Journal
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 44, Issue 36, Pages 20029-20041Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2019.06.038
Keywords
Photocatalysis; H-2; g-C3N4/S-PAN; pi-conjugation heterojunction; Mesoporous
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Funding
- National Natural Science Foundation of China [21805115, 21576112, 21606114]
- NSFC-Shanxi Coal Based Low Carbon Joint Fund [U1810117]
- Postdoctoral Science Foundation of China [2017M611712, 2017M611717]
- Jiangsu Planned Projects for postdoctoral Research Funds [1701025A]
- Scientific Research Foundation for Senior Talent of Jiangsu University [17JDG020]
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Simultaneously extended pi-conjugated system and provide abundant pore structure of semiconductor photocatalysts for hydrogen (H-2) production is highly desirable. Hence, a novel mesoporous sulfurized polyacrylonitrile modified g-C3N4 (g-C3N4/S-PAN) pi-conjugation heterojunction is firstly fabricated by one-step strategy under the sulfur-induced cyclization reaction and pore-creating effect. Excitedly, the g-C3N4/S-PAN pi-conjugation heterojunction extends the n-conjugated system in favor of speeding up the photo generated electron transfer, which is due to strengthen the pi-pi interactions between the SPAN and g-C3N4 and S-PAN is more apt to accept electrons. And the obtained g-C3N4/S-PAN Tc-conjugation heterojunction with mesoporous structure also provide abundant activesites for proton reduction. Accordingly, the g-C3N4/S-PAN-2 pi-conjugation heterojunction shows the optimal photocatalytic H-2 evolution (PHE) activity (736.24 gmol h(-1)g(-1)), which is approximately 2.15 times higher than pristine g-C3N4. In addition, the relationships of the optical and photoelectrochemical properties with photocatalytic activity are revealed in depth based on the first-principles calculations of band structure and density of states (DOS). This work provides a new one-step strategy to obtain g-C3N4-based pi-conjugation heterojunction with the unique microstructure for improving PHE activity. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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