Abstract
<jats:p>Improving platinum catalyst utilization and durability in proton exchange membrane fuel cells (PEMFC) requires carbon supports with well-defined porosity, electronic conductivity, and controlled surface chemistry. This work investigates poly(imine-cyanurate)-derived carbon aerogels as a PEMFC catalyst support platform, synthesized from three aromatic diamine linkers: 4,4′-methylenedianiline, 4,4′-oxydianiline and 2,2-bis[4-(4-aminophenoxy)phenyl] propane, reacted with a triazine-core trifunctional aldehyde and carbonized at temperatures between 500 and 1100 °C. The resulting carbons exhibit tunable surface areas (77-540 m2 g-1), interconnected porous architectures, and intrinsic nitrogen doping inherited from the precursors. Platinum nanoparticles of 2.3-2.8 nm were deposited by polyol reduction, with loading and dispersion governed by the interplay between nitrogen functionality and surface defect density. Rotating disk electrode measurements confirm comparable intrinsic platinum activity across all supports, with differences in limiting current and electron transfer number attributed to variations in electronic conductivity and mass transport. In single-cell PEMFC testing, the new catalysts achieve peak power densities of 1.01 W cm-2 at 100% RH, falling just short of Pt/Vulcan's 1.06 W cm-2. After 30,000 AST cycles, the aerogel-derived support outperforms Pt/Vulcan, and this improved durability is attributed to nitrogen and defect-mediated platinum anchoring and the porous architecture. The results establish aromatic poly(imine-cyanurate)-derived carbon aerogels as a versatile and durable platform for next-generation PEMFC catalyst supports.</jats:p>