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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Acknowledgements
This work was supported by the National Natural Science Foundation of China (Nos.21501096, 22075223), the Natural Science Foundation of Jiangsu Province, China(Nos.BK20150086, BK20201120), the Foundation of the Jiangsu Education Committee, China(No.15KJB150020), the Six Talent Peaks Project in Jiangsu Province, China(No.JY-087), the Innovation Project of Jiangsu Province, Excellent Scientific and Technological Innovation Team of Colleges and Universities of Jiangsu Province, China(No.SUJIAOKE 2021 No.1), the Key Subject of Ecology of Jiangsu Province, China(No.SUJIAOYANHAN 2022 No.2), and the Project of the Scientific and Technological Innovation Team of Nanjing, China (No.NINGJIAOGAOSHI 2021 No.16).
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Qi, Y., Li, T., Hu, Y. et al. Single-atom Fe Embedded CO3S4 for Efficient Electrocatalytic Oxygen Evolution Reaction. Chem. Res. Chin. Univ. 38, 1282–1286 (2022). https://doi.org/10.1007/s40242-022-2248-x
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DOI: https://doi.org/10.1007/s40242-022-2248-x