Citation: ZHANG Hong-guang, FENG Li-juan, LI Chun-hu, WANG Liang. Preparation of graphitic carbon nitride with nitrogen-defects and its photocatalytic performance in the degradation of organic pollutants under visible light[J]. Journal of Fuel Chemistry and Technology, ;2018, 46(7): 871-878. shu

Preparation of graphitic carbon nitride with nitrogen-defects and its photocatalytic performance in the degradation of organic pollutants under visible light

College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao 266100, China

Corresponding author: WANG Liang, wangliang_good@163.com
Received Date: 2 April 2018
Revised Date: 12 June 2018

Fund Project: The project was supported by the State Key Laboratory of Heavy Oil Processing(MCTL contribution NO.137)the State Key Laboratory of Heavy Oil Processing MCTL contribution NO.137

Figures(13)

Various graphitic carbon nitride (g-C₃N₄) materials having nitrogen defects were synthesized by adding NaHCO₃ during the thermal polymerization of melamine. The as-prepared g-C₃N₄ samples were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), nitrogen adsorption-desorption, X-ray photoelectron spectroscopy (XPS), UV-visual diffuse reflectance spectroscopy (UV-vis DRS) and photoluminescence spectroscopy (PL); their photocatalytic activity in the degradation of Rhodamine B (RhB) under visible light irradiation was investigated. The results demonstrated that the unique nitrogen defects in g-C₃N₄ play an important role in broadening the absorption of visible light and enhancing the separation of electron-hole pairs. The photocatalytic activity of g-C₃N₄ with nitrogen defects is enhanced greatly; the RhB removal rates over the CNK0.005, CNK0.01, and CNK0.05 photocatalysts in 30 min reach 79.8%, 100.0% and 87.6%, respectively. In contrast, the pristine g-C₃N₄ free of nitrogen defects only gives an RhB degration rate of 59.8% under the same reaction conditions.
- g-C₃N₄,
- nitrogen defects,
- visible light,
- organic pollutants,
- degradation
1. [1]
  LU J, WANG Y, HUANG J, CAO L Y, LI J Y, HAI G J, BAI Z. One-step synthesis of g-C₃N₄, hierarchical porous structure nanosheets with dramatic ultraviolet light photocatalytic activity[J]. Mater Sci Eng B, 2016,214:19-25. doi: 10.1016/j.mseb.2016.08.003
2. [2]
  LIU Y, ZHANG H, LU Y F, WU J, XIN B F. A simple method to prepare g-C₃N₄/Ag-polypyrrole composites with enhanced visible-light photocatalytic activity[J]. Catal Commun, 2016,87(5):41-44.
3. [3]
  IQBALA W, WANG L Z, TAN X J, ZHANG J L. One-step in situ green template mediated porous graphitic carbon nitride for efficient visible light photocatalytic activity[J]. J Environ Chem Eng, 2017,5(4):3500-3507. doi: 10.1016/j.jece.2017.07.011
4. [4]
  HAO R R, WANG G H, TANG H, SUN L L, XU C, HAN D Y. Template-free preparation of macro/mesoporous g-C₃N₄/TiO₂, heterojunction photocatalysts with enhanced visible light photocatalytic activity[J]. Appl Catal B:Environ, 2016,187(15):47-58.
5. [5]
  SHI X W, Fujitsuka M, LOU Z Z, ZHANG P, Majima T. In situ nitrogen-doped hollow-TiO₂/g-C₃N₄ composite photocatalyst with efficient charge separation boosting water reduction under visible light[J]. J Mater Chem, A, 2017,5(20):9671-9681. doi: 10.1039/C7TA01888F
6. [6]
  CHEN X, CHEN H L, GUAN J, ZHEN J M, SUN Z J, DU P W, LU Y L, YANG S F. A facile mechanochemical route to a covalently bonded graphitic carbon nitride (g-C₃N₄) and fullerene hybrid toward enhanced visible light photocatalytic hydrogen production[J]. Nanoscale, 2017,9(17):5615-5623. doi: 10.1039/C7NR01237C
7. [7]
  HE Y M, CAI J, LI T T, WU Y, LIN H J, ZHAO L H, LUO M F. Efficient degradation of RhB over GdVO₄/g-C₃N₄, composites under visible-light irradiation[J]. Chem Eng J, 2013,215/216:721-730. doi: 10.1016/j.cej.2012.11.074
8. [8]
  LI K, XIE X, ZHANG W D. Photocatalysts based on g-C₃N₄-encapsulating carbon spheres with high visible light activity for photocatalytic hydrogen evolution[J]. Carbon, 2016,110:356-366. doi: 10.1016/j.carbon.2016.09.039
9. [9]
  LU D Z, WANG H M, ZHAO X N, Kondamareddy K K, DING J Q, LI C H, FANG P F. Highly efficient visible-light-induced photoactivity of Z-scheme g-C₃N₄/Ag/MoS₂ ternary photocatalysts for organic pollutant degradation and production of hydrogen[J]. Acs Sustainable Chem Eng, 2017,5(11):1436-1445.
10. [10]
  LI J Q, YUAN H, ZHU Z F. Photoelectrochemical performance of g-C₃N₄/Au/BiPO₄ Z-scheme composites to improve the mineralization property under solar light[J]. Rsc Adv, 2016,6(74):70563-70572. doi: 10.1039/C6RA13570F
11. [11]
  YU X, SHI J J, FENG L J, LI C H, WANG L. A three-dimensional BiOBr/RGO heterostructural aerogel with enhanced and selective photocatalytic properties under visible light[J]. Appl Surf Sci, 2017,396:1775-1782. doi: 10.1016/j.apsusc.2016.11.219
12. [12]
  LIANG S J, XIA Y Z, ZHU S Y, ZHENG S, HE Y H, BI J H, LIU M H, WU L. Au and Pt co-loaded g-C₃N₄, nanosheets for enhanced photocatalytic hydrogen production under visible light irradiation[J]. Appl Surf Sci, 2015,358:304-312. doi: 10.1016/j.apsusc.2015.08.035
13. [13]
  TIAN Y M, GE L, WANG K Y, CHAI Y S. Synthesis of novel MoS₂/g-C₃N₄, heterojunction photocatalysts with enhanced hydrogen evolution activity[J]. Mater Charact, 2014,87:70-73. doi: 10.1016/j.matchar.2013.10.020
14. [14]
  WENG S X, HU J, LU M L, YE X X, PEI Z X, HUANG M L, XIE L Y, LIN S, LIU P. In situ photogenerated defects on surface-complex BiOCl (010) with high visible-light photocatalytic activity:A probe to disclose the charge transfer in BiOCl (010)/surface-complex system[J]. Appl Catal B:Environ, 2015,163:205-213. doi: 10.1016/j.apcatb.2014.07.051
15. [15]
  HONG Z H, SHEN B, CHEN Y L, LIN B Z, GAO B F. Enhancement of photocatalytic H₂ evolution over nitrogen-deficient graphitic carbon nitride[J]. J Mater Chem A, 2013,1(38):11754-11761. doi: 10.1039/c3ta12332d
16. [16]
  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]. Adv Mater, 2014,26(47):8046-8052. doi: 10.1002/adma.v26.47
17. [17]
  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. Potocatalysis:Alkali-assisted synthesis of nitrogen deficient graphitic carbon nitride with tunable band structures for efficient visible light-driven hydrogen evolution[J]. Adv Mater, 2017,29(16):5148-5154.
18. [18]
  WU M, YAN J M, ZHANG X W, ZHAO M. Synthesis of g-C₃N₄with heating acetic acid treated melamine and its photocatalytic activity for hydrogen evolution[J]. Appl Surf Sci, 2015,354(2):196-200.
19. [19]
  SHANG Y Y, MA Y J, CHEN X, XIONG X, PAN J. Effect of sodium doping on the structure and enhanced photocatalytic hydrogen evolution performance of graphitic carbon nitride[J]. Mol Catal, 2017,433:128-135. doi: 10.1016/j.mcat.2016.12.021
20. [20]
  CHIDHAMBARAM N, RAVICHANDRAN K. Single step transformation of urea into metal-free g-C₃N₄ nanoflakes for visible light photocatalytic applications[J]. Mater Lett, 2017,207:44-48. doi: 10.1016/j.matlet.2017.07.040
21. [21]
  CHEN H, YAO J H, QIU P X, XU C M, JIANG F, WANG X. Facile surfactant assistant synthesis of porous oxygen-doped graphitic carbon nitride nanosheets with enhanced visible light photocatalytic activity[J]. Mater Res Bull, 2017,91:42-48. doi: 10.1016/j.materresbull.2017.02.042
22. [22]
  ZHENG Y, ZHANG Z S, LI C H, PROULX S. Surface hydroxylation of graphitic carbon nitride:Enhanced visible light photocatalytic activity[J]. Mater Res Bull, 2016,84:46-56. doi: 10.1016/j.materresbull.2016.07.003
23. [23]
  WANG X J, TIAN X, LI F T, LI Y P, ZHAO J, HAO Y J, LIU Y. Synchronous surface hydroxylation and porous modification of g-C₃N₄ for enhanced photocatalytic H₂ evolution efficiency[J]. Int J Hydrogen Energy, 2016,41(6):3888-3895. doi: 10.1016/j.ijhydene.2016.01.004
24. [24]
  ZHENG Y, ZHANG Z S, LI C H. Beta-FeOOH-supported graphitic carbon nitride as an efficient visible light photocatalyst[J]. J Mol Catal A:Chem, 2016,423:463-471. doi: 10.1016/j.molcata.2016.07.032
25. [25]
  MAO M M, CHEN F, ZHENG C C, NING J Q, ZHONG Y J, HU Y. Facile synthesis of porous Bi₂O₃-BiVO₄ p-n heterojunction composite microrods with highly efficient photocatalytic degradation of phenol[J]. J Alloys Compd, 2016,688:1080-1087. doi: 10.1016/j.jallcom.2016.07.128
26. [26]
  MA X J, LI X R, LI M M, MA X C, YU L, DAI Y. Effect of the structure distortion on the high photocatalytic performance of C₆₀/g-C₃N₄ composite[J]. Appl Surf Sci, 2017,414:124-130. doi: 10.1016/j.apsusc.2017.04.019
27. [27]
  SUN Y J, ZHANG W D, XIONG T, ZHAO Z W, DONG F, WANG R Q, HO W K. Growth of BiOBr nanosheets on C₃N₄ nanosheets to construct two-dimensional nanojunctions with enhanced photoreactivity for NO removal[J]. J Colloid Interface Sci, 2014,418:317-323. doi: 10.1016/j.jcis.2013.12.037
28. [28]
  LI H, ZHANG T X, PAN C, PU C C, HU Y, HU X Y, LIU E Z, FAN J. Self-assembled Bi₂MoO₆/TiO₂ nanofiber heterojunction film with enhanced photocatalytic activities[J]. Appl Surf Sci, 2017,391:303-310. doi: 10.1016/j.apsusc.2016.06.167
29. [29]
  HOFFMANN M R, MARTIN S T, CHOI W Y, BAHNEMANN D W. Environmental applications of semiconductor photocatalysis[J]. Chem Rev, 1995,95(1):69-96. doi: 10.1021/cr00033a004
30. [30]
  DING J, XU W, WAN H, YUAN D S, CHEN C, WANG L, GUAN G F, DAI W L. Nitrogen vacancy engineered graphitic C₃N₄-based polymers for photocatalytic oxidation of aromatic alcohols to aldehydes[J]. Appl Catal B:Environ, 2018,221:626-634. doi: 10.1016/j.apcatb.2017.09.048
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