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Supported Au single atoms and nanoparticles on MoS2 for highly selective CO2-to-CH3COOH photoreduction

Author

Listed:
  • Cai Chen

    (Southwest Petroleum University
    University of Science and Technology of China)

  • Chunyin Ye

    (University of Science and Technology of China)

  • Xinglei Zhao

    (CNPC Research Institute of Safety and Environmental Technology)

  • Yizhen Zhang

    (Southwest Petroleum University)

  • Ruilong Li

    (University of Science and Technology of China)

  • Qun Zhang

    (University of Science and Technology of China)

  • Hui Zhang

    (Southwest Petroleum University)

  • Yuen Wu

    (University of Science and Technology of China
    University of Science and Technology of China)

Abstract

Effectively controlling the selective conversion of CO2 photoreduction to C2 products presents a significant challenge. Here, we develop a heterojunction photocatalyst by controllably implanting Au nanoparticles and single atoms into unsaturated Mo atoms of edge-rich MoS2, denoted as Aun/Au1-CMS. Photoreduction of CO2 results in the production of CH3COOH with a selectivity of 86.4%, which represents a 6.4-fold increase compared to samples lacking single atoms, and the overall selectivity for C2 products is 95.1%. Furthermore, the yield of CH3COOH is 22.4 times higher compared to samples containing single atoms and without nanoparticles. Optical experiments demonstrate that the single atoms domains can effectively capture photoexcited electrons by the Au nanoparticles, or the local electric field generated by the nanoparticles promotes the transfer of photogenerated electrons in MoS2 to Au single atoms, prolonging the relaxation time of photogenerated electrons. Mechanistic investigations reveal that the orbital coupling of Au5d and Mo4d strengthens the oxygen affinity of Mo and carbon affinity of Au. The hybridized orbitals reduce energy splitting levels of CO molecular orbitals, aiding C–C coupling. Moreover, the Mo−Au dual-site stabilize the crucial oxygen-associated intermediate *CH2CO, thereby enhancing the selectivity towards CH3COOH. The cross-scale heterojunctions provide an effective strategy to simultaneously address the kinetical and thermodynamical limitations of CO2-to-CH3COOH conversion.

Suggested Citation

  • Cai Chen & Chunyin Ye & Xinglei Zhao & Yizhen Zhang & Ruilong Li & Qun Zhang & Hui Zhang & Yuen Wu, 2024. "Supported Au single atoms and nanoparticles on MoS2 for highly selective CO2-to-CH3COOH photoreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52291-9
    DOI: 10.1038/s41467-024-52291-9
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    References listed on IDEAS

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    1. Wenchao Shangguan & Qing Liu & Ying Wang & Ning Sun & Yu Liu & Rui Zhao & Yingxuan Li & Chuanyi Wang & Jincai Zhao, 2022. "Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
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