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Construction of hierarchical FeNi3@(Fe,Ni)S2 core-shell heterojunctions for advanced oxygen evolution

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Abstract

The investigation of earth-abundant electrocatalysts for efficient water electrolysis is of central importance in renewable energy system, which is currently impeded by the large overpotential of oxygen evolution reaction (OER). NiFe sulfides show promising OER activity but are troubled by their low intrinsic conductivities. Herein, we demonstrate the construction of the porous core-shell heterojunctions of FeNi3@(Fe,Ni)S2 with tunable shell thickness via the reduction of hierarchical NiFe(OH)x nanosheets followed by a partial sulfidization. The conductive FeNi3 core provides the highway for electron transport, and the (Fe,Ni)S2 shell offers the exposed surface for in situ generation of S-doped NiFe-oxyhydroxides with high intrinsic OER activity, which is supported by the combined experimental and theoretical studies. In addition, the porous hierarchical morphology favors the electrolyte access and O2 liberation. Consequently, the optimized catalyst achieves an excellent OER performance with a low overpotential of 288 mV at 100 mA·cm−2, a small Tafel slope of 48 mV·dec−1, and a high OER durability for at least 1,200 h at 200 mA·cm−2. This study provides an effective way to explore the advanced earth-abundant OER electrocatalysts by constructing the heterojunctions between metal and corresponding metal-compounds via the convenient post treatment, such as nitridation and sulfidization.

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Acknowledgements

This work was jointly supported by the National Key Research and Development Program of China (Nos. 2017YFA0206500 and 2018YFA0209103), the National Natural Science Foundation of China (Nos. 52071174, 21832003, 21773111, and 21972061), and the Fundamental Research Funds for the Central Universities (No. 020514380126). The numerical calculations have been done on the computing facilities in the High Performance Computing Center (HPCC) of Nanjing University. We thank the staff of the BL14W1 beamline at Shanghai Synchrotron Radiation Facility for assistance with the X-ray absorption measurements.

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Authors and Affiliations

  1. Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory of Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China

    Minglei Yan, Zhiyang Zhao, Kun Mao, Xizhang Wang, Qiang Wu, Lijun Yang & Zheng Hu

  2. Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, the Chinese Academy of Sciences, Nanjing, 210008, China

    Peixin Cui

  3. Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210, China

    Chi Chen & Hui Yang

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  1. Minglei Yan
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  2. Zhiyang Zhao
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  4. Kun Mao
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Correspondence to Lijun Yang or Zheng Hu.

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Yan, M., Zhao, Z., Cui, P. et al. Construction of hierarchical FeNi3@(Fe,Ni)S2 core-shell heterojunctions for advanced oxygen evolution. Nano Res. 14, 4220–4226 (2021). https://doi.org/10.1007/s12274-021-3531-8

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