Single-atom Fe Embedded Co3S4 for Efficient Electrocatalytic Oxygen Evolution Reaction

doi:10.1007/s40242-022-2248-x

Abstract

Abstract: Constructing atomically dispersed active sites with densely exposed and dispersed double metal-S_x catalytic sites for favorable OER catalytic activity remains rare and challenging. Herein, we design and construct a Fe₁S_x@Co₃S₄ electrocatalyst with Fe single atoms epitaxially confined in Co₃S₄ nanosheets for catalyzing the sluggish alkaline oxygen evolution reaction(OER). Consequently, in ultralow concentration alkaline solutions(0.1 mol/L KOH), such a catalyst is highly active and robust for OER with low overpotentials of 300 and 333 mV at current densities of 10 and 30 mA/cm², respectively, accompanying long-term stability without significant degradation even for 350 h. In addition, Fe₁S_x@Co₃S₄ shows a turnover frequency(TOF) value of 0.18 s⁻¹, nearly three times that of Co₃S₄(0.07 s⁻¹), suggesting the higher atomic utilization of Fe single atoms. Mössbauer and in-situ Raman spectra confirm that the OER activity of Fe₁S_x@Co₃S₄ origins from a thin catalytic layer of Co(Fe)OOH that interacts with trace-level Fe species in the electrolyte, creating dynamically stable active sites. Combined with experimental characterizations, it suggests that the most active S-coordinated dual-metal site configurations are 2S-bridged (Fe-Co)S₄, in which Co-S and Fe-S moieties are shared with two S atoms, which can strongly regulate the adsorption energy of reaction intermediates, accelerating the OER reaction kinetics.

Key words: Electrocatalyst, Dual-metal site, S coordination, Fe single atom, Oxygen evolution reaction

QI Yuxue, LI Tingting, HU Yajie, XIANG Jiahong, SHAO Wenqian, CHEN Wenhua, MU Xueqin, LIU Suli, CHEN Changyun, YU Min, MU Shichun. Single-atom Fe Embedded Co₃S₄ for Efficient Electrocatalytic Oxygen Evolution Reaction[J]. Chemical Research in Chinese Universities, 2022, 38(5): 1282-1286.

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Single-atom Fe Embedded Co₃S₄ for Efficient Electrocatalytic Oxygen Evolution Reaction

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