Doping-induced enhancement of crystallinity in polymeric carbon nitride nanosheets to improve their visible-light photocatalytic activity

Structural defects can greatly inhibit electron transfer in two-dimensional (2D) layered polymeric carbon nitride (CN) unit, seriously lowering its utilization ratio of photogenerated charges during photocatalysis. Herein, we propose a new strategy based on intra-melon hydrogen bonding interactions...

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Bibliographic Details
Published in:Nanoscale 2019-04, Vol.11 (14), p.6876-6885
Main Authors: Li, Yuan-Yuan, Zhou, Bing-Xin, Zhang, Hua-Wei, Ma, Shao-Fang, Huang, Wei-Qing, Peng, Wei, Hu, Wangyu, Huang, Gui-Fang
Format: Article
Language:English
Subjects:
Carbon
Carbon nitride
Catalytic activity
Charge materials
Charge transfer
Crystal defects
Crystal structure
Crystallinity
Current carriers
Dyes
Electron transfer
Excitons
Heat treatment
Hydrogen bonding
Migration
Nanosheets
Optoelectronics
Oxygen evolution reactions
Photocatalysis
Rhodamine
Separation
Two dimensional materials
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Summary:Structural defects can greatly inhibit electron transfer in two-dimensional (2D) layered polymeric carbon nitride (CN) unit, seriously lowering its utilization ratio of photogenerated charges during photocatalysis. Herein, we propose a new strategy based on intra-melon hydrogen bonding interactions in 2D CN frameworks to improve the crystallinity of CN. This concept was validated by removing some amino groups and connecting melon using codoped B and F atoms via a simple one-step sodium fluoroborate-assisted thermal treatment. The enhancement in crystallinity effectively promoted exciton dissociation and charge transfer in the CN nanosheets. Furthermore, the B/F dopants also improved the separation of photogenerated carriers by promoting charge capture. The highly efficient visible-light photocatalytic activity of the crystalline B/F-codoped CN nanosheets was demonstrated by degrading methyl orange, Rhodamine B, colorless phenol and tetracycline hydrochloride as models, where their degradation rate constant was more than 10, 5, 32 and 3 times higher than that of pure CN, respectively. Moreover, the B/F-codoped CN exhibited an excellent photoelectrocatalytic performance for the oxygen evolution reaction (OER), outperforming the precious-metal IrO2 catalyst. The simple and effective strategy proposed herein provides a direct route to engineer high crystallinity in 2D materials for tunable charge carrier separation and migration for electronic and optoelectronic applications.
ISSN:2040-3364
2040-3372
DOI:10.1039/c9nr00229d