Toluene total oxidation over Pd and Au nanoparticles supported on hydroxyapatite
Comptes Rendus Chimie, ISSN: 1631-0748, Vol: 19, Issue: 4, Page: 525-537
2016
- 37Citations
- 26Captures
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Article Description
The total oxidation of toluene was carried out in a series of catalytic systems composed of either palladium or gold, as active phase, with hydroxyapatite as supports. The influence of different parameters on the catalytic reactivity was investigated: the type of support, the active phase content, the preparation method, and the nature of the active phase. Hydroxyapatite supports, impregnated by the active phase, showed better reactivities than that of the classical alumina one. Moreover, low palladium content (0.25 wt%) is enough to get high toluene conversions at low temperatures. Two preparation methods were used to introduce the active phase on the support: the conventional wet impregnation and the nanoparticle deposition achieved by impregnation of a colloidal suspension of the noble metal using the surfactant HEA16Cl. Introducing palladium by either of these methods leads to similar catalytic efficiencies. In addition to this, palladium is much more active than gold, gold was not probably present under the form of highly dispersed nanoparticles. X-ray Photoelectron Spectroscopy (XPS) evidenced PdO presence on the surface of all our catalysts. Palladium impregnated on apatite by conventional method showed an improvement of catalytic reactivity after 13 h under reacting mixture, probably because of Pd(0) formation besides PdO. As a result and after a literature survey, our catalysts could be classified among the most reactive systems towards total oxidation of toluene. L’oxydation totale du toluène a été étudiée sur la phase active palladium ou or supportée sur différents supports de type hydroxyapatite. L’influence de différents paramètres sur la réactivité catalytique a été étudiée : le type de support, la teneur de la phase active, la méthode de préparation et la nature de la phase active. Les supports hydroxyapatite ont montré de meilleures performances que le support classique alumine. De plus, une teneur en palladium de 0,25 % en masse est suffisante pour obtenir des conversions de toluène élevées à de faibles températures. Deux méthodes de préparation ont été utilisées pour introduire la phase active : l’imprégnation par voie humide conventionnelle et le dépôt de nanoparticules par imprégnation d’une suspension colloïdale du métal noble en utilisant le HEA16Cl comme surfactant. L’introduction du palladium par l’une ou l’autre de ces méthodes conduit à des performances catalytiques similaires. Les résultats obtenus ont montré que le palladium est plus réactif que l’or, l’or ne se trouvant pas, probablement, sous forme de nanoparticules hautement dispersées. L’étude par spectroscopie de photoélectrons induits par rayons X (SPX) a révélé l’existence en surface de la seule espèce PdO sur tous nos catalyseurs. Le système palladium imprégné sur le support hydroxyapatite par méthode conventionnelle a montré une augmentation de la conversion du toluène après 13 h sous flux réactionnel, probablement suite à la formation d’espèces Pd(0) et leur coexistence avec PdO. Finalement, nos systèmes catalytiques se sont avérés être parmi les meilleurs parmi ceux étudiés dans la littérature portant sur l’oxydation totale du toluène.
Bibliographic Details
http://www.sciencedirect.com/science/article/pii/S1631074816000035; http://dx.doi.org/10.1016/j.crci.2015.07.015; http://www.scopus.com/inward/record.url?partnerID=HzOxMe3b&scp=84958225136&origin=inward; https://comptes-rendus.academie-sciences.fr/chimie/articles/10.1016/j.crci.2015.07.015/; https://dx.doi.org/10.1016/j.crci.2015.07.015
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