Optimizing Oxygen Reduction Reaction Performance in Pt-based Catalysts through Fe/Ce Dual-Component Interface Engineering on Nitrogen-Doped Carbon

The advancement of high-efficiency Pt catalysts with reduced Pt loading is crucial for proton exchange membrane fuel cells (PEMFCs). This research presents a methodology that significantly increases the performance of Pt/C through the interactions between Pt and Fe-Nx/Ce-Nx on carbon, thereby effectively reducing Pt consumption. Density functional theory (DFT) calculations indicate that the presence of Fe-Nx/Ce-Nx together enhances the strong interaction between Pt and FeCe-NC, decreasing the d-band energy level (εd) of Pt, which leads to the reduction of O* adsorption and acceleration of desorption at the Pt sites. Consequently, the Pt/FeCe-NC demonstrates exceptional performance for the ORR. The Pt/FeCe-NC has an E1/2 of 0.927 V and decays by only 7 mV after 30,000 accelerated stress test (AST) cycles under acidic conditions. Furthermore, the Pt/FeCe-NC (2.14 W/cm2) surpasses Pt/C (1.78 W/cm2) regarding peak power density in PEMFCs. This innovative approach clarifies the interactions between Pt and Fe-Nx/Ce-Nx, providing a framework for the design of advanced catalysts.