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author:

Zheng, Y. (Zheng, Y..) [1] | Liu, W. (Liu, W..) [2] | Li, G. (Li, G..) [3] | Chen, Y. (Chen, Y..) [4] | Wang, Y. (Wang, Y..) [5] | Fang, L. (Fang, L..) [6] | Rao, X. (Rao, X..) [7] | Sun, K. (Sun, K..) [8] | Qin, C. (Qin, C..) [9] | Jiang, J. (Jiang, J..) [10]

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Scopus

Abstract:

Short-lived shallow trapping states in photocatalysts created from polymeric semiconductors impedes the effective use of charge carriers, leading to a decrease in the solar-to-hydrogen conversion efficiency of covalent triazine frameworks (CTF). In this study, methylene-modified covalent triazine frameworks (M−CTF) with increased structural distortion were synthesized through a dynamic trimerization reaction of cyano groups using the precursors of 1,4-terephthalonitrile and 1,4-phenylenediacetonitrile. The optimal M−CTF catalyst obtained in this approach showed persistent shallow trapping states through n-π* electronic transitions, leading to a noticeable red-shift in the light absorption edge to 600 nm. Femtosecond transient absorption spectroscopy verified the existence of shallow trapping states with extended lifetimes (1103.8 ps) in M−CTF. The distorted structure promote increased involvement of photo-induced electrons in reducing water to generate H2, leading to a substantial improvement in the ability of M−CTF to catalyze the production of H2. M−CTF sample loaded with Pt cocatalysts exhibited an impressive efficiency of 10.1 mmol·g−1·h −1 in producing H2 via photocatalysis under visible light (λ > 420 nm), marking a tenfold improvement compared to the original CTF. The findings underscore the significance of structural distortion in CTF for achieving long-lasting shallow trapping states, leading to improved photocatalytic efficiency. © 2024 Elsevier Inc.

Keyword:

Covalent triazine frameworks Distortion Hydrogen evolution Photocatalysis Shallow trapping state

Community:

  • [ 1 ] [Zheng Y.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 2 ] [Liu W.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 3 ] [Li G.]State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou, 350116, China
  • [ 4 ] [Chen Y.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 5 ] [Wang Y.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 6 ] [Fang L.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 7 ] [Rao X.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 8 ] [Sun K.]College of Materials Science and Engineering, Xiamen Key Laboratory of Optoelectronic Materials and Advanced Manufacturing, Academy of Advanced Carbon Conversion Technology, Fujian Provincial Key Laboratory of Biomass Low-Carbon Conversion, Huaqiao University, Xiamen, 361021, China
  • [ 9 ] [Sun K.]Jiangsu Province Key Laboratory of Biomass Energy and Materials, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry (CAF), No. 16, Suojin Five Village, Nanjing, 210042, China
  • [ 10 ] [Qin C.]Henan Key Laboratory of Infrared Materials and Spectrum Measures and Applications, School of Physics, Henan Normal University, Xinxiang, 453007, China
  • [ 11 ] [Jiang J.]Jiangsu Province Key Laboratory of Biomass Energy and Materials, Institute of Chemical Industry of Forest Products, Chinese Academy of Forestry (CAF), No. 16, Suojin Five Village, Nanjing, 210042, China

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Source :

Journal of Catalysis

ISSN: 0021-9517

Year: 2025

Volume: 442

6 . 5 0 0

JCR@2023

Cited Count:

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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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