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author:

Wu, S. (Wu, S..) [1] | Cheng, X. (Cheng, X..) [2] | Huang, H. (Huang, H..) [3] | Yang, Q. (Yang, Q..) [4] | Wang, Y. (Wang, Y..) [5] | Zhuang, Y. (Zhuang, Y..) [6] | Li, W. (Li, W..) [7] | Liu, Y. (Liu, Y..) [8] | Lin, H. (Lin, H..) [9] | Niu, H. (Niu, H..) [10] | Wang, J. (Wang, J..) [11] | Wu, K. (Wu, K..) [12] | Fu, X. (Fu, X..) [13] | Long, J. (Long, J..) [14]

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Abstract:

Achieving fast exciton dissociation is a critical factor for optimizing the performance of organic photocatalysts in solar energy conversion. This work demonstrates the end-group-dependent ultrafast exciton dissociation in supramolecular perylene monoimide (PMI) nanostructures. A series of PMI molecules are designed by connecting the amide site with methylene carboxyl (─CH2─COOH), methylene phosphonic acid (─CH2─PO3H2), and methylene sulfonic acid (─CH2─SO3H) to increase the dipole moment and built-in electric field, thereby effectively diminishing exciton binding energy. Upon photoexcitation, self-assembled PMI-CH2-SO3H nanoribbons (NRs), which exhibit the lowest exciton binding energy of 29.4 meV, achieve ultrafast exciton dissociation within 0.25 ps, leading to the formation of charge-separated excitons from charge-transfer states. This dissociation rate is ≈40 and 16 times faster than that observed in PMI-CH2-COOH (NRs) and PMI-CH2-PO3H2 (NRs), respectively. Following the deposition of Pt nanoparticles on PMI NRs, Pt/PMI-CH2-SO3H (NRs) demonstrates an H2 evolution of 21.2 mmol g−1 h−1 under visible light irradiation (λ > 420 nm), outperforming Pt/PMI-CH2-COOH (NRs) and Pt/PMI-CH2-PO3H2 (NRs) by factors of 53 and 5.4, respectively. © 2025 Wiley-VCH GmbH.

Keyword:

built-in electric fields hydrogen evolution perylene monoimide photocatalysis supramolecular organic semiconductors

Community:

  • [ 1 ] [Wu S.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 2 ] [Cheng X.]Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, 350002, China
  • [ 3 ] [Huang H.]School of Energy and Environment, Southeast University, Nanjing, 210096, China
  • [ 4 ] [Yang Q.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 5 ] [Wang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 6 ] [Zhuang Y.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 7 ] [Li W.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 8 ] [Liu Y.]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China
  • [ 9 ] [Lin H.]Beijing Key Laboratory for Green Catalysis and Separation, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
  • [ 10 ] [Niu H.]Beijing Key Laboratory for Green Catalysis and Separation, College of Materials Science and Engineering, Beijing University of Technology, Beijing, 100124, China
  • [ 11 ] [Wang J.]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China
  • [ 12 ] [Wu K.]State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China
  • [ 13 ] [Fu X.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 14 ] [Long J.]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350108, China

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Small

ISSN: 1613-6810

Year: 2025

Issue: 14

Volume: 21

1 3 . 0 0 0

JCR@2023

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 2

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