Tailoring N Configurations for Enhanced Methanol Oxidation on Pt Nanoparticles

Direct methanol fuel cells (DMFCs) face significant challenges due to sluggish methanol oxidation reaction (MOR) kinetics and catalyst poisoning by carbon intermediates (e.g., CO ads ). To address this, we rationally designed nitrogen-doped carbon (NC) carriers with tailored N-configurations (pyridinic-N, pyrrolic-N, and graphitic-N) via controlled pyrolysis temperatures (700–1000 °C) and anchored Pt nanoparticles (NPs) to enhance metal-support interaction (MSI). The NC-900 carrier achieved optimal N-configuration distribution (56.7% pyridinic-N, 25.2% pyrrolic-N, 18.1% graphitic-N) and the highest defect density ( I D /I G = 1.12), enabling ultra-dispersed Pt NPs (1.69 nm) and strong electron donation to Pt. XPS confirmed a 61.2% Pt° content in Pt/NPC-900, facilitating efficient methanol adsorption/activation. In alkaline media, Pt/NPC-900 delivered a record mass activity of 4687.5 mA mg −1 Pt - 4.36 × higher than Pt/PC—along with exceptional stability (79.6 % current retention after 500 cycles). In situ Raman spectroscopy revealed a non-CO pathway, circumventing poisoning intermediates. This work establishes a precise N-configuration engineering strategy to optimize MSI for next-generation DMFC catalysts. Graphical Schematic diagram for the preparation of N-doped carbon-supported Pt nanoparticles catalysts by chemical reduction method.By adjusting the roasting temperature, it is possible to control the proportion of different N-configuration distributions. This enables effective control of the dispersion degree and electronic properties of the active metal Pt, thereby enhancing the activity and stability of the catalyst during the alkaline methanol oxidation reaction.