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Ultrafast charge transfer dynamics in 2D covalent organic frameworks/Re-complex hybrid photocatalyst

Author

Listed:
  • Qinying Pan

    (Technical University of Denmark)

  • Mohamed Abdellah

    (Chemical Physics and NanoLund, Lund University
    Qena Faculty of Science, South Valley University)

  • Yuehan Cao

    (State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University)

  • Weihua Lin

    (Chemical Physics and NanoLund, Lund University)

  • Yang Liu

    (State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University)

  • Jie Meng

    (Technical University of Denmark)

  • Quan Zhou

    (Technical University of Denmark)

  • Qian Zhao

    (Technical University of Denmark)

  • Xiaomei Yan

    (Technical University of Denmark)

  • Zonglong Li

    (Institute of Nuclear and New Energy Technology, Tsinghua University)

  • Hao Cui

    (Institute of Nuclear and New Energy Technology, Tsinghua University)

  • Huili Cao

    (Technical University of Denmark)

  • Wenting Fang

    (Technical University of Denmark)

  • David Ackland Tanner

    (Technical University of Denmark)

  • Mahmoud Abdel-Hafiez

    (Uppsala University
    National University of Science and Technology “MISiS”)

  • Ying Zhou

    (State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University)

  • Tonu Pullerits

    (Chemical Physics and NanoLund, Lund University)

  • Sophie E. Canton

    (European XFEL)

  • Hong Xu

    (Institute of Nuclear and New Energy Technology, Tsinghua University)

  • Kaibo Zheng

    (Technical University of Denmark
    Chemical Physics and NanoLund, Lund University)

Abstract

Rhenium(I)-carbonyl-diimine complexes have emerged as promising photocatalysts for carbon dioxide reduction with covalent organic frameworks recognized as perfect sensitizers and scaffold support. Such Re complexes/covalent organic frameworks hybrid catalysts have demonstrated high carbon dioxide reduction activities but with strong excitation energy-dependence. In this paper, we rationalize this behavior by the excitation energy-dependent pathways of internal photo-induced charge transfer studied via transient optical spectroscopies and time-dependent density-functional theory calculation. Under band-edge excitation, the excited electrons are quickly injected from covalent organic frameworks moiety into catalytic RheniumI center within picosecond but followed by fast backward geminate recombination. While under excitation with high-energy photon, the injected electrons are located at high-energy levels in RheniumI centers with longer lifetime. Besides those injected electrons to RheniumI center, there still remain some long-lived electrons in covalent organic frameworks moiety which is transferred back from RheniumI. This facilitates the two-electron reaction of carbon dioxide conversion to carbon monoxide.

Suggested Citation

  • Qinying Pan & Mohamed Abdellah & Yuehan Cao & Weihua Lin & Yang Liu & Jie Meng & Quan Zhou & Qian Zhao & Xiaomei Yan & Zonglong Li & Hao Cui & Huili Cao & Wenting Fang & David Ackland Tanner & Mahmoud, 2022. "Ultrafast charge transfer dynamics in 2D covalent organic frameworks/Re-complex hybrid photocatalyst," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-28409-2
    DOI: 10.1038/s41467-022-28409-2
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    References listed on IDEAS

    as
    1. Tae Wu Kim & Sunhong Jun & Yoonhoo Ha & Rajesh K. Yadav & Abhishek Kumar & Chung-Yul Yoo & Inhwan Oh & Hyung-Kyu Lim & Jae Won Shin & Ryong Ryoo & Hyungjun Kim & Jeongho Kim & Jin-Ook Baeg & Hyotcherl, 2019. "Ultrafast charge transfer coupled with lattice phonons in two-dimensional covalent organic frameworks," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    2. Arthur J. Nozik, 2018. "Utilizing hot electrons," Nature Energy, Nature, vol. 3(3), pages 170-171, March.
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    Cited by:

    1. Chencheng Qin & Xiaodong Wu & Lin Tang & Xiaohong Chen & Miao Li & Yi Mou & Bo Su & Sibo Wang & Chengyang Feng & Jiawei Liu & Xingzhong Yuan & Yanli Zhao & Hou Wang, 2023. "Dual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Ting He & Wenlong Zhen & Yongzhi Chen & Yuanyuan Guo & Zhuoer Li & Ning Huang & Zhongping Li & Ruoyang Liu & Yuan Liu & Xu Lian & Can Xue & Tze Chien Sum & Wei Chen & Donglin Jiang, 2023. "Integrated interfacial design of covalent organic framework photocatalysts to promote hydrogen evolution from water," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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