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Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide

Nature Catalysis volume 4, pages 374–384 (2021)Cite this article

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Abstract

Artificial photosynthesis offers a promising strategy to produce hydrogen peroxide (H2O2)—an environmentally friendly oxidant and a clean fuel. However, the low activity and selectivity of the two-electron oxygen reduction reaction (ORR) in the photocatalytic process greatly restricts the H2O2 production efficiency. Here we show a robust antimony single-atom photocatalyst (Sb-SAPC, single Sb atoms dispersed on carbon nitride) for the synthesis of H2O2 in a simple water and oxygen mixture under visible light irradiation. An apparent quantum yield of 17.6% at 420 nm together with a solar-to-chemical conversion efficiency of 0.61% for H2O2 synthesis was achieved. On the basis of time-dependent density function theory calculations, isotopic experiments and advanced spectroscopic characterizations, the photocatalytic performance is ascribed to the notably promoted two-electron ORR by forming μ-peroxide at the Sb sites and highly concentrated holes at the neighbouring N atoms. The in situ generated O2 via water oxidation is rapidly consumed by ORR, leading to boosted overall reaction kinetics.

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Fig. 1: Photocatalytic performance of Sb-SAPC towards H2O2 production.
Fig. 2: Characterization of Sb-SAPC.
Fig. 3: Excitation properties and OER/ORR reactivities of Sb-SAPC15.
Fig. 4: Mechanism of photocatalytic H2O2 production.

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Source data are provided with this paper. The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

We acknowledge the financial support from the Mitsubishi Chemical Corporation, Japan Society for the Promotion of Science (JSPS) Grant-in-Aid for Scientific Research (B, grant no. 20H02847), Grant-in-Aid for JSPS Fellows (DC2, grant no. 20J13064), Project National Natural Science Foundation of China (grant nos. 21805191, 21972094), the Guangdong Basic and Applied Basic Research Foundation (grant no. 2020A1515010982), Shenzhen Pengcheng Scholar Program, Shenzhen Peacock Plan (grant nos. KQJSCX20170727100802505 and KQTD2016053112042971), the Singapore Ministry of Education (Tier 1: RG4/20 and Tier 2: MOET2EP10120-0002) and the Agency for Science, Technology and Research (A*Star IRG: A20E5c0080). We thank X. Huang from the Department of Physics, Southern University of Science and Technology for his help in theoretical calculation and N. Jian from the Electron Microscope Center of the Shenzhen University for his help in HRTEM measurement.

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  1. These authors contributed equally: Zhenyuan Teng, Qitao Zhang, Hongbin Yang.

Authors and Affiliations

  1. Department of Applied Chemistry, Faculty of Engineering, Kyushu Institute of Technology, Kitakyushu, Japan

    Zhenyuan Teng & Teruhisa Ohno

  2. Joint Laboratory of Yangzhou University, Kyushu Institute of Technology, Yangzhou University, Yangzhou, China

    Zhenyuan Teng, Sixiao Liu, Chengyin Wang & Teruhisa Ohno

  3. International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, China

    Qitao Zhang, Wenjuan Yang & Chenliang Su

  4. School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, Singapore

    Hongbin Yang & Bin Liu

  5. Graduate School of Engineering, Toyota Technological Institute, Tempaku Nagoya, Japan

    Kosaku Kato & Akira Yamakata

  6. National Synchrotron Radiation Research Center, Hsinchu, Taiwan

    Ying-Rui Lu

  7. College of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, China

    Sixiao Liu & Chengyin Wang

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Contributions

Z.T., Q.Z. and T.O. conceptualized the project. T.O., C.S. and B.L. supervised the project. Z.T. synthesized the catalysts, conducted the catalytic tests and the related data processing, and performed materials characterization and analysis with the help of H.Y., Q.Z., Y.-R.L. and S.L. K.K. and A.Y. conducted transient absorption spectroscopy. Z.T., W.Y. and C.W. performed the theoretical study. Z.T., H.Y. and B.L. wrote the paper with support from all authors.

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Correspondence to Chenliang Su, Bin Liu or Teruhisa Ohno.

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Peer review information Nature Catalysis thanks Wei Lin and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–45, Tables 1–8, Notes 1–8 and references.

Supplementary Data 1

Atomic coordinations of optimized models for Vienna ab initio simulation package.

Supplementary Data 2

Atomic coordinations of optimized models for Gaussian.

Supplementary Data 3

TDDFT calculation data.

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Source Data Fig. 1

Statistical source data.

Source Data Fig. 2

Statistical source data and .dm3 data.

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Statistical source data.

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Teng, Z., Zhang, Q., Yang, H. et al. Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide. Nat Catal 4, 374–384 (2021). https://doi.org/10.1038/s41929-021-00605-1

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