Production of H-2 from methanol by steam reforming, partial oxidation, or a combination thereof was studied over Cu/ZnO-based catalysts. The catalysts were characterized by a variety of techniques, including N2O chemisorption, X-ray photoelectron spectroscopy, X-ray diffraction, and temperature-programmed reduction/oxidation. The influence of feed composition, reaction temperature, and catalyst formulation on H-2 production rate, product distribution, and catalyst lifetime was investigated. Distinct differences between the processes were observed with respect to catalyst behavior. ZrO2-containing catalysts, especially Cu/ZnO/ZrO2/Al2O3, exhibit the best performance in the steam reforming reaction. During partial oxidation, however, a binary Cu/ZnO catalyst exhibits the lowest light-off temperature and the lowest level of CO by-product. The redox properties of the catalyst appear to play a key role in determining the pathway for H-2 production. In particular. the extent of methanol and/or H-2 combustion at differential O-2 conversion is strongly dependent on the ease of copper oxidation in the catalyst. (C) 2003 Elsevier Inc. All rights reserved.