INTEC   05402
INSTITUTO DE DESARROLLO TECNOLOGICO PARA LA INDUSTRIA QUIMICA
Unidad Ejecutora - UE
congresos y reuniones científicas
Título:
The Role of Formate Groups in the Mechanism of metanol Síntesis from H2/CO2 over a Pd/Ga2O3 Catalyst
Autor/es:
SEBASTIÁN E. COLLINS; MIGUEL A. BALTANÁS; ADRIAN L. BONIVARDI; LAURA E. BRIAND; LUIS A. GAMBARO
Lugar:
Toledo, España
Reunión:
Congreso; Second International Congress on Operando Spectroscopy; 2006
Institución organizadora:
Instituto de Catálisis y Petroleoquimica, CSIC, Madrid, España
Resumen:
To understand the mechanism of methanol synthesis from CO2 hydrogenation, we previously performed infrared in-situ temperature programmed reaction experiments using H2 and CO2 (323-723 K, 0.1 MPa) over a model Pd/Ga2O3 catalyst. A bifunctional scheme was proposed, where: i) carbon dioxide chemisorbs (weakly) on the galia surface as (bi)carbonate species, which are stepwise hydrogenated to monodentate and bidentate formate species (m-HCOO resp. b-HCOO), methylenebisoxy (H2COO), methoxy (CH3O) and, finally methanol, and ii) Pd provides surface atomic hydrogen for CO2 reduction by spillover. Additionally, an interconversion between b-HCOO and m-HCOO was suggested, where b-HCOO appears to be a spectator, while m-HCOO seems to be the most reactive intermediate. Therefore it was deemed reasonable to further investigate the role of the formate groups in the methanol synthesis.2 hydrogenation, we previously performed infrared in-situ temperature programmed reaction experiments using H2 and CO2 (323-723 K, 0.1 MPa) over a model Pd/Ga2O3 catalyst. A bifunctional scheme was proposed, where: i) carbon dioxide chemisorbs (weakly) on the galia surface as (bi)carbonate species, which are stepwise hydrogenated to monodentate and bidentate formate species (m-HCOO resp. b-HCOO), methylenebisoxy (H2COO), methoxy (CH3O) and, finally methanol, and ii) Pd provides surface atomic hydrogen for CO2 reduction by spillover. Additionally, an interconversion between b-HCOO and m-HCOO was suggested, where b-HCOO appears to be a spectator, while m-HCOO seems to be the most reactive intermediate. Therefore it was deemed reasonable to further investigate the role of the formate groups in the methanol synthesis.