Manipulation of n → π* electronic transitions via implanting thiophene rings into two-dimensional carbon nitride nanosheets for efficient photocatalytic water purification
Abstract
The photocatalytic performance of polymeric carbon nitride (C3N4) is heavily restricted by insufficient n → π* electronic transitions and limited active sites. To this end, we adopted an integrated copolymerization and repyrolysis approach to fabricate two-dimensional thiophene ring implanted (C3N4) nanosheets (2D Thing-CNNS). Advanced characterization studies demonstrated that the fusion of thiophene rings and the formation of 2D nanosheets significantly collectively elevated the n → π* electronic transitions and enlarged the specific surface areas of 2D Thing-CNNS, leading to a dramatically extended π-conjugated system and accelerated charge migration. Transmission electron microscopy, X-ray diffraction, and solid-state 13C NMR proved the existence of the thiophene ring. Additionally, quantum computations of the highest occupied and lowest unoccupied crystal orbitals implied that the 2D Thing-CNNS are more favorable for carrier migration than pristine (C3N4). The finite element method (FEM) analysis indicates that 2D Thing-CNNS have a stronger surface electric field and radiation absorption, which is consistent with the enhanced n → π* transition. Consequently, 2D Thing-CNNS exhibit a 42.7-fold enhancement in photocatalytic performances for bisphenol A oxidation accordingly, compared with pristine C3N4. This work provides a novel strategy for engineering the electronic structure of C3N4 for highly efficient water purification.
RAS ID
52102
Document Type
Journal Article
Date of Publication
1-1-2022
Funding Information
Australian Research Council
School
School of Engineering
Grant Number
ARC Number : DE210100253
Copyright
subscription content
Publisher
Royal Society of Chemistry
Recommended Citation
He, F., Liu, X., Zhao, X., Zhang, J., Dong, P., Zhang, Y., Zhao, C., Sun, H., Duan, X., Wang, S., & Wang, S. (2022). Manipulation of n → π* electronic transitions via implanting thiophene rings into two-dimensional carbon nitride nanosheets for efficient photocatalytic water purification. DOI: https://doi.org/10.1039/d2ta04975a
Comments
He, F., Liu, X., Zhao, X., Zhang, J., Dong, P., Zhang, Y., ... & Wang, S. (2022). Manipulation of n→ π* electronic transitions via implanting thiophene rings into two-dimensional carbon nitride nanosheets for efficient photocatalytic water purification. Journal of Materials Chemistry A, 10(38), 20559-20570.
https://doi.org/10.1039/d2ta04975a