Abstract

<h2>Summary</h2> Because of the poor accessibility of embedded active sites, platinum (Pt)-based electrocatalysts suffer from insufficient Pt utilization and mass transport in membrane electrode assemblies (MEAs), limiting their performance in polymer electrolyte membrane fuel cells. Here, we report a simple and universal approach to depositing sub-3-nm L1<sub>0</sub>-PtM nanoparticles over external surfaces of carbon supports through pore-tailored amino (NH<sub>2</sub>)-modification, which enables not only excellent activity for the oxygen reduction reaction, but also enhanced Pt utilization and mass transport in MEAs. Using a low loading of 0.10 mg<sub>Pt</sub>·cm<sup>−2</sup>, the MEA of PtCo/KB-NH<sub>2</sub> delivered an excellent mass activity of 0.691 A·mg<sub>Pt</sub><sup>−1</sup>, a record-high power density of 0.96 W·cm<sup>−2</sup> at 0.67 V, and only a 30-mV drop at 0.80 A·cm<sup>−2</sup> after 30,000 voltage cycles, which meets nearly all targets set by the Department of Energy. This work provides an efficient strategy for designing advanced Pt-based electrocatalysts and realizing high-power fuel cells.

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