Abstract

Developing low-cost and efficient oxygen evolution electrocatalysts is key to decarbonization. A facile, surfactant-free, and gram-level biomass-assisted fast heating and cooling synthesis method is reported for synthesizing a series of carbon-encapsulated dense and uniform FeNi nanoalloys with a single-phase face-centered-cubic solid-solution crystalline structure and an average particle size of sub-5nm. This method also enables precise control of both size and composition. Electrochemical measurements show that among Fex Ni(1- x ) nanoalloys, Fe0.5 Ni0.5 has the best performance. Density functional theory calculations support the experimental findings and reveal that the optimally positioned d-band center of O-covered Fe0.5 Ni0.5 renders a half-filled antibonding state, resulting in moderate binding energies of key reaction intermediates. By increasing the total metal content from 25 to 60 wt%, the 60% Fe0.5 Ni0.5 /40% C shows an extraordinarily low overpotential of 219mV at 10 mA cm-2 with a small Tafel slope of 23.2 mV dec-1 for the oxygen evolution reaction, which are much lower than most other FeNi-based electrocatalysts and even the state-of-the-art RuO2 . It also shows robust durability in an alkaline environment for at least 50h. The gram-level fast heating and cooling synthesis method is extendable to a wide range of binary, ternary, quaternary nanoalloys, as well as quinary and denary high-entropy-alloy nanoparticles.

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