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Highly Efficient Catalysts Based on Divanadium-Substituted Polyoxometalate and N-Doped Carbon Nanotubes for Selective Oxidation of Alkylphenols Научная публикация

Журнал ACS Catalysis
ISSN: 2155-5435
Вых. Данные Год: 2018, Том: 8, Страницы: 1297-1307 Страниц : 11 DOI: 10.1021/acscatal.7b03933
Ключевые слова alkylphenols, benzoquinones, carbon nanotubes, heterogeneous catalysis, hydrogen peroxide, nitrogen-doped, polyoxometalate, selective oxidation
Авторы Evtushok Vasiliy Yu. 1,2 , Suboch Arina N. 1,2 , Podyacheva Olga Yu. 1,2 , Stonkus Olga A. 1,2 , Zaikovskii Vladimir I. 1,2 , Chesalov Yurii A. 1,2 , Kibis Lidiya S. 1,2 , Kholdeeva Oxana A. 1,2
Организации
1 Boreskov Institute of Catalysis, Lavrentieva ave. 5, Novosibirsk 630090, Russia
2 Novosibirsk State University, Pirogova str. 2, Novosibirsk 630090, Russia

Информация о финансировании (1)

1 Федеральное агентство научных организаций России 0303-2016-0005

Реферат: Alkyl-substituted benzoquinones serve as versatile building blocks for a variety of biologically active compounds. In this work, we present an approach for the environmentally benign synthesis of alkyl-p-benzoquinones, in particular trimethyl-p-benzoquinone (TMBQ, vitamin E precursor), which employs aqueous hydrogen peroxide as oxidant and a divanadium-substituted γ-Keggin polyoxotungstate, [γ-PW10O38V2(μ-O)(μ–OH)]4– (V2-POM), immobilized on nitrogen-doped carbon nanotubes (N-CNTs) as heterogeneous catalyst. A series of supported catalysts V2-POM/N-CNTs containing 5–25 wt % of V2-POM and 0–4.8 atom % of N has been prepared and characterized by elemental analysis, N2 adsorption, SEM, TEM, XPS, and FTIR techniques. The catalytic performance of V2-POM/N-CNTs was assessed in the selective oxidation of 2,3,6-trimethylphenol (TMP) with H2O2 under mild reaction conditions (60 °C, MeCN). The presence of nitrogen in the support ensures strong adsorption and molecular dispersion of V2-POM on the carbon surface, leading to highly active and selective heterogeneous catalysts, which do not suffer from metal leaching and can be used repeatedly without loss of the catalytic performance. By application of the optimal catalyst V2-POM/N-CNTs enclosing 15 wt % of V2-POM and 1.8 atom % of N, TMBQ could be obtained with 99% yield and 80% oxidant utilization efficiency. The catalyst demonstrated the truly heterogeneous nature of the catalysis and high turnover frequencies (500 h–1) and space–time yield (450 g L–1 h–1). FTIR and XPS techniques confirmed the stability of V2-POM and N-CNT support under the turnover conditions.
Библиографическая ссылка: Evtushok V.Y. , Suboch A.N. , Podyacheva O.Y. , Stonkus O.A. , Zaikovskii V.I. , Chesalov Y.A. , Kibis L.S. , Kholdeeva O.A.
Highly Efficient Catalysts Based on Divanadium-Substituted Polyoxometalate and N-Doped Carbon Nanotubes for Selective Oxidation of Alkylphenols
ACS Catalysis. 2018. V.8. P.1297-1307. DOI: 10.1021/acscatal.7b03933 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: 17 нояб. 2017 г.
Опубликована online: 19 янв. 2018 г.
Опубликована в печати: 2 февр. 2018 г.
Идентификаторы БД:
Web of science: WOS:000424735000070
Scopus: 2-s2.0-85041417110
РИНЦ: 35484691
Chemical Abstracts: 2018:18142
Chemical Abstracts (print): 168:158111
OpenAlex: W2782050299
Цитирование в БД:
БД Цитирований
Web of science 73
Scopus 76
РИНЦ 74
OpenAlex 78
Альметрики: