Amplified Interfacial Effect in an Atomically Dispersed RuOx-on-Pd 2D Inverse Nanocatalyst for High-Performance Oxygen Reduction

Atomically dispersed oxide-on-metal inverse nanocatalysts provide a blueprint to amplify the strong oxide-metal interactions for heterocatalysis but remain a grand challenge in fabrication. Here we report a 2D inverse nanocatalyst, RuOx-on-Pd nanosheets, by in situ creating atomically dispersed RuOx/Pd interfaces densely on ultrathin Pd nanosheets via a one-pot synthesis. The product displays unexpected performance toward the oxygen reduction reaction (ORR) in alkaline medium, which represents 8.0- and 22.4-fold enhancement in mass activity compared to the state-of-the-art Pt/C and Pd/C catalysts, respectively, showcasing an excellent Pt-alternative cathode electrocatalyst for fuel cells and metal-air batteries. Density functional theory calculations validate that the RuOx/Pd interface can accumulate partial charge from the 2D Pd host and subtly change the adsorption configuration of O-2 to facilitate the O-O bond cleavage. Meanwhile, the d-band center of Pd nanosubstrates is effectively downshifted, realizing weakened oxygen binding strength.

Automated summary

This study successfully prepared RuOx-on-Pd nanosheets as inverse nanocatalysts, showing unexpected performance towards the oxygen reduction reaction. The RuOx/Pd interface altered the adsorption configuration of O-2, facilitating O-O bond cleavage, while effectively downshifting the d-band center of Pd nanosubstrates to weaken oxygen binding strength.