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A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes, involving direct heating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios. Supramolecular structures formed between the precursor molecules guided nanotube formation. The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier migration and separation, thereby enhancing photocatalytic H2 production in 20 vol.% lactic acid under visible light irradiation. Nanotubes synthesized using melamine and urea in a 1:10 mass ratio (denoted herein as CN-MU nanotubes) exhibited a photocatalytic hydrogen production rate of 1, 073.6 μmol·h-1·g-1 with Pt as the cocatalyst, a rate of 4.7 and 3.1 times higher than traditional Pt/g-C3N4 photocatalysts prepared from graphitic carbon nitride (g-C3N4) obtained by direct thermal polymerization of melamine or urea, respectively. On the basis of their outstanding performance for photocatalytic H2 production, it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas, including photocatalytic CO2 reduction, dye-sensitized solar cells and photoelectrochemical sensors.


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Supramolecular precursor strategy for the synthesis of holey graphitic carbon nitride nanotubes with enhanced photocatalytic hydrogen evolution performance

Show Author's information Xiaoshuai Wang1,3,§Chao Zhou1,§Run Shi1Qinqin Liu3Geoffrey I. N. Waterhouse4Lizhu Wu1Chen-Ho Tung1Tierui Zhang1,2( )
Key Laboratory of Photochemical Conversion and Optoelectronic MaterialsTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing100190China
Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing100049China
School of Materials Science and EngineeringJiangsu UniversityZhenjiang212013China
School of Chemical SciencesThe University of AucklandAuckland1142New Zealand

§ Xiaoshuai Wang and Chao Zhou contributed equally to this work.

Abstract

A simple one-step thermal polymerization method was developed for synthesis of holey graphitic carbon nitride nanotubes, involving direct heating of mixtures of melamine and urea or melamine and cyanuric acid in specific mass ratios. Supramolecular structures formed between the precursor molecules guided nanotube formation. The porous and nanotubular structure of the nanotubes facilitated efficient charge carrier migration and separation, thereby enhancing photocatalytic H2 production in 20 vol.% lactic acid under visible light irradiation. Nanotubes synthesized using melamine and urea in a 1:10 mass ratio (denoted herein as CN-MU nanotubes) exhibited a photocatalytic hydrogen production rate of 1, 073.6 μmol·h-1·g-1 with Pt as the cocatalyst, a rate of 4.7 and 3.1 times higher than traditional Pt/g-C3N4 photocatalysts prepared from graphitic carbon nitride (g-C3N4) obtained by direct thermal polymerization of melamine or urea, respectively. On the basis of their outstanding performance for photocatalytic H2 production, it is envisaged that the holey g-C3N4 nanotubes will find widespread uptake in other areas, including photocatalytic CO2 reduction, dye-sensitized solar cells and photoelectrochemical sensors.

Keywords: graphitic carbon nitride, photocatalysis, hydrogen evolution, holey nanotubes, visible-light response

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Publication history
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Acknowledgements

Publication history

Received: 31 December 2018
Revised: 19 February 2019
Accepted: 22 February 2019
Published: 08 March 2019
Issue date: September 2019

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Acknowledgements

Acknowledgements

The authors are grateful for the financial support from the National Key R&D Program of China (Nos. 2018YFB1502002, 2017YFA0206904, 2017YFA0206900, and 2016YFB0600901), the National Natural Science Foundation of China (Nos. 51825205, U1662118, 51772305, 51572270, 21871279, and 21802154), the Beijing Natural Science Foundation (Nos. 2191002, 2182078, and 2194089), the Beijing Municipal Science and Technology Project (No. Z181100005118007), the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB17000000), the Royal Society-Newton Advanced Fellowship (No. NA170422), the International Partnership Program of Chinese Academy of Sciences (No. GJHZ1819) and the K. C. Wong Education Foundation. G. I. N. W. acknowledges funding support from the Energy Education Trust of New Zealand and the University of Auckland Faculty Research Development Fund.

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