, Novosibirsk 630090, Russia
4	Institut de Recherches sur la Catalyse et l’Environnement de Lyon (IRCELYON), UMR 5256, CNRS-Université Lyon 1, 2, av. A. Einstein, 69626 Villeurbanne Cedex, France

Информация о финансировании (3)

1	Российский фонд фундаментальных исследований	13-03-00413
2	Министерство образования и науки Российской Федерации
3	Посольство Франции в России

Catalytic properties of Fe- and Cr-based metal-organic frameworks (MOFs) MIL-100 and MIL-101 have been assessed in two liquid-phase reactions: solvent-free allylic oxidation of alkenes (cyclohexene, α- and β-pinenes) with molecular oxygen and oxidation of anthracene (AN) with tert-butyl hydroperoxide (TBHP). In the oxidation of alkenes, the product selectivity strongly depends on the nature of metal (Fe or Cr) but, for the same metal, only slightly differs for the MIL-100 and MIL-101 structures. The Fe-containing MOFs afford the formation of unsaturated alcohols while Cr-based MOFs give mainly unsaturated ketones. Both Cr-MIL-100 and Cr-MIL-101 favor decomposition of cyclohexenyl hydroperoxide to produce 2-cyclohexen-1-one with 67–69% selectivity. Stability toward destruction reduced in the order Cr-MIL-101, Cr-MIL-100 > Fe-MIL-100 > Fe-MIL-101. In the oxidation of anthracene over both Cr-MOFs and Fe-MIL-101, the selectivity toward 9,10-anthraquinone (AQ) attained 100% at 92–100% AN conversion. The turnover frequency (TOF) decreased in the order Cr-MIL-101 > Fe-MIL-101 > Cr-MIL-100 > Fe-MIL-100. Cr-MIL-101 revealed superior catalytic performance in terms of AN conversion, AQ selectivity and TOF. Nearly quantitative yield of AQ was obtained after 1.5 h at 100 °C in chlorobenzene as solvent. No leaching of active metal occurred under optimal reaction conditions and the MOFs could be recycled several times without deterioration of the catalytic properties.

Kholdeeva O.A. , Skobelev I.Y. , Ivanchikova I.D. , Kovalenko K.A. , Fedin V.P. , Sorokin A.B.
Hydrocarbon Oxidation over Fe- and Cr-Containing Metal-Organic Frameworks MIL-100 and MIL-101– A Comparative Study
Catalysis Today. 2014. V.238. P.54-61. DOI: 10.1016/j.cattod.2014.01.010 WOS Scopus РИНЦ CAPlusCA OpenAlex

Поступила в редакцию:	1 дек. 2013 г.
Принята к публикации:	14 янв. 2014 г.
Опубликована online:	13 февр. 2014 г.
Опубликована в печати:	1 дек. 2014 г.

Web of science:	WOS:000341878600008
Scopus:	2-s2.0-84907712175
РИНЦ:	23992980
Chemical Abstracts:	2014:251003
Chemical Abstracts (print):	161:566426
OpenAlex:	W2060605455

БД	Цитирований
Web of science	104
Scopus	113
РИНЦ	100
OpenAlex	111