On the reducibility of sulfated Pt/CeXZr1−XO2 solids: A coupled thermogravimetric FT-IR study using CO as the reducing agent

Autor: Virginie Harle, Jean Claude Lavalley, A. M Le Govic, Philippe Bazin, Olivier Marie, Gilbert Blanchard, Marco Daturi, Odette Saur
Přispěvatelé: Laboratoire catalyse et spectrochimie (LCS), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Université de Caen Normandie (UNICAEN), Normandie Université (NU), RHODIA Res & Technol, PSA Peugeot Citroën, PSA Peugeot Citroën (PSA), Roland, Pascal
Rok vydání: 2012
Předmět:
Zdroj: Applied Catalysis B: Environmental
Applied Catalysis B: Environmental, Elsevier, 2012, 119 (DOI: 10.1016/j.apcatb.2012.02.037), pp.207--216
ISSN: 0926-3373
DOI: 10.1016/j.apcatb.2012.02.037
Popis: The reducibility of sulfate species by CO was studied over ceria and Ce0.63Zr0.37O2 mixed oxide with or without platinum, using infrared spectroscopy and thermogravimetry. The mechanism for sulfate reduction appeared to be based on three main points. Firstly, the exchange between surface and bulk-like sulfate species is required. The sulfate reduction indeed occurs at the oxide surface and bulk-like species need to migrate toward the surface to be further reduced. Secondly, it was observed that surface sulfate species are more easily reduced by CO on the reduced oxide. Therefore, platinum loading which favors the oxide reduction, also favors the sulfate reduction by CO. Finally, the reduction of sulfated Pt-free samples occurs in only one step, which is linked to the own reducibility of the surface sulfate species, probably through a direct interaction with CO. The amount of sulfur stored from sulfate reduction with CO is markedly more important than the one detected from reduction with H2. Furthermore, the oxygen storage capacity (OSC) for sulfated samples is higher than the one for sulfate-free samples. This is tentatively explained by the partial replacement of oxygen by sulfur atoms in the compound lattice.
Databáze: OpenAIRE