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Bipyridine-Confined Silver Single-Atom Catalysts Facilitate In-Plane C–O Coupling for Propylene Electrooxidation
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    Bipyridine-Confined Silver Single-Atom Catalysts Facilitate In-Plane C–O Coupling for Propylene Electrooxidation
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    • Mingfang Chi
      Mingfang Chi
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
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    • Jiankang Zhao
      Jiankang Zhao
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
    • Jingwen Ke
      Jingwen Ke
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
      More by Jingwen Ke
    • Yan Liu
      Yan Liu
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
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    • Ruyang Wang
      Ruyang Wang
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
      More by Ruyang Wang
    • Chuanhao Wang
      Chuanhao Wang
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
    • Sung-Fu Hung
      Sung-Fu Hung
      Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu 300, Taiwan
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    • Tsung-Ju Lee
      Tsung-Ju Lee
      Department of Applied Chemistry, National Yang Ming Chiao Tung University, Hsinchu 300, Taiwan
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    • Zhigang Geng*
      Zhigang Geng
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
      *[email protected]
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    • Jie Zeng*
      Jie Zeng
      Hefei National Research Center for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
      School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma’anshan, Anhui 243002, P. R. China
      *[email protected]
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    Other Access OptionsSupporting Information (1)

    Nano Letters

    Cite this: Nano Lett. 2024, 24, 5, 1801–1807
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    https://doi.org/10.1021/acs.nanolett.3c04978
    Published January 26, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    The electrooxidation of propylene presents a promising route for the production of 1,2-propylene glycol (PG) under ambient conditions. However, the C–O coupling process remains a challenge owing to the high energy barrier. In this work, we developed a highly efficient electrocatalyst of bipyridine-confined Ag single atoms on UiO-bpy substrates (Ag SAs/UiO-bpy), which exposed two in-plane coordination vacancies during reaction for the co-adsorption of key intermediates. Detailed structure and electronic property analyses demonstrate that CH3CHCH2OH* and *OH could stably co-adsorb in a square planar configuration, which then accelerates the charge transfer between them. The combination of stable co-adsorption and efficient charge transfer facilitates the C–O coupling process, thus significantly lowering its energy barrier. At 2.4 V versus a reversible hydrogen electrode, Ag SAs/UiO-bpy achieved a record-high activity of 61.9 gPG m–2 h–1. Our work not only presents a robust electrocatalyst but also advances a new perspective on catalyst design for propylene electrooxidation.

    Copyright © 2024 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.nanolett.3c04978.

    • Detailed methods (synthesis, instrumentation, characterizations, electrochemical measurements, and DFT calculations) and additional data (PDF)

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    Cited By

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    This article is cited by 8 publications.

    1. Yini Chen, Zirui Ma, Lei Song, Yuan Hu, Yanbei Hou, Fukai Chu, Weizhao Hu. Pyridine-N-Anchored Ag Strategy Facilitated Br– Adsorption via Ultrahigh Exposure and Coordination Unsaturation of Ag. Nano Letters 2025, 25 (14) , 5697-5704. https://doi.org/10.1021/acs.nanolett.4c06683
    2. Areti Moutsiou, Andrea Olivati, Luis A. Cipriano, Alessandra Sivo, Sean M. Collins, Quentin M. Ramasse, Ik Seon Kwon, Giovanni Di Liberto, Mohamad Kanso, Robert Wojcieszak, Gianfranco Pacchioni, Annamaria Petrozza, Gianvito Vilé. Tracking Charge Dynamics in a Silver Single-Atom Catalyst During the Light-Driven Oxidation of Benzyl Alcohol to Benzaldehyde. ACS Catalysis 2025, 15 (7) , 5601-5613. https://doi.org/10.1021/acscatal.4c05208
    3. Nana Sun, Syed Shoaib Ahmad Shah, Zhongyuan Lin, Yan-Zhen Zheng, Long Jiao, Hai-Long Jiang. MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design. Chemical Reviews 2025, 125 (5) , 2703-2792. https://doi.org/10.1021/acs.chemrev.4c00664
    4. Ming Cheng, Jintong Lan, Xiaoxian Sun, Fanyu Wang, Ailijiang Tuerdi, Falong Jia, Yanbing Guo, Xiao Liu. Cascading Water Activation and Interfacial Lattice Oxygen over Nanocluster CuO x ‐Modified MnO 2 for Electrocatalytic Propylene Oxidation. Angewandte Chemie 2025, 137 (6) https://doi.org/10.1002/ange.202420780
    5. Ming Cheng, Jintong Lan, Xiaoxian Sun, Fanyu Wang, Ailijiang Tuerdi, Falong Jia, Yanbing Guo, Xiao Liu. Cascading Water Activation and Interfacial Lattice Oxygen over Nanocluster CuO x ‐Modified MnO 2 for Electrocatalytic Propylene Oxidation. Angewandte Chemie International Edition 2025, 64 (6) https://doi.org/10.1002/anie.202420780
    6. Peipei Zhao, Chunmei Liu, Jiamin Ma, Zimei Fu, Meng Bai, Yang Gao, He Xiao, Junwei Wu, Man Zhao, Jianfeng Jia. Recent advances in constructing efficient materials for electrocatalytic oxidation of propylene. Journal of Molecular Structure 2025, 1323 , 140778. https://doi.org/10.1016/j.molstruc.2024.140778
    7. Cheng Peng, Mingyue Wang, Sha Li, Xuezhi Zeng, Jieyue Wang, Wenhai Wang, Zhirong Zhang, Mingfu Ye, Xianwen Wei, Konglin Wu, Kui Zhang, Jie Zeng. A General Strategy Based on Hetero‐Charge Coupling Effect for Constructing Single‐Atom Sites. Angewandte Chemie International Edition 2024, 63 (36) https://doi.org/10.1002/anie.202408771
    8. Cheng Peng, Mingyue Wang, Sha Li, Xuezhi Zeng, Jieyue Wang, Wenhai Wang, Zhirong Zhang, Mingfu Ye, Xianwen Wei, Konglin Wu, Kui Zhang, Jie Zeng. A General Strategy Based on Hetero‐Charge Coupling Effect for Constructing Single‐Atom Sites. Angewandte Chemie 2024, 136 (36) https://doi.org/10.1002/ange.202408771

    Nano Letters

    Cite this: Nano Lett. 2024, 24, 5, 1801–1807
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.3c04978
    Published January 26, 2024
    Copyright © 2024 American Chemical Society

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