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Cu–Sb Atomic Pair Site in Metal Halide Perovskite for CO2 Reduction to Methanol
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    Cu–Sb Atomic Pair Site in Metal Halide Perovskite for CO2 Reduction to Methanol
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    • Yayun Pu
      Yayun Pu
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Fan Yang
      Fan Yang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
      More by Fan Yang
    • Haowen Wang
      Haowen Wang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Chengfan Fu
      Chengfan Fu
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Jun’an Lai
      Jun’an Lai
      Key Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China
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    • Zixian Wang
      Zixian Wang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Fei Qi
      Fei Qi
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Nan Zhang
      Nan Zhang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
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    • Limin Huang
      Limin Huang
      Department of Chemistry, Southern University of Science and Technology, No. 1088 Xueyuan Blvd, Shenzhen, Guangdong 518055, China
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    • Xiaosheng Tang
      Xiaosheng Tang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
      Key Laboratory of Optoelectronic Technology & Systems (Ministry of Education), College of Optoelectronic Engineering, Chongqing University, Chongqing 400044, China
    • Qiang Huang*
      Qiang Huang
      School of Optoelectronic Engineering, Chongqing University of Posts and Telecommunications, Chongqing 400065, China
      *Email: [email protected]
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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2025, 64, 5, 2480–2488
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    https://doi.org/10.1021/acs.inorgchem.4c04970
    Published January 24, 2025
    Copyright © 2025 American Chemical Society

    Abstract

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    Electrochemical conversion of CO2 into methanol has received extensive attention in recent years since methanol is an efficient energy carrier and industrial feedstock. However, the selectivity to methanol remains unsatisfied. In this work, Sb-doped Cs3Cu2I5 is first and rationally developed for CO2 electrochemical reduction, achieving remarkable high selectivity of methanol. UV–vis absorption, X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations show that the Sb dopants narrow the band gap of Cs3Cu2I5 and enhance the metal–ligand hybridization due to the introduction of Sb 5p orbitals, which accordingly enhance the charge transfer. In addition, the Cu–Sb pair in Sb@Cs3Cu2I5 perovskite synergistically catalyzes the CO2 conversion. The Cu sites serve for CO2 absorption and activation, while the Sb sites stabilize the intermediate *OCH2 through the Sb–O bond due to superior oxygen affinity. The plasma-treated sample with electron-deficient Sb exhibits the best methanol selectivity as high as 88.38%. This work provides new insight into highly efficient metal halide perovskite-based catalysts for CO2 electrochemical conversion.

    Copyright © 2025 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/acs.inorgchem.4c04970.

    • SEM images; HAADF-STEM measurement and the corresponding EDS mapping of CsCuI; calculated band diagram and Nyquist curves of CsCuI and CsCuSbI; survey XPS spectrum and long-term electrolysis experiments of CsCuI, CsCuSbI, and the plasma-treated sample; UV–vis absorption spectrum and Tauc curves of the plasma-treated sample; and in situ FTIR spectra of CsCuI, CsCuSbI, CsCuSbI_20 V, and CsCuSbI_40 V (PDF)

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    Inorganic Chemistry

    Cite this: Inorg. Chem. 2025, 64, 5, 2480–2488
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.inorgchem.4c04970
    Published January 24, 2025
    Copyright © 2025 American Chemical Society

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