Plasma‐Induced Formation of Pt Nanoparticles with Optimized Surface Oxidation States for Methanol Oxidation and Oxygen Reduction Reactions to Achieve High‐Performance DMFCs

Abstract Plasma treatment and reduction are used to synthesize Pt nanoparticles (NPs) on nitrogen‐doped carbon nanotubes (p‐Pt/p‐NCNT) with a low Pt content. In particular, the plasma treatment is used to treat the NCNT to give it with more surface defects, facilitating a better growth of the Pt NPs, while the plasma reduction produces the Pt NPs with a reduced fraction of the surface atoms at the high oxidation states, increasing the catalytic activities of the p‐Pt@p‐NCNT. Even at the low Pt content (7.8 wt.%), the p‐Pt@p‐NCNT shows superior catalytic activities and good stabilities for methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR). The density functional theory (DFT) calculations indicate that the defects generated in the plasma treatment can help the growth of the Pt NPs on the NCNTs, leading to the stronger electronic coupling between Pt and NCNT and the increased stability of the catalyst. The plasma reduction can give the Pt NPs with optimized surface oxidation states, decreasing the energy barriers of the rate‐determining steps for MOR and ORR. When used as the anode and cathode catalysts for the direct methanol fuel cells (DMFCs), the p‐Pt@p‐NCNT exhibits a higher maximum power density of 81.9 mW cm −2 at 80 °C and shows good durability.