Hydrogen production by steam reforming of methanol is studied over Cu/Zn-based catalysts (Cu/ZnO, Cu/ZnO/Al2O3, Cu/ZnO/ZrO2/Al2O3). Cu/Zn-based catalysts are derived from hydrotalcite-like precursors prepared by a co-precipitation method. The catalysts are characterized by N2O chemisorption, XRD, and BET surface area measurements. ZrO2 added to the Cu/Zn-based catalyst enhances copper dispersion on the catalyst surface. Among the catalysts tested, Cu/ZnO/ZrO2/Al2O3 exhibits the highest methanol conversion and the lowest CO concentration in the outlet gas. A micro-channel reactor coated with a Cu/ZnO/ZrO2/Al2O3 catalyst in the presence of an undercoated Al2O3 buffer layer exhibits higher methanol conversion and lower CO concentration in the outlet gas than in the absence of an undercoated Al2O3 buffer layer. The micro-channel reactor with a undercoated Al2O3 buffer layer produces large amounts of hydrogen compared with one without a buffer layer. The undercoated Al2O3 buffer layer enhances the adhesion between catalysts and micro-channel walls, which leads to improvement in reactor performance. (c) 2005 Elsevier B.V. All rights reserved.