Support-Free, Connected Core-Shell Nanoparticle Catalysts Synthesized via a Low-Temperature Process for Advanced Oxygen Reduction Performance.

Nanostructured Pt-based catalysts have attracted considerable attention for fuel-cell applications. This study introduces a novel one-pot and low-temperature polyol approach for synthesizing support-free, connected nanoparticles with non-Pt metal cores and Pt shells. Unlike conventional heat treatment methods, the developed support-free and Fe-free connected Pd@Pt (Pd@Pt) nanoparticle catalyst possesses a stable nanonetwork structure with a high surface area. This approach can precisely control the atomic-level structure of the Pt shell on the Pd core at a low deposition temperature. The optimized Pd@Pt catalyst with a Pt/Pd atomic ratio of 0.8 and a Pt shell thickness of 1.1 nm exhibits a threefold improvement in oxygen reduction reaction (ORR) mass activity compared to that of commercial carbon-supported Pt nanoparticle catalyst (Pt/C). Durability evaluation demonstrated 100% retention of specific activity after 10,000 load cycles, owing to the stable nanonetwork and uniform coverage of the Pt shell. In addition, the support-free, connected core-shell nanoparticle catalyst overcomes the carbon corrosion issues commonly associated with conventional carbon-supported catalysts while simultaneously improving both ORR activity and load cycle durability. These findings highlight the potential of this innovative approach to develop support-free catalysts for polymer electrolyte fuel cells and other energy devices.