Boosting Oxygen and Peroxide Reduction Reactions on PdCu Intermetallic Cubes

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Abstract

Abstract Palladium‐based nanocatalysts have the potential to replace platinum‐based catalysts for fuel‐cell reactions in alkaline electrolytes, especially PdCu intermetallic nanoparticles with high electrochemical activity and stability. However, unlike the synthetic methods for obtaining the nanoparticles, the effect of PdCu shape on the performance is relatively less well studied. Here, we demonstrate the facet dependence of PdCu intermetallics on the oxygen reduction reaction (ORR) and peroxide reduction, and reveal that the {100} dominant PdCu cubes have a much higher ORR mass activity and specific activity than spheres at 0.9 V vs. RHE, which is four and five times that of commercial Pd/C and Pt/C catalysts, respectively, and show only a 31.7 % decay after 30 000 cycles in the stability test. Moreover, cubic PdCu nanoparticles show higher peroxide electroreduction activity than Pd cubes and PdCu spheres. Density functional theory (DFT) calculation reveals that the huge difference originates from the reduction in oxygen adsorption energy and energy barrier of peroxide decomposition on the ordered {100} PdCu surface. Given the relationship between the shape and electrochemical performance, this study will contribute to further research on electrocatalytic improvements of catalysts in alkaline environments.

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