Manipulation of n → π* electronic transitions via implanting thiophene rings into two-dimensional carbon nitride nanosheets for efficient photocatalytic water purification

Document Type

Journal Article

Publication Title

Journal of Materials Chemistry A

Publisher

Royal Society of Chemistry

School

School of Engineering

RAS ID

52102

Funders

Australian Research Council

Grant Number

ARC Number : DE210100253

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

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.

DOI

10.1039/d2ta04975a

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