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Dry reforming of methane over LaNi1?yByO3±δ (B = Mg,Co) perovskites used as catalyst precursor
Authors:Germán Sierra Gallego  Catherine Batiot-Dupeyrat  Joël Barrault  Elizabeth Florez  Fanor Mondragón
Affiliation:1. Institute of Chemistry, University of Antioquia, A.A. 1226, Medellín, Colombia;2. Laboratoire de Catalyse en Chimie Organique, UMR CNRS 6503, Université de Poitiers, Ecole Supérieure d’Ingénieurs de Poitiers, 40, Avenue du Recteur Pineau, 86022 Poitiers Cedex, France;1. Technische Universität Berlin, Fakultät II, Institut für Chemie, Sekretariat TC 8, Straße des 17, Juni 124, 10623 Berlin, Germany;2. Technische Universität Berlin, Fakultät II, Institut für Chemie, Sekretariat BA 2, Hardenbergstraße 40, 10623 Berlin, Germany;1. Institut de Chimie des Milieux et Matériaux de Poitiers (IC2MP), Ecole Nationale Supérieure d''Ingénieurs de Poitiers (ENSIP), Université de Poitiers—UMR CNRS 7285, 1 rue Marcel Doré, TSA 41105, 86073 Poitiers cedex 9, France;2. Laboratory LGCVR UAE/L01FST, Faculty of Sciences and Techniques of Tangier, University Abdelmalek Essaadi, Tangier, Morocco;3. Unité de Catalyse et de Chimie du solide (UCCS), Université de Lille 1- UMR CNRS 8181, Cité scientifique Bat C3, 59655 Villeneuve d’Ascq, France;1. Department of Chemical and Process Engineering, University of Surrey, Guildford, GU2 7XH, United Kingdom;2. Laboratorio de Materiales Avanzados, Departamento de Química Inorgánica - Instituto Universitario de Materiales de Alicante Universidad de Alicante, Apartado 99, E-03080 Alicante, Spain;3. Department of Chemistry, University of Surrey, Guildford, GU2 7XH, United Kingdom
Abstract:Perovskites LaNiO3, LaNi1?xMgxO3?δ and LaNi1?xCoxO3?δ were synthesized by auto combustion method. TPR analysis reveled that Mg or Co substituted perovskites were more difficult to reduce. The perovskites were evaluated as catalyst precursors in the dry reforming of methane. Catalysts obtained by reduction of LaNiO3 and LaNi1?xMgxO3?δ perovskite had the highest catalytic activity for CO2 reforming of CH4 at 700 °C using drastic reaction conditions (10 mg of catalyst, a mixture of CH4/CO2 without dilution gas). Methane and carbon dioxide conversions were 57% and 67%, respectively, with a H2/CO ratio equal to 0.47.The presence of cobalt leads to a decrease of the catalytic activity. This decreasing of activity may be attributed to the Co–Ni alloy formation. Computational calculations revealed that Ni atom cleaves the C–H atom while Co is not able to activate the CH4 molecule. The interaction energy of CH4 with the Ni and CO atom was 18 kcal/mol and 0.7 kcal/mol, respectively.The catalysts were characterized by TPR, TEM and in situ XRD.
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