Citation: Wang Huijing, Zhang Jun, Wang Pu, Yin Linlin, Tian Yu, Li Junjing. Bifunctional copper modified graphitic carbon nitride catalysts for efficient tetracycline removal: Synergy of adsorption and photocatalytic degradation[J]. Chinese Chemical Letters, ;2020, 31(10): 2789-2794. doi: 10.1016/j.cclet.2020.07.043 shu

Bifunctional copper modified graphitic carbon nitride catalysts for efficient tetracycline removal: Synergy of adsorption and photocatalytic degradation

Wang Huijing ^a, ,
Zhang Jun ^a,*, ,
Wang Pu ^a, ,
Yin Linlin ^a, ,
Tian Yu ^a, ,
Li Junjing ^b,

a.
State Key Laboratory of Urban Water Resources and Environment(SKLUWRE), School of Environment, Harbin Institute of Technology, Harbin 150090, China
b.
State Key Laboratory of Separation Membranes and Membrane Processes, School of Environmental and Chemical Engineering, Tianjin Polytechnic University, Tianjin 300387, China

hitsunyboy@126.com

Received Date: 13 March 2020
Revised Date: 3 July 2020
Accepted Date: 17 July 2020
Available Online: 30 July 2020

Figures(4)

In order to efficiently remove tetracycline in wastewater through the synergistic effect of adsorption and photocatalytic degradation, a series of novel composite materials (Cu doped g-C₃N₄) were synthesized by two-pot hydrothermal method. It was found that the composite materials with optimized ratio (Cu/CN-1) displayed outstanding adsorption and photocatalytic performance as compared with pure g-C₃N₄ photocatalyst. The removal efficiency of tetracycline (TC, 50 mg/L) reached almost 99% within 30 min by Cu/CN-1 through the synergy of adsorption and photocatalysis under visible-light irradiation, which was the highest removal efficiency ever reported. The adsorption kinetics and isotherms of TC on the Cu/CN-1 were well fitted with the pseudo-second-order kinetic model and Langmuir model, respectively. Moreover, it was confirmed that the main effective reactive groups were O₂^·- and h⁺ in photocatalytic process. The Cu/CN-1 exhibited high stability and excellent reusability after five cycle experiments. Finally, the mechanism of synergy between Cu and g-C₃N₄ was proposed: on the one hand, the decoration of Cu particles significantly increased the adsorption sites of Cu/CN-1 to tetracycline, on the other hand, the modification of Cu particles effectively inhibits charge recombination and broadens the visible light absorption range of the photocatalyst.This study provided a promising photocatalyst to be used for TC removal in the actual wastewater.
- Carbon nitride,
- Tetracycline,
- Adsorption,
- Photocatalysis,
- Environment remediation
1. [1]
  K.J. Choi, S.G. Kim, C.W. Kim, S.H. Kim, Chemosphere 66(2007) 977-984. doi: 10.1016/j.chemosphere.2006.07.037
2. [2]
  Y. Wang, H. Zhang, J. Zhang, et al., J. Hazard. Mater. 192(2011) 35-43.
3. [3]
  R. Daghrir, P. Drogui, Environ. Chem. Lett. 11(2013) 209-227. doi: 10.1007/s10311-013-0404-8
4. [4]
  D. Jiang, T. Wang, Q. Xu, et al., Appl. Catal. B: Environ. 201(2017) 617-628. doi: 10.1016/j.apcatb.2016.09.001
5. [5]
  Z. Li, L. Zhu, W. Wu, S. Wang, L. Qiang, Appl. Catal. B: Environ. 192(2016) 277-285. doi: 10.1016/j.apcatb.2016.03.045
6. [6]
  H. Xiong, D. Zou, D. Zhou, et al., Chem. Eng. J. 316(2017) 7-14. doi: 10.1016/j.cej.2017.01.083
7. [7]
  R. Gothwal, T. Shashidhar, Air Water 43(2015) 479-489. doi: 10.1002/clen.201300989
8. [8]
  S. Gartiser, E. Urich, R. Alexy, K. Kummerer, Chemosphere 67(2007) 604-613. doi: 10.1016/j.chemosphere.2006.08.038
9. [9]
  A.G. Trovo, R.F. Nogueira, A. Aguera, et al., Water Res. 45(2011) 1394-1402. doi: 10.1016/j.watres.2010.10.029
10. [10]
  Y. Yue, Z. Peng, W. Wang, et al., Powder Technol. 347(2019) 211-219.
11. [11]
  Y. Wu, J. Lu, M. Meng, et al., Chem. Eng. J. 309(2017) 263-271. doi: 10.1016/j.cej.2016.10.044
12. [12]
  C. Song, B.B. Guo, X.F. Sun, et al., Chem. Eng. J. 358(2019) 1139-1146. doi: 10.1016/j.cej.2018.10.119
13. [13]
  F. Chen, Q. Yang, S. Wang, et al., Appl. Catal. B: Environ. 209(2017) 493-505. doi: 10.1016/j.apcatb.2017.03.026
14. [14]
  Q. Gu, Y. Liao, L. Yin, et al., Appl. Catal. B: Environ. 165(2015) 503-510. doi: 10.1016/j.apcatb.2014.10.045
15. [15]
  Y. Song, J. Qi, J. Tian, S. Gao, F. Cui, Chem. Eng. J. 341(2018) 547-555. doi: 10.1016/j.cej.2018.02.063
16. [16]
  M. Wu, H. Lv, T. Wang, T. An, S. Wang, Catal. Today 315(2018) 205-212. doi: 10.1016/j.cattod.2018.01.019
17. [17]
  J. Chen, X. Xiao, Y. Wang, Z. Ye, Appl. Surf. Sci. 467(2019) 1000-1010.
18. [18]
  L. Li, Z. Cai, Q. Wu, et al., J. Am. Chem. Soc. 138(2016) 7681-7686. doi: 10.1021/jacs.6b03472
19. [19]
  J. Xu, M. Fujitsuka, S. Kim, Z. Wang, T. Majima, et al., Appl. Catal. B: Environ. 241(2019) 141-148. doi: 10.1016/j.apcatb.2018.09.023
20. [20]
  J. Xu, Z. Wang, Y. Zhu, ACS Appl. Mater. Interfaces 9(2017) 27727-27735. doi: 10.1021/acsami.7b07657
21. [21]
  H. Wang, Y. Wu, M. Feng, J.W. Chew, et al., Water Res. 144(2018) 215-225. doi: 10.1016/j.watres.2018.07.025
22. [22]
  H. Yi, M. Yan, D. Huang, et al., Appl. Catal. B: Environ. 250(2019) 52-62. doi: 10.1016/j.apcatb.2019.03.008
23. [23]
  S.C. Wang, Z.Y. Teng, Y.Q. Xu, et al., Appl. Catal. B: Environ. 260(2020)118145. doi: 10.1016/j.apcatb.2019.118145
24. [24]
  Y. Luo, X. Wei, B. Gao, et al., Chem. Eng. J. 375(2019)122019. doi: 10.1016/j.cej.2019.122019
25. [25]
  A. Shahzeydi, M. Ghiaci, H. Farrokhpour, et al., Chem. Eng. J. 370(2019) 1310-1321. doi: 10.1016/j.cej.2019.03.227
26. [26]
  Y. Sheng, Z. Wei, H. Miao, et al., Chem. Eng. J. 370(2019) 287-294. doi: 10.1016/j.cej.2019.03.197
27. [27]
  N. Li, Y. Tian, J. Zhao, et al., Chem. Eng. J. 352(2018) 412-422. doi: 10.1016/j.cej.2018.07.038
28. [28]
  H. Sudrajat, J. Alloys. Compd. 716(2017) 119-127. doi: 10.1016/j.jallcom.2017.04.302
29. [29]
  M. Zhou, M. Tian, C. Li, Chem 27(2016) 1188-1199.
30. [30]
  M. Zhu, L.S. Zhang, S. Liu, et al., Chin. Chem. Lett. 31(2020) 1961-1965. doi: 10.1016/j.cclet.2020.01.017
31. [31]
  H. Zhang, Q.Q. Ji, L.D. Lai, G. Yao, B. Lai, Chin. Chem. Lett. 30(2019) 1129-1132. doi: 10.1016/j.cclet.2019.01.025
32. [32]
  C.K. Wu, M. Yin, S. O'Brien, J.T. Koberstein, Chem. Mater. 18(2006) 6054-6058. doi: 10.1021/cm061596d
33. [33]
  J. Kang, H.J. Liu, Y.M. Zheng, J.H. Qu, J.P. Chen, J. Colloid Interface Sci. 344(2010) 117-125. doi: 10.1016/j.jcis.2009.11.049
34. [34]
  F.C. Wu, R.L. Tseng, R.S. Juang, J. Colloid Interf. Sci. 283(2005) 49-56. doi: 10.1016/j.jcis.2004.08.037
35. [35]
  W.R. Chen, C.H. Huang, Chemosphere 79(2010) 779-785. doi: 10.1016/j.chemosphere.2010.03.020
36. [36]
  L.L. Ji, W. Chen, L. Duan, D.Q. Zhu, Environ. Sci. Technol. 43(2009) 2322-2327. doi: 10.1021/es803268b
37. [37]
  P.H. Chang, Z.H. Li, T.L. Yu, et al., J. Hazard. Mater. 165(2009) 148-155. doi: 10.1016/j.jhazmat.2008.09.113
38. [38]
  J. Kang, H. Liu, Y.M. Zheng, J. Qu, J.P. Chen, J. Colloid Interface Sci. 354(2010) 261-267.
39. [39]
  M.A. Gondal, X.F. Chang, Z.H. Yamani, Chem. Eng. J. 165(2010) 250-257. doi: 10.1016/j.cej.2010.09.025
40. [40]
  M.B. Gawande, A. Goswami, F.X. Felpin, T. Asefa, X. Huang, et al., Chem. Rev. 116(2016) 3722-3811. doi: 10.1021/acs.chemrev.5b00482
41. [41]
  W.P. Xiong, Z.T. Zeng, X. Li, et al., Chemosphere 210(2018) 1061-1069. doi: 10.1016/j.chemosphere.2018.07.084
42. [42]
  G. Zhang, J. Qu, H. Liu, A.T. Cooper, R. Wu, Chemosphere 68(2007) 1058-1066. doi: 10.1016/j.chemosphere.2007.01.081
43. [43]
  H. Xiong, D. Zou, D. Zhou, et al., Chem. Eng. J. 316(2017) 7-14. doi: 10.1016/j.cej.2017.01.083
44. [44]
  Y. Zhang, J. Zhou, X. Chen, L. Wang, W. Cai, Chem. Eng. J. 369(2019) 745-757. doi: 10.1016/j.cej.2019.03.108
45. [45]
  X. Chang, G. Ji, K. Shen, et al., J. Alloys. Compd. 482(2009) 240-245. doi: 10.1016/j.jallcom.2009.03.169
46. [46]
  D. Zhang, H. Niu, X. Zhang, Z. Meng, Y. Cai, J. Hazard. Mater. 192(2011) 1088-1093. doi: 10.1016/j.jhazmat.2011.06.015
47. [47]
  G.L. Liu, J.H. Zhou, W.N. Zhao, Z.M. Ao, T.C. An, Chin. Chem. Lett. 31(2020) 1966-1969. doi: 10.1016/j.cclet.2019.12.023
48. [48]
  L. Duan, L. Li, Z. Xu, W. Chen, Environ. Sci. Proc. Impacts 16(2014) 1462-1468. doi: 10.1039/c4em00096j
49. [49]
  K. Hu, X. Xiao, X. Cao, J. Nan, et al., J. Hazard. Mater. 192(2011) 514-520. doi: 10.1016/j.jhazmat.2011.05.053
50. [50]
  J. Xue, S. Ma, Y. Zhou, Z. Zhang, M. He, ACS Appl. Mater. Interfaces 7(2015) 9630-9637. doi: 10.1021/acsami.5b01212
51. [51]
  X. Shi, M. Fujitsuka, Z. Lou, P. Zhang, T. Majima, J.Mater. Chem. A 5(2017) 9671-9681. doi: 10.1039/C7TA01888F
52. [52]
  M.A. Gondal, X.F. Chang, Z.H. Yamani, Chem. Eng. J. 165(2010) 250-257. doi: 10.1016/j.cej.2010.09.025
53. [53]
  Y. Gao, Y. Li, L. Zhang, et al., J. Colloid Interface Sci. 368(2012) 540-546. doi: 10.1016/j.jcis.2011.11.015
54. [54]
  R.A. Figueroa, A. Allison Leonard, A.A. Mackay, Environ. Sci. Technol. 38(2004) 476-483. doi: 10.1021/es0342087
55. [55]
  P. Niu, L. Zhang, G. Liu, H.M. Cheng, Adv. Funct. Mater. 22(2012) 4763-4770. doi: 10.1002/adfm.201200922
56. [56]
  Y. Wang, Y. Zheng, S. Lu, et al., ACS Appl. Mater. Interf.aces 7(2015) 6093-6101. doi: 10.1021/acsami.5b00980
57. [57]
  J. Zhang, M. Zhang, C. Yang, X. Wang, Adv. Mater. 26(2014) 4121-4126. doi: 10.1002/adma.201400573
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