Construction of double-functionalized g-C3N4 heterojunction structure via optimized charge transfer for the synergistically enhanced photocatalytic degradation of sulfonamides and H2O2 production

Jiapeng Zhong; Jiaxing Huang; Yang Liu; Daguang Li; Cuiwen Tan; Pin Chen; Haijin Liu; Xiaoshan Zheng; Chenghui Wen; Wenying Lv; Guoguang Liu

doi:10.1016/j.jhazmat.2021.126868

Construction of double-functionalized g-C₃N₄ heterojunction structure via optimized charge transfer for the synergistically enhanced photocatalytic degradation of sulfonamides and H₂O₂ production

J Hazard Mater. 2022 Jan 15:422:126868. doi: 10.1016/j.jhazmat.2021.126868. Epub 2021 Aug 10.

Authors

Affiliations

¹ School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China.
² Guangdong Provincial Key laboratory of Petrochemical Pollution processes and Control, School of Environmental Science and Engineering, Guangdong University of Petrochemical Technology, Maoming, Guangdong 525000, China.
³ School of Environment, Henan Normal University, Key Laboratory for Yellow River and Huaihe River Water Environment and Pollution Control, Xinxiang 453007, China.
⁴ School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China. Electronic address: liugg615@163.com.

PMID: 34418826
DOI: 10.1016/j.jhazmat.2021.126868

Abstract

Herein, supporting g-C₃N₄ embedded with benzene-ring (BCN) on P-modified g-C₃N₄ (PCN) successfully synthesized the homogeneous photocatalyst BCN/PCN (PBCN) via a simple thermal polymerization reaction. Under blue-light (LED) irradiation, the optimized PBCN (0.448 min^-1) demonstrated excellent photocatalytic performance, attaining over 74 times the degradation rate for sulfisoxazole (SSZ) in contrast to non-functionalized g-C₃N₄ (CN, 0.006 min^-1). Theoretical calculations revealed that the substitution of heterocyclic rings in the g-C₃N₄ triazine networks with benzene-rings enabled them to serve as electron donors, while promoting photoinduced spatial charge dissociation. Further, the carrier PCN tended to serve as electron acceptors to form electron-rich corner-phosphorous sites. Reactive species experiments demonstrate that the O₂˙^- and h⁺ constituted the primary photocatalytic mechanism of SSZ degradation. The potential SSZ degradation routes were predicted based on the transformation products via mass spectrometry. Finally, the composite materials also exhibited excellent photocatalytic activity in the conversion of solar energy to chemical energy (H₂O₂). This study guides the rational modification of g-C₃N₄-based semiconductors to achieve green energy production and beneficial ecological applications.

Keywords: Density functional theory; Graphite carbon nitride; H(2)O(2) production; Heterojunction; Photocatalytic degradation sulfonamides.