Polarization Engineering of Covalent Triazine Frameworks for Highly Efficient Photosynthesis of Hydrogen Peroxide from Molecular Oxygen and Water

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review

130 Scopus Citations
View graph of relations

Author(s)

  • Chongbei Wu
  • Zhenyuan Teng
  • Chao Yang
  • Fangshuai Chen
  • Hong Bin Yang
  • Lei Wang
  • Hangxun Xu
  • Gengfeng Zheng
  • Qing Han

Detail(s)

Original languageEnglish
Article number2110266
Journal / PublicationAdvanced Materials
Volume34
Issue number28
Online published7 May 2022
Publication statusPublished - 14 Jul 2022
Externally publishedYes

Abstract

Two-electron oxygen photoreduction to hydrogen peroxide (H2O2) is seriously inhibited by its sluggish charge kinetics. Herein, a polarization engineering strategy is demonstrated by grafting (thio)urea functional groups onto covalent triazine frameworks (CTFs), giving rise to significantly promoted charge separation/transport and obviously enhanced proton transfer. The thiourea-functionalized CTF (Bpt-CTF) presents a substantial improvement in the photocatalytic H2O2 production rate to 3268.1 µmol h−1 g−1 with no sacrificial agents or cocatalysts that is over an order of magnitude higher than unfunctionalized CTF (Dc-CTF), and a remarkable quantum efficiency of 8.6% at 400 nm. Mechanistic studies reveal the photocatalytic performance is attributed to the prominently enhanced two-electron oxygen reduction reaction by forming endoperoxide at the triazine unit and highly concentrated holes at the thiourea site. The generated O2 from water oxidation is subsequently consumed by the oxygen reduction reaction (ORR), thereby boosting overall reaction kinetics. The findings suggest a powerful functional-groups-mediated polarization engineering method for the development of highly efficient metal-free polymer-based photocatalysts. © 2022 Wiley-VCH GmbH.

Research Area(s)

  • charge separation and transfer, covalent triazine frameworks, photosynthesis of hydrogen peroxide, polarization engineering, thio(urea) functional groups

Citation Format(s)

Polarization Engineering of Covalent Triazine Frameworks for Highly Efficient Photosynthesis of Hydrogen Peroxide from Molecular Oxygen and Water. / Wu, Chongbei; Teng, Zhenyuan; Yang, Chao et al.
In: Advanced Materials, Vol. 34, No. 28, 2110266, 14.07.2022.

Research output: Journal Publications and ReviewsRGC 21 - Publication in refereed journalpeer-review