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Accessing parity-forbidden d-d transitions for photocatalytic CO2 reduction driven by infrared light

Author

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  • Xiaodong Li

    (Max Planck Institute of Microstructure Physics, Weinberg 2)

  • Li Li

    (University of Science and Technology of China)

  • Guangbo Chen

    (Dresden University of Technology)

  • Xingyuan Chu

    (Dresden University of Technology)

  • Xiaohui Liu

    (Dresden University of Technology)

  • Chandrasekhar Naisa

    (Dresden University of Technology)

  • Darius Pohl

    (Dresden University of Technology, Helmholtzstreet)

  • Markus Löffler

    (Dresden University of Technology, Helmholtzstreet)

  • Xinliang Feng

    (Max Planck Institute of Microstructure Physics, Weinberg 2
    Dresden University of Technology)

Abstract

A general approach to promote IR light-driven CO2 reduction within ultrathin Cu-based hydrotalcite-like hydroxy salts is presented. Associated band structures and optical properties of the Cu-based materials are first predicted by theory. Subsequently, Cu4(SO4)(OH)6 nanosheets were synthesized and are found to undergo cascaded electron transfer processes based on d-d orbital transitions under infrared light irradiation. The obtained samples exhibit excellent activity for IR light-driven CO2 reduction, with a production rate of 21.95 and 4.11 μmol g−1 h−1 for CO and CH4, respectively, surpassing most reported catalysts under the same reaction conditions. X-ray absorption spectroscopy and in situ Fourier-transform infrared spectroscopy are used to track the evolution of the catalytic sites and intermediates to understand the photocatalytic mechanism. Similar ultrathin catalysts are also investigated to explore the generality of the proposed electron transfer approach. Our findings illustrate that abundant transition metal complexes hold great promise for IR light-responsive photocatalysis.

Suggested Citation

  • Xiaodong Li & Li Li & Guangbo Chen & Xingyuan Chu & Xiaohui Liu & Chandrasekhar Naisa & Darius Pohl & Markus Löffler & Xinliang Feng, 2023. "Accessing parity-forbidden d-d transitions for photocatalytic CO2 reduction driven by infrared light," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39666-0
    DOI: 10.1038/s41467-023-39666-0
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    References listed on IDEAS

    as
    1. Xiaodong Li & Yongfu Sun & Jiaqi Xu & Yanjie Shao & Ju Wu & Xiaoliang Xu & Yang Pan & Huanxin Ju & Junfa Zhu & Yi Xie, 2019. "Selective visible-light-driven photocatalytic CO2 reduction to CH4 mediated by atomically thin CuIn5S8 layers," Nature Energy, Nature, vol. 4(8), pages 690-699, August.
    2. Yimin A. Wu & Ian McNulty & Cong Liu & Kah Chun Lau & Qi Liu & Arvydas P. Paulikas & Cheng-Jun Sun & Zhonghou Cai & Jeffrey R. Guest & Yang Ren & Vojislav Stamenkovic & Larry A. Curtiss & Yuzi Liu & T, 2019. "Facet-dependent active sites of a single Cu2O particle photocatalyst for CO2 reduction to methanol," Nature Energy, Nature, vol. 4(11), pages 957-968, November.
    3. 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.
    4. Ulrich Ulmer & Thomas Dingle & Paul N. Duchesne & Robert H. Morris & Alexandra Tavasoli & Thomas Wood & Geoffrey A. Ozin, 2019. "Fundamentals and applications of photocatalytic CO2 methanation," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    5. Virgil Andrei & Geani M. Ucoski & Chanon Pornrungroj & Chawit Uswachoke & Qian Wang & Demetra S. Achilleos & Hatice Kasap & Katarzyna P. Sokol & Robert A. Jagt & Haijiao Lu & Takashi Lawson & Andreas , 2022. "Floating perovskite-BiVO4 devices for scalable solar fuel production," Nature, Nature, vol. 608(7923), pages 518-522, August.
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    1. Xiaodong Li & Li Li & Xingyuan Chu & Xiaohui Liu & Guangbo Chen & Quanquan Guo & Zhen Zhang & Mingchao Wang & Shuming Wang & Alexander Tahn & Yongfu Sun & Xinliang Feng, 2024. "Photothermal CO2 conversion to ethanol through photothermal heterojunction-nanosheet arrays," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Xiaoyue Zhang & Shunlong Ju & Chaoqun Li & Jiazheng Hao & Yahui Sun & Xuechun Hu & Wei Chen & Jie Chen & Lunhua He & Guanglin Xia & Fang Fang & Dalin Sun & Xuebin Yu, 2024. "Atomic reconstruction for realizing stable solar-driven reversible hydrogen storage of magnesium hydride," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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