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  Defect-rich ultrathin poly-heptazine-imide-framework nanosheets with alkali-ion doping for photocatalytic solar hydrogen and selective benzylamine oxidation

Zhu, C., Luo, X., Liu, C., Wang, Y., Chen, X., Wang, Y., et al. (2022). Defect-rich ultrathin poly-heptazine-imide-framework nanosheets with alkali-ion doping for photocatalytic solar hydrogen and selective benzylamine oxidation. Nano Research. doi:10.1007/s12274-022-4519-8.

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 Creators:
Zhu, Chaofeng, Author
Luo, Xiao, Author
Liu, Congyan, Author
Wang, Yang, Author
Chen, Xihai, Author
Wang, Yang1, Author           
Hu, Qing, Author
Wu, Xiaojun, Author
Liu, Bo, Author
Affiliations:
1Markus Antonietti, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863321              

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Free keywords: carbon nitride; photocatalysis; alkali ion doping; hydrogen production; amine oxidative coupling
 Abstract: Polymeric carbon nitride (CN) as a metal-free photocatalyst holds great promise to produce high-value chemicals and H2 fuel utilizing clean solar energy. However, the wider deployment of pristine CN is critically hampered by the poor charge carrier transport and high recombination. Herein, we develop a facile salt template-assisted interfacial polymerization strategy that in-situ introduces alkali ions (Na+, K+) and nitrogen defects in CN (denoted as v-CN-KNa) to simultaneously promote charge separation and transportation and steer photoexcited holes and electrons to their oxidation and reduction sites. The photocatalyst exhibits an impressive photocatalytic H2 evolution rate of 8641.5 µmol·g-1·h-1 (33-fold higher than pristine CN) and also works readily in real seawater (10752.0 µmol·g-1·h-1) with a high apparent quantum efficiency up to 18.5% at 420 nm. In addition, we further demonstrate that the v-CN-KNa can simultaneously produce H2 and N-benzylidenebenzylamine without using any other sacrificial reagent. In situ characterizations and DFT calculations reveal that the alkali ions notably promote charge transport, while the nitrogen defects generate abundant edge active sites, which further contribute to efficient electron excitation to trigger photoredox reactions.

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Language(s): eng - English
 Dates: 2022-07-23
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1007/s12274-022-4519-8
 Degree: -

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Title: Nano Research
  Abbreviation : Nano Res.
Source Genre: Journal
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Publ. Info: Beijing, China : Tsinghua University Press
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 1998-0124