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High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis

Nature Sustainability volume 6, pages 816–826 (2023)Cite this article

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Abstract

The electrocatalytic oxygen reduction and evolution of molecular oxygen, known as oxygen electrocatalysis, is one of the most important reactions that are central to a range of energy and environmental technologies. While the current best-performing electrocatalysts remain dominated by precious metals, carbon-based systems provide a compelling alternative owing to their intrinsic sustainability and practical applicability. Here we show a design guided by theoretical calculations that pushes the activity boundaries of carbon electrocatalysts to an unprecedented level. The rationale is that incorporating high-entropy heteroatoms could effectively minimize the local symmetry to destabilize the π-electron network of graphitic carbons and avoid too strong or too weak binding energies for intermediate species of the oxygen reduction reaction and the oxygen evolution reaction. Accordingly, our catalyst embeds five metal single atoms—Fe, Mn, Co, Ni and Cu—and two sources of N, and it exhibits superior bifunctional activities in an alkaline environment that exceed the oxygen reduction reaction and evolution reaction performance of commercial Pt/C and RuO2 catalysts, respectively. Our work establishes electrocatalyst design principles that could open the door to sustainable solutions for critical green technologies such as fuel cells, batteries and water splitting.

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Fig. 1: The relationship between symmetry and electrocatalytic performance.
Fig. 2: Results of the DFT calculations of the HESA.
Fig. 3: Structural characterization.
Fig. 4: XANES spectra.
Fig. 5: Electrochemical tests of the ORR/OER performance.
Fig. 6: In situ ATR–FTIR spectra characterization of the ORR/OER processes on HESA.

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Data availability

All data that support the findings in the current study are available within the Article and its Supplementary Information. Source data are available from the corresponding authors upon reasonable request.

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Acknowledgements

We acknowledge financial support from the National Key R&D Program of China (grant no. 2022YFB2402600), the National Natural Science Foundation of China (grant nos 52125105, 51902339, 52273312, 51972329 and 52173242), the Shenzhen Science and Technology Planning Project (grant nos JCYJ20200109115424940 and JCYJ20210324101015037), and the Science and Technology Planning Project of Guangdong Province (grant no. 2019TX05L389).

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Author notes

  1. These authors contributed equally: Xin Lei, Qingyun Tang.

Authors and Affiliations

  1. Advanced Energy Storage Technology Research Center, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China

    Xin Lei, Qingyun Tang, Yongping Zheng, Xiaolong Zhou, Bifa Ji & Yongbing Tang

  2. Shenzhen College of Advanced Technology, University of Chinese Academy of Sciences, Shenzhen, China

    Xin Lei, Bifa Ji & Yongbing Tang

  3. Nano Science and Technology Institute, University of Science and Technology of China, Suzhou, China

    Qingyun Tang

  4. Synchrotron Light Research Institute, Nakhon Ratchasima, Thailand

    Pinit Kidkhunthod

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  1. Xin Lei
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Contributions

Y.T. and Y.Z. conceived and designed the experiments and calculations. Q.T., X.L. and B.J. fabricated the samples and conducted the structure characterization and electrochemical experiments. X.L. and Y.Z. conducted the simulation work. P.K. and X.Z. performed the synchrotron-based characterizations. X.L., Y.Z. and Y.T. wrote the paper. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Yongping Zheng or Yongbing Tang.

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Nature Sustainability thanks Shuhui Sun and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Lei, X., Tang, Q., Zheng, Y. et al. High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis. Nat Sustain 6, 816–826 (2023). https://doi.org/10.1038/s41893-023-01101-z

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