Single-atom Fe Embedded Co3S4 for Efficient Electrocatalytic Oxygen Evolution Reaction |
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Authors: | QI Yuxue LI Tingting HU Yajie XIANG Jiahong SHAO Wenqian CHEN Wenhua MU Xueqin LIU Suli CHEN Changyun YU Min MU Shichun |
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Affiliation: | 1. Key Laboratory of Advanced Functional Materials of Nanjing, Nanjing Xiaozhuang University, Nanjing 211171, P. R. China;2. Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, College of Materials Science and Engineering, Nanjing Forestry University, Nanjing 210037, P. R. China;3. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, P. R. China |
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Abstract: | Constructing atomically dispersed active sites with densely exposed and dispersed double metal-Sx catalytic sites for favorable OER catalytic activity remains rare and challenging. Herein, we design and construct a Fe1Sx@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, Fe1Sx@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 Fe1Sx@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. |
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Keywords: | Electrocatalyst Dual-metal site S coordination Fe single atom Oxygen evolution reaction |
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