Structurally Tunable Graphitized Mesoporous Carbon for Enhancing the Accessibility and Durability of Cathode Pt‐Based Catalysts for Proton Exchange Membrane Fuel Cells

Low Pt utilization and intense carbon corrosion of cathode catalysts is a crucial issue for high-efficiency proton exchange membrane fuel cells due to the highly demanded long-term durability and less acquisition/application cost. Herein, structurally tunable graphitized mesoporous carbon (GMC) is obtained by direct high-temperature pyrolysis and in situ-controlled mesopore formation; the structure-optimized GMC1300-1800 exhibits a mesopore size of 7.54 nm and enhanced corrosion resistance. Functionalized GMC1300-1800 is loaded with small-sized Pt nanoparticles (NPs) (1.5 nm) uniformly by impregnation method to obtain Pt/GMC1300-1800 and form an "internal platinum structure" to avoid sulfonic acid groups poisoning as well as ensure O₂/proton accessibility. Hence, the electrochemically active surface area (ECSA) of Pt/GMC1300-1800 reaches 106.1 m² g^-1 _Pt, while mass activity and specific activity at 0.9 V are 2.1 and 1.4 times those of commercial Pt/C, respectively. Notably, the ECSA decay is less than 17% for both 30 000 cycles' accelerated durability tests (ADTs) of Pt attenuation and carbon attenuation. Accordingly, the optimized mesoporous structure of GMC1300-1800 significantly decreases the coverage of sulfonic acid groups on Pt NPs, leading to the highest peak power density in the single-cell test. Density functional theory calculations demonstrate the synergistic effect between graphitization and mesoporosity on enhancing the accessibility and durability of the catalysts.