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  C=C π bond modified graphitic carbon nitride films for enhanced photoelectrochemical cell performance

Bian, J., Xi, L., Li, J., Xiong, Z., Huang, C., Lange, K., et al. (2017). C=C π bond modified graphitic carbon nitride films for enhanced photoelectrochemical cell performance. Chemistry – An Asian Journal, 12(9), 1005-1012. doi:10.1002/asia.201700178.

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 Creators:
Bian, Juncao1, Author              
Xi, Lifei, Author
Li, Jianfu, Author
Xiong, Ze, Author
Huang, Chao, Author
Lange, Kathrin, Author
Tang, Jinyao, Author
Shalom, Menny2, Author              
Zhang, Rui-Qin, Author
Affiliations:
1Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_1863288              
2Menny Shalom, Kolloidchemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2205635              

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Free keywords: graphitic carbon nitride film, π bond, annealing, electron delocalization, photoelectrochemical cell
 Abstract: Applications of graphitic carbon nitride (g-CN) in photoelectrochemical and optoelectronic devices are still hindered due to the difficulties in synthesis of g-CN films with tunable chemical, physical and catalytic properties. Herein we present a general method to alter the electronic and photoelectrochemical properties of g-CN films by annealing. We found that N atoms can be removed from the g-CN networks after annealing treatment. Assisted by theoretical calculations, we confirm that upon appropriate N removal, the adjacent C atoms will form new C=C π bonds. Detailed calculations demonstrate that the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) are localized at the structure unit with C=C π bonds and the electrons are more delocalized. Valence band X-ray photoelectron spectroscopy spectra together with the absorption spectra unveil that the structure changes result in the alteration of the g-CN energy levels and position of band edges. Our results show that the photocurrent density of the annealed g-CN film is doubled compared with the pristine one, thanks to the better charge separation and transport within the film induced by the new C=C π bonds. An ultrathin TiO2 film (2.2 nm) is applied as stabilizer and the photocurrent density is kept at 0.05 mA/cm2 at 1.23 V vs. reversible hydrogen electrode after two-cycle stability assessment. This work enables the applications of g-CN films in many electronic and optoelectronic devices.

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 Dates: 2017-03-082017
 Publication Status: Published in print
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 Identifiers: DOI: 10.1002/asia.201700178
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Title: Chemistry – An Asian Journal
  Other : Chem. – Asian J.
  Other : Chem. Asian J.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 12 (9) Sequence Number: - Start / End Page: 1005 - 1012 Identifier: ISSN: 1861-4728