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    Spin-Polarized Photocatalytic CO2 Reduction of Mn-Doped Perovskite Nanoplates
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    • Cheng-Chieh Lin
      Cheng-Chieh Lin
      International Graduate Program of Molecular Science and Technology, National Taiwan University (NTU-MST), Taipei 10617, Taiwan
      Molecular Science and Technology Program, Taiwan International Graduate Program (TIGP), Academia Sinica, Taipei 11529, Taiwan
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      Orcidhttps://orcid.org/0000-0003-1895-493X
    • Ting-Ran Liu
      Ting-Ran Liu
      Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan
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    • Sin-Rong Lin
      Sin-Rong Lin
      Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan
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    • Karunakara Moorthy Boopathi
      Karunakara Moorthy Boopathi
      Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan
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      Orcidhttps://orcid.org/0000-0003-2042-9595
    • Chun-Hao Chiang
      Chun-Hao Chiang
      Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan
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      Orcidhttps://orcid.org/0000-0002-9066-4657
    • Wen-Yen Tzeng
      Wen-Yen Tzeng
      Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan
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    • Wan-Hsiu Chang Chien
      Wan-Hsiu Chang Chien
      Department of Applied Physics, National Pingtung University, Pingtung 90044, Taiwan
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    • Hua-Shu Hsu
      Hua-Shu Hsu
      Department of Applied Physics, National Pingtung University, Pingtung 90044, Taiwan
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      Orcidhttps://orcid.org/0000-0002-5773-2451
    • Chih-Wei Luo
      Chih-Wei Luo
      Department of Electrophysics, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan
      Institute of Physics and Center for Emergent Functional Matter Science, National Yang Ming Chiao Tung University, Hsinchu 30010, Taiwan
      National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan
      Taiwan Consortium of Emergent Crystalline Materials (TCECM), Ministry of Science and Technology, Taipei 10622, Taiwan
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      Orcidhttps://orcid.org/0000-0002-6453-7435
    • Hui-Ying Tsai
      Hui-Ying Tsai
      Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan
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    • Hsin-An Chen
      Hsin-An Chen
      Institute of Materials Science and Engineering, National Taipei University of Technology, Taipei 10608, Taiwan
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    • Pai-Chia Kuo
      Pai-Chia Kuo
      Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan
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    • Jessie Shiue
      Jessie Shiue
      Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan
      Institute of Physics, Academia Sinica, Taipei 11520, Taiwan
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    • Jau-Wern Chiou
      Jau-Wern Chiou
      Department of Applied Physics, National University of Kaohsiung, Kaohsiung 81148, Taiwan
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    • Way-Faung Pong
      Way-Faung Pong
      Department of Physics, Tamkang University, New Taipei City 25137, Taiwan
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    • Chia-Chun Chen*
      Chia-Chun Chen
      Department of Chemistry, National Taiwan Normal University, Taipei 11677, Taiwan
      Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-6491-0482
    • Chun-Wei Chen*
      Chun-Wei Chen
      International Graduate Program of Molecular Science and Technology, National Taiwan University (NTU-MST), Taipei 10617, Taiwan
      Department of Materials Science and Engineering, National Taiwan University, Taipei 10617, Taiwan
      Center for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan
      Center of Atomic Initiative for New Materials (AI-MAT), National Taiwan University (NTU), Taipei 10617, Taiwan
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0003-3096-249X
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 34, 15718–15726
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c06060
    Published August 17, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    “Spin” has been recently reported as an important degree of electronic freedom to improve the performance of electrocatalysts and photocatalysts. This work demonstrates the manipulations of spin-polarized electrons in CsPbBr3 halide perovskite nanoplates (NPLs) to boost the photocatalytic CO2 reduction reaction (CO2RR) efficiencies by doping manganese cations (Mn2+) and applying an external magnetic field. Mn-doped CsPbBr3 (Mn-CsPbBr3) NPLs exhibit an outstanding photocatalytic CO2RR compared to pristine CsPbBr3 NPLs due to creating spin-polarized electrons after Mn doping. Notably, the photocatalytic CO2RR of Mn-CsPbBr3 NPLs is significantly enhanced by applying an external magnetic field. Mn-CsPbBr3 NPLs exhibit 5.7 times improved performance of photocatalytic CO2RR under a magnetic field of 300 mT with a permanent magnet compared to pristine CsPbBr3 NPLs. The corresponding mechanism is systematically investigated by magnetic circular dichroism spectroscopy, ultrafast transient absorption spectroscopy, and density functional theory simulation. The origin of enhanced photocatalytic CO2RR efficiencies of Mn-CsPbBr3 NPLs is due to the increased number of spin-polarized photoexcited carriers by synergistic doping of the magnetic elements and applying a magnetic field, resulting in prolonged carrier lifetime and suppressed charge recombination. Our result shows that manipulating spin-polarized electrons in photocatalytic semiconductors provides an effective strategy to boost photocatalytic CO2RR efficiencies.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c06060.

    • Experimental section, AFM data, band gaps of perovskite NPLs, spin-polarized DOS of the pristine CsPbBr3, setup of photocatalytic CO2RR, calibration curves of CO and CH4, evolutions of products over perovskite NPLs under different external magnetic fields, control experiments and 13CO2 isotopic experiment, comparison of photocatalytic CO2RR conversion efficiencies, decay times of perovskite NPLs, and setup of MCD measurements (PDF)

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    This article is cited by 41 publications.

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    Cite this: J. Am. Chem. Soc. 2022, 144, 34, 15718–15726
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c06060
    Published August 17, 2022
    Copyright © 2022 American Chemical Society
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