Enhanced O2 reduction on atomically thin Pt-based nanoshells by integrating surface facet, interfacial electronic, and substrate stabilization effects

Abstract

To fully realize the commercial viability of Pt in fuel cells, the usage of scarce Pt must be reduced while the activity and durability in O2 reduction reaction (ORR) must be enhanced. Here we report a metallic stack design achieving these goals for ORR, based on atomically precise materials synthesis. Au@Pd@Pt nanostructures with atomically thin Pt shells and high-index surfaces form an excellent platform for integrating the effects of electronic structures, surface facets, and substrate stabilization to boost ORR performance. Au@Pd@Pt trisoctahedrons (TOH) achieve mass activity 6.1 times higher than that of commercial Pt/C and dramatically enhanced durability beyond 1.0 V vs. a reversible hydrogen electrode in oxidation potential. Meanwhile, Pt comprises only 3.2% of the nanostructures. To further improve the ORR activity and demonstrate the versatility of our strategy, we implement the same design in PtNi alloy electrocatalysts. The Au@Pd@PtNi TOHs exhibit mass activity 14.3 times higher than that of commercial Pt/C as well as excellent durability. This work demonstrates an alternative strategy for fabricating high-performance and low-cost catalysts, and highlights the importance of simultaneous surface and interfacial engineering with atomic precision in designing catalysts.