Single-Site VOx Moieties Generated on Silica by Surface Organometallic Chemistry: A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane

Samir Barman; Niladri Maity; Kushal Bhatte; Samy Ould-Chikh; Oliver Dachwald; Carmen Haeßner; Youssef Saih; Edy Abou-Hamad; Isabelle Llorens; Jean Louis Hazemann; Klaus Köhler; Valerio D'Elia; Jean Marie Basset

doi:10.1021/acscatal.6b01263

Single-Site VO_x Moieties Generated on Silica by Surface Organometallic Chemistry: A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane

Samir Barman, Niladri Maity, Kushal Bhatte, Samy Ould-Chikh, Oliver Dachwald, Carmen Haeßner, Youssef Saih, Edy Abou-Hamad, Isabelle Llorens, Jean Louis Hazemann, Klaus Köhler, Valerio D'Elia^*, Jean Marie Basset

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

85 Scopus citations

Abstract

We report here an accurate surface organometallic chemistry (SOMC) approach to propane oxidative dehydrogenation (ODH) using a μ²-oxo-bridged, bimetallic [V₂O₄(acac)₂] (1) (acac = acetylacetonate anion) complex as a precursor. The identity and the nuclearity of the product of grafting and of the subsequent oxidative treatment have been systematically studied by means of FT-IR, Raman, solid-state (SS) NMR, UV-vis DRS, EPR and EXAFS spectroscopies. We show that the grafting of 1 on the silica surface under a rigorous SOMC protocol and the subsequent oxidative thermal treatment lead exclusively to well-defined and isolated monovanadate species. The resulting material has been tested for the oxidative dehydrogenation of propane in a moderate temperature range (400-525 °C) and compared with that of silica-supported vanadium catalysts prepared by the standard impregnation technique. The experimental results show that the catalytic activity in propane ODH is strongly upgraded by the degree of isolation of the VO_x species that can be achieved by employing the SOMC protocol.

Original language	English
Pages (from-to)	5908-5921
Number of pages	14
Journal	ACS Catalysis
Volume	6
Issue number	9
DOIs	https://doi.org/10.1021/acscatal.6b01263
State	Published - 2 Sep 2016
Externally published	Yes

Bibliographical note

Funding Information:
The research was supported by the King Abdullah University of Science and Technology (KAUST). O.D. would like to thank KAUST ORS for research support.

Publisher Copyright:
© 2016 American Chemical Society.

Keywords

olefins
oxidative dehydrogenation
propylene production
silica-supported vanadium catalysts
single-site catalysis
surface organometallic chemistry

ASJC Scopus subject areas

Catalysis
General Chemistry

Access to Document

10.1021/acscatal.6b01263

Cite this

Barman, S., Maity, N., Bhatte, K., Ould-Chikh, S., Dachwald, O., Haeßner, C., Saih, Y., Abou-Hamad, E., Llorens, I., Hazemann, J. L., Köhler, K., D'Elia, V., & Basset, J. M. (2016). Single-Site VO_x Moieties Generated on Silica by Surface Organometallic Chemistry: A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane. ACS Catalysis, 6(9), 5908-5921. https://doi.org/10.1021/acscatal.6b01263

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title = "Single-Site VOx Moieties Generated on Silica by Surface Organometallic Chemistry: A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane",

abstract = "We report here an accurate surface organometallic chemistry (SOMC) approach to propane oxidative dehydrogenation (ODH) using a μ2-oxo-bridged, bimetallic [V2O4(acac)2] (1) (acac = acetylacetonate anion) complex as a precursor. The identity and the nuclearity of the product of grafting and of the subsequent oxidative treatment have been systematically studied by means of FT-IR, Raman, solid-state (SS) NMR, UV-vis DRS, EPR and EXAFS spectroscopies. We show that the grafting of 1 on the silica surface under a rigorous SOMC protocol and the subsequent oxidative thermal treatment lead exclusively to well-defined and isolated monovanadate species. The resulting material has been tested for the oxidative dehydrogenation of propane in a moderate temperature range (400-525 °C) and compared with that of silica-supported vanadium catalysts prepared by the standard impregnation technique. The experimental results show that the catalytic activity in propane ODH is strongly upgraded by the degree of isolation of the VOx species that can be achieved by employing the SOMC protocol.",

keywords = "olefins, oxidative dehydrogenation, propylene production, silica-supported vanadium catalysts, single-site catalysis, surface organometallic chemistry",

author = "Samir Barman and Niladri Maity and Kushal Bhatte and Samy Ould-Chikh and Oliver Dachwald and Carmen Hae{\ss}ner and Youssef Saih and Edy Abou-Hamad and Isabelle Llorens and Hazemann, {Jean Louis} and Klaus K{\"o}hler and Valerio D'Elia and Basset, {Jean Marie}",

note = "Funding Information: The research was supported by the King Abdullah University of Science and Technology (KAUST). O.D. would like to thank KAUST ORS for research support. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

year = "2016",

month = sep,

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doi = "10.1021/acscatal.6b01263",

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Barman, S, Maity, N, Bhatte, K, Ould-Chikh, S, Dachwald, O, Haeßner, C, Saih, Y, Abou-Hamad, E, Llorens, I, Hazemann, JL, Köhler, K, D'Elia, V & Basset, JM 2016, 'Single-Site VO_x Moieties Generated on Silica by Surface Organometallic Chemistry: A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane', ACS Catalysis, vol. 6, no. 9, pp. 5908-5921. https://doi.org/10.1021/acscatal.6b01263

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T1 - Single-Site VOx Moieties Generated on Silica by Surface Organometallic Chemistry

T2 - A Way to Enhance the Catalytic Activity in the Oxidative Dehydrogenation of Propane

AU - Barman, Samir

AU - Maity, Niladri

AU - Bhatte, Kushal

AU - Ould-Chikh, Samy

AU - Dachwald, Oliver

AU - Haeßner, Carmen

AU - Saih, Youssef

AU - Abou-Hamad, Edy

AU - Llorens, Isabelle

AU - Hazemann, Jean Louis

AU - Köhler, Klaus

AU - D'Elia, Valerio

AU - Basset, Jean Marie

N1 - Funding Information: The research was supported by the King Abdullah University of Science and Technology (KAUST). O.D. would like to thank KAUST ORS for research support. Publisher Copyright: © 2016 American Chemical Society.

PY - 2016/9/2

Y1 - 2016/9/2

N2 - We report here an accurate surface organometallic chemistry (SOMC) approach to propane oxidative dehydrogenation (ODH) using a μ2-oxo-bridged, bimetallic [V2O4(acac)2] (1) (acac = acetylacetonate anion) complex as a precursor. The identity and the nuclearity of the product of grafting and of the subsequent oxidative treatment have been systematically studied by means of FT-IR, Raman, solid-state (SS) NMR, UV-vis DRS, EPR and EXAFS spectroscopies. We show that the grafting of 1 on the silica surface under a rigorous SOMC protocol and the subsequent oxidative thermal treatment lead exclusively to well-defined and isolated monovanadate species. The resulting material has been tested for the oxidative dehydrogenation of propane in a moderate temperature range (400-525 °C) and compared with that of silica-supported vanadium catalysts prepared by the standard impregnation technique. The experimental results show that the catalytic activity in propane ODH is strongly upgraded by the degree of isolation of the VOx species that can be achieved by employing the SOMC protocol.

AB - We report here an accurate surface organometallic chemistry (SOMC) approach to propane oxidative dehydrogenation (ODH) using a μ2-oxo-bridged, bimetallic [V2O4(acac)2] (1) (acac = acetylacetonate anion) complex as a precursor. The identity and the nuclearity of the product of grafting and of the subsequent oxidative treatment have been systematically studied by means of FT-IR, Raman, solid-state (SS) NMR, UV-vis DRS, EPR and EXAFS spectroscopies. We show that the grafting of 1 on the silica surface under a rigorous SOMC protocol and the subsequent oxidative thermal treatment lead exclusively to well-defined and isolated monovanadate species. The resulting material has been tested for the oxidative dehydrogenation of propane in a moderate temperature range (400-525 °C) and compared with that of silica-supported vanadium catalysts prepared by the standard impregnation technique. The experimental results show that the catalytic activity in propane ODH is strongly upgraded by the degree of isolation of the VOx species that can be achieved by employing the SOMC protocol.

KW - olefins

KW - oxidative dehydrogenation

KW - propylene production

KW - silica-supported vanadium catalysts

KW - single-site catalysis

KW - surface organometallic chemistry

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DO - 10.1021/acscatal.6b01263

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JO - ACS Catalysis

JF - ACS Catalysis

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