Hydrazone-Linked Heptazine Polymeric Carbon Nitrides for Synergistic Visible-Light-Driven Catalysis
Abstract
Heptazine-based conjugated polymeric carbon nitrides (PCNs) are promising metal-free photocatalysts, yet their synthesis is challenging due to the electron-deficiency and insolubility of heptazine units. Indeed, heptazine-containing polymers have only been prepared through nucleophilic substitution with amines by using toxic cyameluric chloride as the starting material. Herein, we report the novel and environmentally friendly method for preparing heptazine-based mesoporous PCNs with hydrazone links formed through a simple Schiff base condensation of melem-NH2 and aldehydes. Unlike cyameluric chloride, melem-NH2 is non-toxic, stable, and can be readily obtained from melem and hydrazine in solution. We demonstrate that the hydrazone linkages and the heptazine units synergistically enhance the photocatalytic activity of PCNs in visible-light-driven aerobic oxidation of benzyl alcohol to benzaldehyde. In particular, the polymer constructed from melem-NH2 and p-phthalaldehyde shows 17 times more activity than graphitic carbon nitride (g-C3N4).
- Authors:
-
[2];
[4]
- Fuzhou Univ. (China). College of Materials Science and Engineering; Univ. of Amsterdam (Netherlands). Van't Hoff Inst. for Molecular Sciences (HIMS)
- Fuzhou Univ. (China). College of Materials Science and Engineering
- Ames Lab., Ames, IA (United States)
- Ames Lab., and Iowa State Univ., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Ames Laboratory (AMES), Ames, IA (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1632322
- Alternate Identifier(s):
- OSTI ID: 1631509
- Report Number(s):
- IS-J-10,237
Journal ID: ISSN 0947-6539
- Grant/Contract Number:
- 51703031; 201506140058; AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry - A European Journal
- Additional Journal Information:
- Journal Volume: 26; Journal Issue: 33; Journal ID: ISSN 0947-6539
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; heptazines; hydrazone linkages; porous polymers; synergistic effects; visible light
Citation Formats
Zhang, Wei, Xu, Congying, Kobayashi, Takeshi, Zhong, Yun, Guo, Zhiyong, Zhan, Hongbing, Pruski, Marek, and Huang, Wenyu. Hydrazone-Linked Heptazine Polymeric Carbon Nitrides for Synergistic Visible-Light-Driven Catalysis. United States: N. p., 2020.
Web. doi:10.1002/chem.202000934.
Zhang, Wei, Xu, Congying, Kobayashi, Takeshi, Zhong, Yun, Guo, Zhiyong, Zhan, Hongbing, Pruski, Marek, & Huang, Wenyu. Hydrazone-Linked Heptazine Polymeric Carbon Nitrides for Synergistic Visible-Light-Driven Catalysis. United States. https://doi.org/10.1002/chem.202000934
Zhang, Wei, Xu, Congying, Kobayashi, Takeshi, Zhong, Yun, Guo, Zhiyong, Zhan, Hongbing, Pruski, Marek, and Huang, Wenyu. Tue .
"Hydrazone-Linked Heptazine Polymeric Carbon Nitrides for Synergistic Visible-Light-Driven Catalysis". United States. https://doi.org/10.1002/chem.202000934. https://www.osti.gov/servlets/purl/1632322.
@article{osti_1632322,
title = {Hydrazone-Linked Heptazine Polymeric Carbon Nitrides for Synergistic Visible-Light-Driven Catalysis},
author = {Zhang, Wei and Xu, Congying and Kobayashi, Takeshi and Zhong, Yun and Guo, Zhiyong and Zhan, Hongbing and Pruski, Marek and Huang, Wenyu},
abstractNote = {Heptazine-based conjugated polymeric carbon nitrides (PCNs) are promising metal-free photocatalysts, yet their synthesis is challenging due to the electron-deficiency and insolubility of heptazine units. Indeed, heptazine-containing polymers have only been prepared through nucleophilic substitution with amines by using toxic cyameluric chloride as the starting material. Herein, we report the novel and environmentally friendly method for preparing heptazine-based mesoporous PCNs with hydrazone links formed through a simple Schiff base condensation of melem-NH2 and aldehydes. Unlike cyameluric chloride, melem-NH2 is non-toxic, stable, and can be readily obtained from melem and hydrazine in solution. We demonstrate that the hydrazone linkages and the heptazine units synergistically enhance the photocatalytic activity of PCNs in visible-light-driven aerobic oxidation of benzyl alcohol to benzaldehyde. In particular, the polymer constructed from melem-NH2 and p-phthalaldehyde shows 17 times more activity than graphitic carbon nitride (g-C3N4).},
doi = {10.1002/chem.202000934},
journal = {Chemistry - A European Journal},
number = 33,
volume = 26,
place = {United States},
year = {Tue Jun 02 00:00:00 EDT 2020},
month = {Tue Jun 02 00:00:00 EDT 2020}
}
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