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Constructing hierarchical nanosheet-on-microwire FeCo LDH@Co3O4 arrays for high-rate water oxidation

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Abstract

Alkaline electrochemical water oxidation powered by renewable energies is a promising and environmentally friendly way to produce hydrogen. The industrial water electrolyzers are commonly operated at a high current density, calling for abundant and durable active sites to participate in. The rational design of hierarchically structured electrocatalysts is thus essential to industrial water electrolyzers. Herein, we develop a Fe3+ induced nanosizing strategy for fabricating such a hierarchical FeCo LDH@Co3O4 (LDH: layered double hydroxide) nanostructure array for high-rate water oxidation. Density functional theory (DFT) simulations indicate that the introduction of Fe3+ with a small ion radius and high electrical repulsion in the LDH layer distorted the LDH layer, resulting in a reduced nanosheet size and enabling the formation of a hierarchical structure. Such structure cannot be achieved without the participation of Fe3+ cations. Benefiting from the significantly enhanced electrochemical surface areas and charge/mass transport due to the hierarchical structure together with the boosted intrinsic activity by electronic modulation of Fe3+, such FeCo LDH@Co3O4 electrode can deliver an industrial-level current density of 1,000 mA·cm−2 at a small overpotential of 392 mV for water oxidation. When assembled in a water electrolyzer, it delivers a current density of 100 mA·cm−2 at a low operation voltage of 1.61 V. Powered by solar light, the electrolyzer demonstrates high solar-to-hydrogen efficiency of 18.15% with stable and reproducible photoresponse. These results provide new insights for constructing hierarchical nanostructures for advanced water oxidation and other diverse applications.

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Acknowledgements

The authors acknowledge the financial support from the National Natural Science Foundation of China (Nos. 22025208, 22075300, and 21902162), the China National Postdoctoral Program for Innovative Talents (No. BX2021319), the DNL Cooperation Fund, CAS (No. DNL202008), and the Chinese Academy of Sciences. We also thank Dr. Z.-J. Z., X.-Y. Z., and B.-L. Q. for the XPS analysis; Y. S. for the XRD analysis; and Dr. B. G., Y.-X. C, and J.-L. Y. for SEM and TEM support.

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Authors and Affiliations

  1. Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China

    Tang Tang, Zhe Jiang, Shuai Niu, Ze-Cheng Yao, Wen-Jie Jiang & Jin-Song Hu

  2. University of the Chinese Academy of Sciences, Beijing, 100049, China

    Tang Tang, Zhe Jiang, Shuai Niu, Ze-Cheng Yao & Jin-Song Hu

  3. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China

    Jun Deng

  4. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201800, China

    Lin-Juan Zhang

  5. Dalian National Laboratory for Clean Energy, Dalian, 116023, China

    Lin-Juan Zhang & Jin-Song Hu

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  1. Tang Tang
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Tang, T., Jiang, Z., Deng, J. et al. Constructing hierarchical nanosheet-on-microwire FeCo LDH@Co3O4 arrays for high-rate water oxidation. Nano Res. 15, 10021–10028 (2022). https://doi.org/10.1007/s12274-022-5094-8

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