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The Evolution of the M1 Local Structure during Preparation of VMoNbTeO Catalysts for Ethane Oxidative Dehydrogenation to Ethylene Научная публикация

Журнал RSC Advances
ISSN: 2046-2069
Вых. Данные Год: 2018, Том: 8, Номер: 63, Страницы: 35903-35916 Страниц : 14 DOI: 10.1039/c8ra06424e
Ключевые слова Catalyst selectivity; Crystal structure; Dehydrogenation; Distribution functions; Ethane; Ethylene; Hydration; Tellurium compounds
Авторы Kardash T.Yu. 1 , Lazareva E.V. 1 , Svintsitskiy D.A. 1 , Ishchenko A.V. 1 , Bondareva V.M. 1 , Neder R.B. 2
Организации
1 Boreskov Institute of Catalysis SB RAS, Pr. Ak. Lavrentieva, 5, Novosibirsk, Russia
2 Friedrich-Alexander University of Erlangen-Nuremberg, Staudtstr. 3., 91058 Erlangen, Germany

Информация о финансировании (1)

1 Российский научный фонд 17-73-20073

Реферат: The so-called M1 phase (the common formula (TeO)x(Mo, V, Nb)5O14) is a very promising catalyst for ethane oxidative dehydrogenation (ODE). It shows 90% selectivity to ethylene at 78% ethane conversion (400 °C, contact time – 5.5 s). The active crystal structure is formed under certain synthetic conditions in VMoNbTe mixed oxides. This paper is devoted to the analysis of how the local and average structure of the M1 phase is developed during the synthesis and what happens at particular synthetic steps. The analysis of the local structure was performed using the EXAFS and pair distribution function (PDF) methods. The EXAFS analysis of the initial VMoTe water solution and VMoNbTe slurry showed that Anderson-type heteropoly anions are formed in the solution and are preserved after fast spray-drying of the slurry. Nb cations do not enter the structure of the polyanions, but form an extended hydrated oxide matrix, where distorted NbO6 and NbO7 polyhedrons are connected to each other. The hydrated oxide matrix with captured polyanions provides the compositional homogeneity of the precursor. The distances in the second coordination shell are redistributed after thermal treatment at 310 °C. After being heated at T > 350°, the local structure of the M1 phase is organized and pentagonal domains are formed. These domains consist of a NbO7 pentagonal bipyramid and five MeO6 adjacent octahedra (Me = Mo, V). In the first stages, the building blocks are stacked along the [001] direction. The crystallization process results in the connection of the pentagonal domains to the extended polygonal grid. The formation of the regular grid with TeOx containing channels is accompanied by the increase in ethane conversion and ethylene selectivity of the catalysts.
Библиографическая ссылка: Kardash T.Y. , Lazareva E.V. , Svintsitskiy D.A. , Ishchenko A.V. , Bondareva V.M. , Neder R.B.
The Evolution of the M1 Local Structure during Preparation of VMoNbTeO Catalysts for Ethane Oxidative Dehydrogenation to Ethylene
RSC Advances. 2018. V.8. N63. P.35903-35916. DOI: 10.1039/c8ra06424e WOS Scopus РИНЦ CAPlus PMID OpenAlex
Файлы: Полный текст от издателя
Даты:
Поступила в редакцию: 30 июл. 2018 г.
Принята к публикации: 11 окт. 2018 г.
Опубликована online: 22 окт. 2018 г.
Идентификаторы БД:
Web of science: WOS:000448663500006
Scopus: 2-s2.0-85056088522
РИНЦ: 38663170
Chemical Abstracts: 2018:1961311
PMID (PubMed): 35558492
OpenAlex: W2896842647
Цитирование в БД:
БД Цитирований
Web of science 28
Scopus 30
РИНЦ 27
OpenAlex 31
Альметрики: