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Wiley, Small, 41(18), 2022

DOI: 10.1002/smll.202203340

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Tuning Electronic Structure and Composition of FeNi Nanoalloys for Enhanced Oxygen Evolution Electrocatalysis via a General Synthesis Strategy

This paper was not found in any repository, but could be made available legally by the author.
This paper was not found in any repository, but could be made available legally by the author.

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Abstract

AbstractDeveloping 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‐5 nm. This method also enables precise control of both size and composition. Electrochemical measurements show that among FexNi(1−x) nanoalloys, Fe0.5Ni0.5 has the best performance. Density functional theory calculations support the experimental findings and reveal that the optimally positioned d‐band center of O‐covered Fe0.5Ni0.5 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% Fe0.5Ni0.5/40% C shows an extraordinarily low overpotential of 219 mV 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 50 h. 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.