Increasing Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Doping through in situ Polycondensation

doi:10.7517/j.issn.1674-0475.2015.05.434

Abstract

Abstract:

In this paper, g-C₃N₄ with nitrogen vacancy was obtained by carbon doping during in situ polycondensation process from the mixture of dicyandiamide precursor and polyethylene glycol additive. XRD, FTIR, XPS, UV-Vis and FL spectroscopies were employed to investigate the influence of the nitrogen vacancy on the phase structure, composition and chemical states, the light absorption and photocatalytic activity of the as-prepared g-C₃N₄. The results show that in situ carbon doping in the framework of g-C₃N₄ can effectively extend its visible light absorption range to 850 nm. As a consequence, the nitrogen-deficient g-C₃N₄shows much superior photocatalytic activities compared to the pristine g-C₃N₄ in degrading the organic pollutant Rhodamine B and generating hydrogen from aqueous solution containing triethanolamine scavenger under both UV-visible light and visible light irradiation, especially more prominent under visible light irradiation.

Key words: photocatalysis, g-C₃N₄, doping, vacancy, polyethylene glycol

HONG Xingxing, KANG Xiangdong, LIU Gang, CHENG Huiming. Increasing Photocatalytic Activity of Graphitic Carbon Nitride by Carbon Doping through in situ Polycondensation[J]. Imaging Science and Photochemistry, 2015, 33(5): 434-440.

References

[1] Fujishima A, Honda K. Electrochemical photolysis of water at a semiconductor electrode[J]. Nature (London),1972,238(5358): 37-38.
[2] Kudo A,Miseki Y. Heterogeneous photocatalyst materials for water splitting[J]. Chemical Society Reviews,2009, 38(1): 253-278.
[3] Wen F Y,Yang J H,Zong X,Ma Y,Xu Q,Ma B J,Li C. Photocatalytic hydrogen production utilizing solar energy[J]. Progress in Chemistry,2009,21(11): 2285-2302.
[4] Wang X, Maeda K, Thomas A, Takanabe K, Xin G, Carlsson J M, Domen K,Antonietti M. A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J]. Nature Materials, 2009, 8(1): 76-80.
[5] Zhang J H, Wang B, Wang X C. Carbon nitride polymeric semiconductor for photocatalysis[J]. Progress in Chemistry,2014, 26(1) : 19-29.
[6] Goettmann F, Fischer A, Antonietti M,Thomas A. Metal-free catalysis of sustainable Friedel-Crafts reactions: direct activation of benzene by carbon nitrides to avoid the use of metal chlorides and halogenated compounds[J]. Chemical Communications,2006, (43): 4530-4532.
[7] Goettmann F, Fischer A, Antonietti M,Thomas A. Chemical synthesis of mesoporous carbon nitrides using hard templates and their use as a metal-free catalyst for Friedel-Crafts reaction of benzene[J]. Angewandte Chemie-International Edition, 2006, 45(27): 4467-4471.
[8] Niu P, Liu G, Cheng H M. Nitrogen vacancy-promoted photocatalytic activity of graphitic carbon nitride[J]. The Journal of Physical Chemistry C,2012, 116(20): 11013-11018.
[9] Niu P, Yin L C, Yang Y Q, Liu G, Cheng H M. Increasing the visible light absorption of graphitic carbon nitride (melon) photocatalysts by homogeneous self-modification with nitrogen vacancies[J]. Advanced Materials,2014, 26(47): 8046-8052.
[10] Tong H, Ouyang S, Bi Y, Umezawa N, Oshikiri M,Ye J. Nano-photocatalytic materials: possibilities and challenges[J]. Advanced Materials,2012, 24(2): 229-251.
[11] Ni M, Leung M K H, Leung D Y C,Sumathy K. A review and recent developments in photocatalytic water-splitting using TiO₂ for hydrogen production[J]. Renewable and Sustainable Energy Reviews,2007,11(3): 401-425.
[12] Thomas A, Fischer A, Goettmann F, Antonietti M, Müller J O, Schlgl R,Carlsson J M. Graphitic carbon nitride materials: variation of structure and morphology and their use as metal-free catalysts[J]. Journal of Materials Chemistry,2008, 18(41): 4893-4908.
[13] Lotsch B Y, Doeblinger M, Sehnert J, Seyfarth L, Senker J, Oeckler O,Schnick W. Unmasking melon by a complementary approach employing electron diffraction, solid-state NMR spectroscopy, and theoretical calculations-structural characterization of a carbon nitride polymer[J]. Chemistry A Europe Journal,2007, 13(17): 4969-4980.
[14] Bojdys M J, Mueller J O, Antonietti M,Thomas A. Ionothermal synthesis of crystalline, condensed, graphitic carbon nitride[J]. Chemistry A Europe Journal, 2008, 14(27): 8177-8182.
[15] Qiu Y,Gao L. Chemical synthesis of turbostratic carbon nitride, containing C-N crystallites, at atmospheric pressure[J]. Chemical Communications,2003, (18): 2378-2379.