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CO2 -to-Methanol Hydrogenation on Zirconia-Supported Copper Nanoparticles: Reaction Intermediates and the Role of the Metal-Support Interface.
Larmier, Kim; Liao, Wei-Chih; Tada, Shohei; Lam, Erwin; Verel, René; Bansode, Atul; Urakawa, Atsushi; Comas-Vives, Aleix; Copéret, Christophe.
Afiliación
  • Larmier K; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Liao WC; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Tada S; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Lam E; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Verel R; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Bansode A; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
  • Urakawa A; Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, Av. Països Catalans 16, 43007, Tarragona, Spain.
  • Comas-Vives A; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
  • Copéret C; Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog Weg 1-5, 8093, Zürich, Switzerland.
Angew Chem Int Ed Engl ; 56(9): 2318-2323, 2017 02 20.
Article en En | MEDLINE | ID: mdl-28111850
Methanol synthesis by CO2 hydrogenation is a key process in a methanol-based economy. This reaction is catalyzed by supported copper nanoparticles and displays strong support or promoter effects. Zirconia is known to enhance both the methanol production rate and the selectivity. Nevertheless, the origin of this observation and the reaction mechanisms associated with the conversion of CO2 to methanol still remain unknown. A mechanistic study of the hydrogenation of CO2 on Cu/ZrO2 is presented. Using kinetics, in situ IR and NMR spectroscopies, and isotopic labeling strategies, surface intermediates evolved during CO2 hydrogenation were observed at different pressures. Combined with DFT calculations, it is shown that a formate species is the reaction intermediate and that the zirconia/copper interface is crucial for the conversion of this intermediate to methanol.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2017 Tipo del documento: Article País de afiliación: Suiza Pais de publicación: Alemania
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2017 Tipo del documento: Article País de afiliación: Suiza Pais de publicación: Alemania