Journal
CHEMICAL ENGINEERING JOURNAL
Volume 425, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.131844
Keywords
Photocatalyst H-2 evolution; Visible-light-driven; Nitrogen defects; pi-conjugated system; g-C3N4
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Funding
- National Natural Science Foundation of China [21706104, 21806060]
- Natural Science Foundation of Jiangsu Province [BK20190245]
- China Postdoctoral Science Foundation [2017M611732, 2016M590418, 2019M661750]
- Jiangsu Province Postdoctoral Research Funding Project [2020Z005]
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The study demonstrates the potential of utilizing a precise molecular tunability strategy to enhance the photocatalytic performance of metal-free photocatalysts for hydrogen evolution. By integrating N defect engineering and pi-conjugation structure into g-C3N4, the photocatalytic hydrogen evolution rate was significantly increased, providing insights on the role of structural defects in improving photocatalytic activity.
The precise molecular tunability strategy is deemed to have great potential to improve the photocatalytic performance of metal-free photocatalysts for applying in hydrogen evolution but remains a formidable task. We herein cover a logical design for integrating N defect engineering and pi-conjugation structure into g-C3N4. The photocatalytic hydrogen evolution rate of up to 1541.6 mu mol g(-1) h(-1) is acquired over the optimum DCN350, which has 7.5-fold increase over primal g-C3N4 (205.9 mu mol g(-1) h(-1)). The experimental study and density functional theory (DFT) investigations confirm that DCN350 with N defects not only can shorten band gaps for expanding the light absorption range via optimizing the electronic band structure, but also act as active sites for facilitating hydrogen evolution reaction. Besides, the -C=N as strong electron-withdrawing functional group can make the isolated valence electrons delocalized to drive the charge spatial separation. Therefore, the light absorption capacity and charge separation/transfer of g-C3N4 can be flexibly mastered via changing calcination temperature of g-C3N4 and NaBH4. Overall, this study provides an opportunity for having a deep understanding the role of structural defects on ameliorating the photocatalytic evolution hydrogen activity.
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