Basic evidences for methanol-synthesis catalyst design

A series of Cu-ZnO/ZrO2 catalysts (Zn-at/Cu-at, 0-3; ZrO2, 42-44 wt.%) with markedly improved total (SA, 120-180 m(2)/g) and metal surface area (MSA, 9-63 m(2)/g) has been synthesized via the reverse co-precipitation under ultrasound field. Structure, adsorption properties and surface reactivity were probed by BET, XRD, TPR, N2O-titration and TPD measurements of H-2, CO and CO2, while the activity pattern in the CO2 to CH3OH hydrogenation reaction (T-R, 433-473 K: P-R, 1.0 MPa) has been addressed. An optimum ZnO loading (Zn-at/Cu-at, 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 Cu delta+/Cu-0 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. (C) 2008 Published by Elsevier B.V.