Two-Dimensional Benzobisthiazole-Vinylene-Linked Covalent Organic Frameworks Outperform One-Dimensional Counterparts in Photocatalysis

Publikation: Beitrag in FachzeitschriftForschungsartikelBeigetragenBegutachtung

Beitragende

  • Shengxu Li - , CAS - Ningbo Institute of Material Technology and Engineering, Zhejiang University of Technology (Autor:in)
  • Rui Ma - , CAS - Technical Institute of Physics and Chemistry (Autor:in)
  • Shunqi Xu - , Professur für Molekulare Funktionsmaterialien (cfaed) (Autor:in)
  • Tianyue Zheng - , CAS - Ningbo Institute of Material Technology and Engineering (Autor:in)
  • Huaping Wang - , CAS - Technical Institute of Physics and Chemistry (Autor:in)
  • Guangen Fu - , CAS - Ningbo Institute of Material Technology and Engineering (Autor:in)
  • Haoyong Yang - , CAS - Ningbo Institute of Material Technology and Engineering (Autor:in)
  • Yang Hou - , Zhejiang University (Autor:in)
  • Zhongquan Liao - , Fraunhofer-Institut für Keramische Technologien und Systeme (Autor:in)
  • Bozhen Wu - , Zhejiang University of Technology (Autor:in)
  • Xinliang Feng - , Professur für Molekulare Funktionsmaterialien (cfaed) (Autor:in)
  • Li Zhu Wu - , CAS - Technical Institute of Physics and Chemistry (Autor:in)
  • Xu Bing Li - , CAS - Technical Institute of Physics and Chemistry (Autor:in)
  • Tao Zhang - , CAS - Ningbo Institute of Material Technology and Engineering (Autor:in)

Abstract

Vinylene/olefin-linked two-dimensional covalent organic frameworks (v-2D-COFs), featured with vinylene-linked in-plane conjugations, high chemical stabilities, and designable chemical structures, are promising for optoelectronic/photocatalytic applications. Developing v-2D-COFs with superior π-conjugation and optoelectronic properties is meaningful but remains challenging. In this work, we present the crystalline benzobisthiazole-bridged unsubstituted v-2D-COF (v-2D-COF-NS1 and v-2D-COF-NS2) synthesized via a benzothiazole-mediated aldol-type polycondensation. Interestingly, the resultant v-2D-COF exhibits a high chemical stability under both strong acidic (12 M HCl) and basic conditions (saturated KOH) due to the robust vinylene-linked skeletons. Moreover, the electron-deficient thiazole units and 2D π-conjugations endow v-2D-COFs (i.e., v-2D-COF-NS1) a narrow band gap of ∼1.85 eV with a conduction band of −3.65 eV vs vacuum, which are desirable for photocatalytic hydrogen evolution. As such, the v-2D-COF-NS1-based photoelectrode gives a photocurrent up to ∼47 μA cm-2 at 0.3 V vs reversible hydrogen electrode (RHE), which is much higher than the value of the corresponding linear polymer (LP-NS1) and outstanding among the reported COF photoelectrodes. Under a continuous visible light irradiation, v-2D-COF-NS1 generates hydrogen gas with an excellent rate of ∼4.4 mmol h-1 g-1 over 12 h. This work demonstrates the synthesis of unsubstituted v-2D-COFs that intrinsically contain benzobisthiazole-based building blocks and shows great potential in photocatalytic reactions.

Details

OriginalspracheEnglisch
Seiten (von - bis)1089-1096
Seitenumfang8
FachzeitschriftACS catalysis
Jahrgang13
Ausgabenummer2
PublikationsstatusVeröffentlicht - 20 Jan. 2023
Peer-Review-StatusJa

Externe IDs

WOS 000915560200001

Schlagworte

Forschungsprofillinien der TU Dresden

ASJC Scopus Sachgebiete

Schlagwörter

  • 2D materials, benzothiazole-mediated aldol-type polycondensation, organic semiconductor, photocatalytic hydrogen evolution, vinylene-linked covalent organic frameworks, Photocatalytic hydrogen evolution, Benzothiazole-mediated aldol-type polycondensation, Vinylene-linked covalent organic frameworks, Organic semiconductor