Template-free large-scale synthesis of g-C3N4 microtubes for enhanced visible light-driven photocatalytic H2 production
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A template-free hydrothermal-assisted thermal polymerization method has been developed for the large-scale synthesis of one-dimensional (1D) graphitic carbonnitride (g-C3N4) microtubes. The g-C3N4 microtubes were obtained by simple thermal polymerization of melamine-cyanuric acid complex microrods under N2 atmosphere, which were synthesized by hydrothermal treatment of melamine solution at 180 °C for 24 h. The as-obtained g-C3N4microtubes exhibited a large surface area and a unique one-dimensional tubular structure, which provided abundant active sites for proton reduction and also facilitated the electron transfer processes. As such, the g-C3N4 microtubes showed enhanced photocatalytic H2 productionactivity in lactic acid aqueous solutions under visible light irradiation (λ ≥ 420 nm), which was ∼ 3.1 times higher than that of bulk g-C3N4 prepared by direct thermal polymerization of the melamine precursor under the same calcination conditions.
Keywordsg-C3N4 microtubes photocatalytic water splitting visible light response
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This work was supported by the National Basic Research Program of China (No. 2014CB239402), the National Key Projects for Fundamental Research and Development of China (Nos. 2016YFB0600901, 2017YFA0206904, and 2017YFA0206900), the National Natural Science Foundation of China (Nos. 51772305, 51572270, U1662118, and 21401207), the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB17000000), and the Youth Innovation Promotion Association of the CAS.
- Yu, H. J.; Shi, R.; Zhao, Y X.; Bian, T.; Zhao, Y. F.; Zhou, C.; Waterhouse, G. I. N.; Wu, L.-Z. Tung, C.-H.; Zhang, T. R. Alkali-assisted synthesis of nitrogen deficient graphitic carbon nitride with tunable band structures for efficient visible-light-driven hydrogen evolution. Adv. Mater. 2017, 29, 1605148.CrossRefGoogle Scholar
- Zhang, G G.; Li, G. S.; Lan, Z. A.; Lin, L. H.; Savateev, A.; Heil, T.; Zafeiratos, S.; Wang, X. C.; Antonietti, M. Optimizing optical absorption, exciton dissociation, and charge transfer of a polymeric carbon nitride with ultrahigh solar hydrogen production activity. Angew. Chem, Int. Ed 2017, 56, 13445–13449.CrossRefGoogle Scholar
- Liu, C. Y; Huang, H. W.; Ye, L. Q.; Yu, S. X.; Tian, N.; Du, X.; Zhang, T. R.; Zhang, Y. H. Intermediate-mediated strategy to horn-like hollow mesoporous ultrathin g-C3N4 tube with spatial anisotropic charge separation for superior photocatalytic H2 evolution. Nano Energy 2017, 41, 738–748.CrossRefGoogle Scholar
- Zhao, Y; Zhao, F.; Wang, X. P.; Xu, C. Y.; Zhang, Z. P.; Shi, G. Q.; Qu, L. T. Graphitic carbon nitride nanoribbons: Grapheneassisted formation and synergic function for highly efficient hydrogen evolution. Angew. Chem., Int. Ed. 2014, 53, 1393413939.Google Scholar
- Tahir, M.; Cao, C. B.; Mahmood, N.; Butt, F. K.; Mahmood, A.; Idrees, F.; Hussain, S.; Tanveer, M.; Ali, Z.; Aslam, I. Multifunctional g-C3N4 nanofibers: A template-free fabrication and enhanced optical, electrochemical, and photocatalyst properties. ACSAppl. Mater. Interfaces 2014, 6, 1258–1265.CrossRefGoogle Scholar
- Guo, Q. X.; Xie, Y; Wang, X. J.; Zhang, S. Y; Hou. T.; Lv, S. C. Synthesis of carbon nitride nanotubes with the C3N4 stoichiometry via a benzene-thermal process at low temperatures. Chem. Commun. 2004, 26–27.Google Scholar
- Lee, K.; Mazare, A.; Schmuki, P. One-dimensional titanium dioxide nanomaterials: Nanotubes. Chem. Rev. 2014, 114, 93859454.Google Scholar
- Zhang, H. J.; Zuo, X. Q.; Tang, H. B.; Li, G; Zhou, Z. Origin of photoactivity in graphitic carbon nitride and strategies for enhancement of photocatalytic efficiency: Insights from firstprinciples computations. Phys. Chem. Chem. Phys. 2015, 17, 62806288.Google Scholar
- Ong, W. J.; Putri, L. K.; Tan, Y C.; Tan, L. L.; Li, N.; Ng, Y. H.; Wen, X. M.; Chai, S. P. Unravelling charge carrier dynamics in protonated g-C3N4 interfaced with carbon nanodots as co-catalysts toward enhanced photocatalytic CO2 reduction: A combined experimental and first-principles DFT study. Nano Res. 2017, 10, 1673–1696.CrossRefGoogle Scholar
- Guo, S. E.; Deng, Z. P.; Li, M. X.; Jiang, B. J.; Tian, C. G.; Pan, Q. J.; Fu, H. G. Phosphorus-doped carbon nitride tubes with a layered micro-nanostructure for enhanced visible-light photocatalytic hydrogen evolution. Angew. Chem., Int. Ed. 2016, 55, 18301834.Google Scholar
- Zhang, Q.; Joo, J.-B.; Lu, Z. D.; Dahl, M.; Oliveira, D. Q. L.; Ye, M. M.; Yin, Y. D. Self-assembly and photocatalysis of mesoporous TiO2 nanocrystal clusters. Nano Res. 2011, 4, 103114.Google Scholar