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High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials


Hydrogen peroxide (H2O2) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H2O2 involves an energy-intensive anthraquinone process. The electrochemical synthesis of H2O2 from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H2O2 production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. The density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments.

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Fig. 1: Oxygen reduction performance of CNTs and O-CNTs.
Fig. 2: Characterizations of CNTs and O-CNTs.
Fig. 3: ORR activities of O-CNTs with diverse oxygen content and other carbon materials.
Fig. 4: DFT results of the ORR activities of different oxygen functional groups.


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This work was initiated by the support of the Materials Sciences and Engineering Division of the Basic Energy Sciences office at the US Department of Energy, under contract DEAC02-76-SFO0515. We acknowledge support from SUNCAT seed funding in SLAC. We also gratefully acknowledge support from the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Sciences at the US Department of Energy to the SUNCAT Center for Interface Science and Catalysis under award number DE-SC0004993.

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Z.L., G.C., S.S. and Y.C. conceived the research. Z.L., G.C., Z.C., K.L., J.X., L.L., T.W., D.L. and Y.L. performed the experiments. S.S. and J.K.N. performed the theoretical calculation. Z.L., G.C., Z.C., T.F.J. and Y.C. contributed new reagents and analytical tools. Z.L., G.C., S.S., Z.C., T.F.J., J.K.N. and Y.C. analysed the data. Z.L., G.C., S.S., Z.C., T.F.J., J.K.N. and Y.C. wrote the paper.

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Correspondence to Yi Cui.

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Supplementary Figures 1–17, Supplementary Tables 1–4, Supplementary Note 1, Supplementary Reference

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Lu, Z., Chen, G., Siahrostami, S. et al. High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials. Nat Catal 1, 156–162 (2018).

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