We present results for H 2 production by reforming of oxygenates on Pt-based bimetallic surfaces using temperature-programmed desorption (TPD), highresolution electron energy loss spectroscopy (HREELS) and density functional theory (DFT) calculations. Methanol, ethanol, ethylene glycol, and glycerol were employed as probe molecules. The formation of bimetallic surfaces with a 3d metal monolayer on Pt(111), designated 3d-PtPt(111), led to increased H 2 production as compared to the parent metal surfaces. The combined experimental and DFT results suggest that the reforming activity tracks the energy of the surface d-band center of various monometallic and bimetallic surfaces.