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Free keywords:
Alkaline, Amorphization, Multimetallic, Oxygen reduction reaction, Palladium, Amorphization, Electrolytic reduction, Free energy, Nanostructured materials, Oxygen, Palladium, Palladium alloys, Alkalines, Amorphizations, Metal nanomaterials, Multimetallic, Oxygen reduction catalysis, Oxygen reduction reaction, Pd alloy, Pd-based, Reaction activity, Unique features, Catalyst activity
Abstract:
Amorphous nanomaterials have drawn extensive attention owing to their unique features, while amorphization on noble metal nanomaterials still remains formidably challenging. Herein, we demonstrate a universal strategy to synthesize amorphous Pd-based nanomaterials from unary to quinary metals through the introduction of phosphorus (P). The amorphous Pd-based nanoparticles (NPs) exhibit generally promoted oxygen reduction reaction (ORR) activity and durability compared with their crystalline counterparts. Significantly, the quinary P-PdCuNiInSn NPs, benefiting from the amorphous structure and multimetallic component effect, exhibit mass activities as high as 1.04 A mgPd-1 and negligible activity decays of 1.8% among the stability tests, which are much better than values for original Pd NPs (0.134 A mgPd-1 and 28.4%). Experimental and theoretical analyses collectively reveal that the synergy of P-induced amorphization and the expansion of metallic components can considerably lower the free energy changes in the rate-determined step, thereby explaining the positive correlation with the catalytic activity. © 2024 American Chemical Society.