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Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

Author

Listed:
  • Zhongshan Chen

    (North China Electric Power University)

  • Jingyi Wang

    (North China Electric Power University)

  • Mengjie Hao

    (North China Electric Power University)

  • Yinghui Xie

    (North China Electric Power University)

  • Xiaolu Liu

    (North China Electric Power University)

  • Hui Yang

    (North China Electric Power University)

  • Geoffrey I. N. Waterhouse

    (The University of Auckland)

  • Xiangke Wang

    (North China Electric Power University)

  • Shengqian Ma

    (University of North Texas)

Abstract

Covalent organic frameworks (COFs) represent an emerging class of organic photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry to construct a family of isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties and local pore characteristics of the COFs modulated using different linkers. The excited state electronic distribution and transport pathways in the COFs are probed using a host of experimental methods and theoretical calculations at a molecular level. One of our developed COFs (denoted as COF-4) exhibits a remarkable excited state electron utilization efficiency and charge transfer properties, achieving a record-high photocatalytic uranium extraction performance of ~6.84 mg/g/day in natural seawater among all techniques reported so far. This study brings a new understanding about the operation of COF-based photocatalysts, guiding the design of improved COF photocatalysts for many applications.

Suggested Citation

  • Zhongshan Chen & Jingyi Wang & Mengjie Hao & Yinghui Xie & Xiaolu Liu & Hui Yang & Geoffrey I. N. Waterhouse & Xiangke Wang & Shengqian Ma, 2023. "Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36710-x
    DOI: 10.1038/s41467-023-36710-x
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    Cited by:

    1. Yanghui Hou & Peng Zhou & Fuyang Liu & Ke Tong & Yanyu Lu & Zhengmao Li & Jialiang Liang & Meiping Tong, 2024. "Rigid covalent organic frameworks with thiazole linkage to boost oxygen activation for photocatalytic water purification," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Yinghui Xie & Qiuyu Rong & Fengyi Mao & Shiyu Wang & You Wu & Xiaolu Liu & Mengjie Hao & Zhongshan Chen & Hui Yang & Geoffrey I. N. Waterhouse & Shengqian Ma & Xiangke Wang, 2024. "Engineering the pore environment of antiparallel stacked covalent organic frameworks for capture of iodine pollutants," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Wei Li & Wen Duan & Guocheng Liao & Fanfan Gao & Yusen Wang & Rongxia Cui & Jincai Zhao & Chuanyi Wang, 2024. "0.68% of solar-to-hydrogen efficiency and high photostability of organic-inorganic membrane catalyst," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Xiaolu Liu & Yinghui Xie & Mengjie Hao & Yang Li & Zhongshan Chen & Hui Yang & Geoffrey I. N. Waterhouse & Xiangke Wang & Shengqian Ma, 2024. "Secondary metal ion-induced electrochemical reduction of U(VI) to U(IV) solids," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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