LAUSR

DFT calculations were employed to study the catalytic oxidation pathways of methanol on Pt(111), Pt(200), Pt(220), and Pt(311) surface and PtNi surface by introducing Ni to four Pt crystal planes. The pathway CH 3 OH-CH 2 OH-CHOH-COH-CO-COOH-CO 2 was designed as a basic oxidation route in acid medium. All the geometry configurations and reaction energies of reactant, intermediates and product were optimized as research models and analyzed. It is found that the Pt(111) crystal plane and Pt(311) crystal plane prefer to oxidize the methanol among four pure Pt crystal planes. The Pt(111)-1,2,3Ni-4Pt presented the lowest energy barrier, which was proved to be an optimal catalyst for Ni-doped Pt among Pt crystal planes. The present study can provide a new insight into modeling oxidation reaction pathways for methanol on Pt and PtNi surface and give guidance to achieve the ultimate goal of the designing Pt-based alloy catalysts and guiding the experiments for methanol oxidation.