A series of Cu-ZnO/ZrO2 catalysts (Znat/Cuat, 0-3; ZrO2, 42-44 wt.%) with markedly improved total (SA, 120-180 m2/g) and metal surface area (MSA, 9-63 m2/g) has been synthesized via the reverse coprecipitation under ultrasound field. Structure, adsorption properties and surface reactivity were probed by BET, XRD, TPR, N2O-titration and TPD measurements of H2, CO and CO2, while the activity pattern in the CO2 to CH3OH hydrogenation reaction (TR, 433-473 K; PR, 1.0 MPa) has been addressed. An optimum ZnO loading (Znat/Cuat, 0.3-0.8) ensures higher process productivity, while the apparent structure sensitive character of the title reaction relies on the synergism of metal hydrogenation and oxide basic sites (dual-site). The extent of the oxide/metal interface, probed by Cud+/Cu0 and oxide-to-metal surface area (OSA/MSA) ratios, is the key-parameter allowing the normalization of the catalytic specific activity in a wide range (3-60%) of metal dispersion and the consequent structure insensitive character of the CO2 hydrogenation reaction.

Basic evidences for methanol-synthesis catalyst design

F Arena;G Bonura;L Spadaro;F Frusteri
2009

Abstract

A series of Cu-ZnO/ZrO2 catalysts (Znat/Cuat, 0-3; ZrO2, 42-44 wt.%) with markedly improved total (SA, 120-180 m2/g) and metal surface area (MSA, 9-63 m2/g) has been synthesized via the reverse coprecipitation under ultrasound field. Structure, adsorption properties and surface reactivity were probed by BET, XRD, TPR, N2O-titration and TPD measurements of H2, CO and CO2, while the activity pattern in the CO2 to CH3OH hydrogenation reaction (TR, 433-473 K; PR, 1.0 MPa) has been addressed. An optimum ZnO loading (Znat/Cuat, 0.3-0.8) ensures higher process productivity, while the apparent structure sensitive character of the title reaction relies on the synergism of metal hydrogenation and oxide basic sites (dual-site). The extent of the oxide/metal interface, probed by Cud+/Cu0 and oxide-to-metal surface area (OSA/MSA) ratios, is the key-parameter allowing the normalization of the catalytic specific activity in a wide range (3-60%) of metal dispersion and the consequent structure insensitive character of the CO2 hydrogenation reaction.
2009
Istituto di Tecnologie Avanzate per l'Energia - ITAE
Cu-ZnO/ZrO2 catalysts
Solid-state interactions
Adsorption properties
Surface sites
Dispersion
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/76399
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