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Catalysts 2015, 5(1), 460-477; doi:10.3390/catal5010460

Structural Evolution under Reaction Conditions of Supported (NH4)3HPMo11VO40 Catalysts for the Selective Oxidation of Isobutane

1
CNRS UMR 8181, Unité de Catalyse et Chimie du Solide (UCCS), Université Lille 1 Sciences et Technologies, F-59655 Villeneuve d'Ascq Cedex, France
2
Ecole Centrale de Lille, ECLille, F-59651 Villeneuve d'Ascq, France
3
Ecole Nationale Supérieure de Chimie de Lille, ENSCL, F-59659 Villeneuve d'Ascq, France
4
Institut Universitaire de France, IUF, Maison des Universités, 103 Bd St-Michel, F-75005 Paris, France
*
Author to whom correspondence should be addressed.
Academic Editor: Keith Hohn
Received: 24 November 2014 / Revised: 28 February 2015 / Accepted: 6 March 2015 / Published: 23 March 2015
(This article belongs to the Special Issue Feature Papers to Celebrate the Landmarks of Catalysts)
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Abstract

When using heteropolycompounds in the selective oxidation of isobutane to methacrolein and methacrylic acid, both the keeping of the primary structure (Keggin units) and the presence of acidic sites are necessary to obtain the desired products. The structural evolution of supported (NH4)3HPMo11VO40 (APMV) catalysts under preliminary thermal oxidizing and reducing treatments was investigated. Various techniques, such as TGA/DTG (Thermo-Gravimetric Analysis/Derivative Thermo-Gravimetry), H2-TPR (Temperature Programed Reduction), in situ XRD (X-Ray Diffraction) and XPS (X-ray Photoelectron Spectroscopy), were applied. It was clearly evidenced that the thermal stability and the reducibility of the Keggin units are improved by supporting 40% APMV active phase on Cs3PMo12O40 (CPM). The partial degradation of APMV takes place depending on temperature and reaction conditions. The decomposition of ammonium cations (releasing NH3) leads to the formation of vacancies favoring cationic exchanges between vanadium coming from the active phase and cesium coming from the support. In addition, the vanadium expelled from the Keggin structure is further reduced to V4+, species, which contributes (with Mo5+) to activate isobutane. The increase in reducibility of the supported catalyst is assumed to improve the catalytic performance in comparison with those of unsupported APMV. View Full-Text
Keywords: isobutane; methacrylic acid; selective oxidation; characterization by in situ methods; heteropolymolybdates isobutane; methacrylic acid; selective oxidation; characterization by in situ methods; heteropolymolybdates
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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MDPI and ACS Style

Jing, F.; Katryniok, B.; Bordes-Richard, E.; Dumeignil, F.; Paul, S. Structural Evolution under Reaction Conditions of Supported (NH4)3HPMo11VO40 Catalysts for the Selective Oxidation of Isobutane. Catalysts 2015, 5, 460-477.

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