Highly productive iron molybdate mixed oxides and their relevant catalytic properties for direct synthesis of 1,1-dimethoxymethane from methanol
| Autor: | Franck Dumeignil, Jean-Luc Dubois, Louise Jalowiecki-Duhamel, Hervé Vezin, Mickaël Capron, Anne-Sophie Mamede, Jérémy Faye, Martine Trentesaux, Kaew-arpha Thavornprasert, Nadia Touati, Ge Fang, Olivier Gardoll, Jean-Luc Couturier |
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| Přispěvatelé: | Unité de Catalyse et Chimie du Solide - UMR 8181 (UCCS), Centrale Lille Institut (CLIL)-Université d'Artois (UA)-Centrale Lille-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Lille, Université Lille Nord de France (COMUE), Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 (LASIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Centrale Lille Institut (CLIL), Arkema, Arkema (Arkema), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Centre de recherche Rhône-Alpes (CRRA), Université d'Artois (UA)-Centrale Lille-Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS) |
| Rok vydání: | 2014 |
| Předmět: |
Inorganic chemistry
chemistry.chemical_element 02 engineering and technology Molybdate 010402 general chemistry 7. Clean energy 01 natural sciences Oxygen Redox Catalysis Acetalization chemistry.chemical_compound Iron molybdate catalysts X-ray photoelectron spectroscopy Lewis acids and bases General Environmental Science Chemistry 1-Dimethoxymethane Process Chemistry and Technology Methanol oxidation 021001 nanoscience & nanotechnology 0104 chemical sciences [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry Dimethoxymethane Methanol 0210 nano-technology |
| Zdroj: | Applied Catalysis B: Environmental Applied Catalysis B: Environmental, Elsevier, 2014, 145, pp.126-135. ⟨10.1016/j.apcatb.2013.01.043⟩ Applied Catalysis B: Environmental, 2014, 145, pp.126-135. ⟨10.1016/j.apcatb.2013.01.043⟩ |
| ISSN: | 0926-3373 |
| DOI: | 10.1016/j.apcatb.2013.01.043 |
| Popis: | The one-step gas phase conversion of methanol to 1,1-dimethoxymethane (DMM) was studied over highly productive iron molybdate mixed oxides in a fixed-bed reactor working at atmospheric pressure. When placing the Fe-Mo-O catalyst under a reaction mixture highly concentrated in methanol, the DMM selectivity was drastically boosted. This specific and unique feature encouraged us to extensively characterize this family of particular catalysts. LEIS analysis revealed the presence of both Mo and Fe species on the outermost atomic layer of the catalysts. X-ray photoelectron spectroscopy (XPS) and in situ EPR measurements showed that the Fe centres are responsible for the redox properties. The acidic properties of the FeMo mixed oxides were then attributed to anionic vacancies acting as Lewis acid sites produced by dehydroxylation of the catalyst surface. XPS analysis also showed that oxygen from the gas phase was responsible for reoxidation of the catalyst surface with regeneration of the active sites, which suggests a Mars-van Krevelen mechanism. The good catalytic performances were then attributed to a synergistic effect between Mo and Fe species. A Mo/Fe molar ratio of 3.2 for an optimal remarkable yield in DMM of 50% was found. |
| Databáze: | OpenAIRE |
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