Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H2O2 production


Despite the growing demand for hydrogen peroxide it is almost exclusively manufactured by the energy-intensive anthraquinone process. Alternatively, H2O2 can be produced electrochemically via the two-electron oxygen reduction reaction, although the performance of the state-of-the-art electrocatalysts is insufficient to meet the demands for industrialization. Interestingly, guided by first-principles calculations, we found that the catalytic properties of the Co–N4 moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic properties of metalloenzymes. Using this principle, we designed and synthesized a single-atom electrocatalyst that comprises an optimized Co–N4 moiety incorporated in nitrogen-doped graphene for H2O2 production and exhibits a kinetic current density of 2.8 mA cm−2 (at 0.65 V versus the reversible hydrogen electrode) and a mass activity of 155 A g−1 (at 0.65 V versus the reversible hydrogen electrode) with negligible activity loss over 110 hours.

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Fig. 1: Theoretical predictions of catalyst materials.
Fig. 2: Structural characterization of GO, Co1–NG(O) and Co1–NG(R).
Fig. 3: Electrochemical ORR performance.
Fig. 4: Summary of H2O2 production activity and stability.

Data availability

All data is available in the main text or in the Supplementary Information.


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Synthesis and physicochemical property analysis of the catalysts were supported by the Research Center Program of the IBS (IBS-R006-D1) in Korea (T.H.). Electrochemical analysis was supported by Research Center Program of the IBS (IBS-R006-A2, Y.-E.S.). X-ray absorption spectra characterization at the Pohang Accelerator Laboratory (PAL) 8C beamline was supported by a National Research Foundation of Korea (NRF) grant funded by the Korea government (no. 2018M1A2A2061998). Theoretical analysis was supported by the 2019 Research Fund of the University of Seoul (J.S.Y.).

Author information

E.J., H.S., B.-H.L., J.S.Y., Y.-E.S. and T.H. conceived the research. E.J., H.S. and B.-H.L. designed the experiments. E.J., B.-H.L., H.S.L., J.K. and W.H.A. performed and analysed the results. H.S. and S.P. performed electrochemical measurements. V.E., S.L. and J.S.Y. performed the computational analysis. S.-P.C. conducted the high-angle annular dark-field scanning transmission electron microscopy analysis. K.-S.L. contributed to the X-ray absorption experiments and analysis. E.J., H.S., B.-H.L., J.S.Y., Y.-E.S. and T.H. wrote the manuscript. J.S.Y., Y.-E.S. and T.H. supervised the project. All the authors commented on the manuscript.

Correspondence to Jong Suk Yoo or Yung-Eun Sung or Taeghwan Hyeon.

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Supplementary Information

Supplementary Notes, Figs. 1–41, Tables 1–4 and references 1–18.

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Jung, E., Shin, H., Lee, B. et al. Atomic-level tuning of Co–N–C catalyst for high-performance electrochemical H2O2 production. Nat. Mater. 19, 436–442 (2020).

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