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• W2000453191 abstract "Carboxylate species have been proposed as intermediates in the alcohol and/or hydrocarbon formation in the CO-H2 synthesis. Our aim was to study the evolution of acetates under CO-H2 reaction conditions. Acetic acid reacts with the catalytic surface at atmospheric pressure and at temperatures between 200 and 375°C, and has been chosen as precursor of these species. In this study we compare the evolution of acetic acid under argon or hydrogen on three (supported or not) metals: copper, iron and cobalt, which can give essentially three types of reactions: reduction, ketonization and methanation respectively. On cobalt and under argon, acetic acid decomposes with the formation of C02, CO, H2, H2O and C and the reaction is in accordance with a mechanism in which acetic anhydride is an intermediate. Under hydrogen, methanation becomes preponderant, this is again in agreement with a reaction scheme passing through acetic anhydride. On copper and under argon the acetate species are stable and the proposed mechanism explains the formation of C02, CH4, ketenes and of carbon deposits. Under hydrogen, the reduction to ethanol, acetaldehyde (and ethyl acetate) becomes effective with a selectivity higher than 93% and a conversion of 80%. On iron, the formation of acetone is selective under argon as well as under hydrogen, but the acetate species is not formed on this system, which is essentially constituted by Fe3O4. The difference between these three metals can be explained by the presence of acetate species on the surface. These species may or may not be formed (Fe3O4 ketonization, on clean cobalt surfaces) or may have very different stabilities: a very low one on cobalt, thus we have no reduction; a high one on copper, leading to a practically selective reduction. La réactivité de l'acide acétique sur systèmes catalytiques comportant trois métaux: cobalt, cuivre, fer a été étudiée sous argon et sous hydrogène dans le but d'éclairer le mécanisme de la réduction des espèces carboxylates en espèces éthoxy postulées dans le cadre de la croissance de chaîne en synthèse CO-H2. Selon la nature du métal trois réactions peuvent intervenir: méthanation (Co), reduction (Cu), cétonisation (Fe). Le comportement différent des trois métaux s'explique au niveau de l'éventuelle espèce acéte formée à la surface. Cette espèce peut soit ne pas être observée (Fe3O4, cétonisation pratiquement sélective, cobalt sur surface propre…), soit présenter une stabilité très différente: très faible stabilité sur cobalt ne permettant pas la rśduction, au contraire grande stabilité sur cuivre conditionnant une réduction pratiquement totale." @default.
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• W2000453191 date "1984-11-01" @default.
• W2000453191 modified "2023-09-23" @default.
• W2000453191 title "Evolution des especes carboxylates dans le cadre des syntheses CO-H2. Reduction de l'acide acetique sur systeme Co, Cu, Fe" @default.
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• W2000453191 doi "https://doi.org/10.1016/0254-0584(84)90065-8" @default.
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