Zirconium oxide was synthesized by a modified sol-gel method, and was evaluated for the selective formation of isobutane and isobutene from synthesis gas. Due to increased basicity, zirconia from sol-gel preparation showed higher selectivities to iso-C4’S, while maintaining the same level of activity as zirconia prepared by calcination of zirconyl salts. The catalyst was further modified with Group I and II elements, and the activity tests showed increased iso-C4 and decreased methane production for the catalysts doped with potassium, magnesium, calcium, or barium.