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Antimony Oxide-Modified Vanadia-Based CatalystssPhysical Characterization and Catalytic Properties Научная публикация

Журнал The Journal of Physical Chemistry B
ISSN: 1520-6106 , E-ISSN: 1520-5207
Вых. Данные Год: 2001, Том: 105, Номер: 44, Страницы: 10772-10783 Страниц : 12 DOI: 10.1021/jp012228u
Ключевые слова SOLID-STATE REACTION; ORTHO-XYLENE; SELECTIVE OXIDATION; O CATALYSTS; V-51 NMR; SURFACE; AMMOXIDATION; REACTIVITY; V2O5; SPECTRA
Авторы Spengler J. 1 , Anderle F. 1 , Bosch E. 1 , Grasselli R.K. 1 , Pillep B. 2 , Behrens P. 2 , Lapina O.B. 3 , Shubin A.A. 3 , Eberle H.-J. 4 , Knözinger H. 1
Организации
1 Department Chemie, Universität München, Butenandtstrasse 5-13 (Haus E), 81377 München, Germany
2 Institut für Anorganische Chemie, Universität München, Meiserstrasse 1, 80333 München, Germany
3 Boreskov Institute of Catalysis, Pr. Akad. Lavrentieva 5, Novosibirsk 630090, Russia
4 Consortium für elektrochemische Industrie, Zielstattstrasse 20, 81379 München, Germany

Информация о финансировании (2)

1 International Association for the Promotion of Co-operation with Scientists from the New Independent States of the Former Soviet Union IR-97-0059
2 Российский фонд фундаментальных исследований 01-03-32364

Реферат: Antimony-modified vanadia-on-titania catalysts were prepared for the selective oxidation of o-xylene to phthalic anhydride by ball milling of powder mixtures followed by calcination. A binary Sb2O3−V2O5 system was also prepared for comparison purposes. The resulting materials were physically characterized by surface area measurements, X-ray diffraction analysis (XRD), laser Raman spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, electron spin resonance (ESR), magnetic susceptibility determination, and 15V solid-state NMR. The catalytic performance of the TiO2-supported materials was tested for o-xylene oxidation. After calcination of the Sb2O3−V2O5 binary mixture at 673 K, Sb3+ is almost quantitatively oxidized to Sb5+, while both V3+ and V4+ are detected. V3+ and some V4+ are most likely located in a nonstoichiometric VSbO4-like structure, while the majority of V4+ preferentially concentrates within shear domains in oxygen-deficient V2O5-x particles. In the titania-supported catalyst system, both Sb2O3 and V2O5 spread on the anatase surface. Sb3+ is oxidized to Sb5+, and V3+, V4+, and V5+ are detected. VSbO4-like structures are not observed. The presence of antimony leads to the formation of presumably V3+−O−V5+ redox couples. The paramagnetic centersin contrast to the binary mixtureare largely isolated. Antimony preferentially migrates to the surface and appears to exhibit a dual function catalytically. It is inferred from the experimental data that the addition of antimony leads to site isolation and to a reduction of surface acidity. We suggest that V−O−V−O−V domains or clusters are interrupted by incorporation of Sb to form V−O−Sb−O−V species. As a consequence of this site isolation and a reduction of surface acidity, overoxidation of o-xylene is reduced. These two effects are therefore most probably responsible for the improved selectivity of the ternary catalyst system over the binary one toward phthalic anhydride.
Библиографическая ссылка: Spengler J. , Anderle F. , Bosch E. , Grasselli R.K. , Pillep B. , Behrens P. , Lapina O.B. , Shubin A.A. , Eberle H.-J. , Knözinger H.
Antimony Oxide-Modified Vanadia-Based CatalystssPhysical Characterization and Catalytic Properties
The Journal of Physical Chemistry B. 2001. V.105. N44. P.10772-10783. DOI: 10.1021/jp012228u WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
Поступила в редакцию: 13 июн. 2001 г.
Опубликована в печати: 1 нояб. 2001 г.
Идентификаторы БД:
Web of science: WOS:000172049100006
Scopus: 2-s2.0-0035829918
РИНЦ: 41817433
Chemical Abstracts: 2001:722188
Chemical Abstracts (print): 136:20263
OpenAlex: W1985084446
Цитирование в БД:
БД Цитирований
Web of science 46
Scopus 55
РИНЦ 52
OpenAlex 51
Альметрики: