Abstract

To enhance nanocatalyst performance and durability for the methanol oxidation reaction (MOR) in a direct methanol fuel cell, small-sized (2.1 nm) and structurally ordered Pt3Co intermetallic nanoparticles are uniformly anchored onto nitrogen-doped carbon nanotubes (N-CNTs) via a low-temperature N-anchoring method, and the N-doping abilities of different N-containing reagents are compared. After investigating the microstructure of Pt3Co/N-CNTs and evaluating their catalytic activity for the MOR, the results show that N-doping facilitates the uniform loading of Pt3Co NPs and plays a crucial role in improving the electrocatalytic activity of Pt3Co NPs supported on CNTs. Pt3Co/N-CNT-M with melamine as the N dopant exhibits the highest MOR activity and stability among all N-CNT-supported Pt3Co NPs and Pt/N-CNT-M. Density functional theory calculations suggest that the doping of N enhances the binding energy of CNTs to Pt3Co NPs, and the MOR mechanism shows that the introduction of Co is the reason for the enhancement of MOR reaction kinetics. The excellent electrochemical performance of Pt3Co/N-CNT-M is mainly attributed to the synergistic effect of N and Pt3Co intermetallic nanoparticles. The combination of ordered alloy nanoparticles and high-performance carrier N-CNT-M described herein exhibits great potential for fuel cells and may provide an unequivocal direction for the optimization of catalyst performance.

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