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author:

Fu, Guangen (Fu, Guangen.) [1] | Yang, Denghui (Yang, Denghui.) [2] | Xu, Shunqi (Xu, Shunqi.) [3] | Li, Shengxu (Li, Shengxu.) [4] | Zhao, Yuxiang (Zhao, Yuxiang.) [5] | Yang, Haoyong (Yang, Haoyong.) [6] | Wu, Daheng (Wu, Daheng.) [7] | Petkov, Petko Stoev (Petkov, Petko Stoev.) [8] | Lan, Zhi-An (Lan, Zhi-An.) [9] | Wang, Xinchen (Wang, Xinchen.) [10] (Scholars:王心晨) | Zhang, Tao (Zhang, Tao.) [11]

Indexed by:

EI Scopus SCIE

Abstract:

Sp(2)-carbon-conjugated covalent organic frameworks (sp(2)c-COFs) have emerged as promising platforms for phototo-chemical energy conversion due to their tailorable optoelectronic properties, in-plane pi-conjugations, and robust structures. However, the development of sp(2)c-COFs in photocatalysis is still highly hindered by their limited linkage chemistry. Herein, we report a novel thiadiazole-bridged sp(2)c-COF (sp(2)c-COF-ST) synthesized by thiadiazole-mediated aldol-type polycondensation. The resultant sp(2)c-COF-ST demonstrates high chemical stability under strong acids and bases (12 M HCl or 12 M NaOH). The electro-deficient thiadiazole together with fully conjugated and planar skeleton endows sp(2)c-COF-ST with superior photoelectrochemical performance and charge-carrier separation and migration ability. As a result, when employed as a photocathode, sp(2)c-COF-ST exhibits a significant photocurrent up to similar to 14.5 mu A cm(-2) at 0.3 V vs reversible hydrogen electrode (RHE) under visible-light irradiation (>420 nm), which is much higher than those analogous COFs with partial imine linkages (mix-COF-SNT similar to 9.5 mu A cm(-2)) and full imine linkages (imi-COF-SNNT similar to 4.9 mu A cm(-2)), emphasizing the importance of the structure-property relationships. Further temperature-dependent photoluminescence spectra and density functional theory calculations demonstrate that the sp(2)c-COF-ST has smaller exciton binding energy as well as effective mass in comparison to mix-COF-SNT and imi-COF-SNNT, which suggests that the sp(2)c-conjugated skeleton enhances the exciton dissociation and carrier migration under light irradiation. This work highlights the design and preparation of thiadiazole-bridged sp(2)c-COFs with promising photocatalytic performance.

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Community:

  • [ 1 ] [Fu, Guangen]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 2 ] [Li, Shengxu]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 3 ] [Zhao, Yuxiang]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 4 ] [Yang, Haoyong]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 5 ] [Wu, Daheng]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 6 ] [Zhang, Tao]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China
  • [ 7 ] [Yang, Denghui]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 8 ] [Lan, Zhi-An]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 9 ] [Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China
  • [ 10 ] [Xu, Shunqi]Tech Univ Dresden, Ctr Adv Elect Dresden CFAED, D-01062 Dresden, Germany
  • [ 11 ] [Xu, Shunqi]Tech Univ Dresden, Fac Chem & Food Chem, D-01062 Dresden, Germany
  • [ 12 ] [Xu, Shunqi]Univ Strasbourg, CNRS, ISIS, UMR7006, 8 Allee Gaspard Monge, F-67000 Strasbourg, France
  • [ 13 ] [Petkov, Petko Stoev]Univ Sofia, Fac Chem & Pharm, Sofia 1164, Bulgaria

Reprint 's Address:

  • 蓝志安 王心晨

    [Zhang, Tao]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Marine Mat & Related Technol, Ningbo 315201, Peoples R China;;[Lan, Zhi-An]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China;;[Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350108, Peoples R China

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Source :

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

ISSN: 0002-7863

Year: 2024

Issue: 2

Volume: 146

Page: 1318-1325

1 4 . 5 0 0

JCR@2023

Cited Count:

WoS CC Cited Count: 62

SCOPUS Cited Count: 64

ESI Highly Cited Papers on the List: 4 Unfold All

  • 2025-1
  • 2024-11
  • 2024-9
  • 2024-7

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

Online/Total:118/10071228
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