Citation: Yang Bo, Zhang Yongli. Synergistic Removal of Co-contamination by Heterogeneous Fenton System: Chemical Conversion, pH Effect and Mechanism Analysis[J]. Acta Chimica Sinica, ;2019, 77(10): 1017-1023. doi: 10.6023/A19060203 shu

Synergistic Removal of Co-contamination by Heterogeneous Fenton System: Chemical Conversion, pH Effect and Mechanism Analysis

Yang Bo ,
Zhang Yongli ^,

College of Architecture & Environment, Sichuan University, Chengdu 610065, China

Corresponding author: Zhang Yongli, zxm581212@163.com
Received Date: 8 June 2019
Available Online: 4 October 2019
Fund Project: Project supported by the National Natural Science Foundation of China (No. 51878422)the National Natural Science Foundation of China 51878422

Figures(7)

The chemical transformation of ZVI micro-surface and the degradation mechanism in the process of synergistic removal of copper ions and methylene blue pollutants by ZVI-Fenton system were studied systematically. The samples of ZVI, before and after reaction in the ZVI/H₂O₂ and ZVI/H₂O₂-Cu systems, were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectrometer (EDS), X-ray diffraction (XRD), X-ray photoelectron spectra (XPS) and Fourier Transform infrared spectroscopy (FTIR) to research the changes of ZVI surface structure, Fe and Cu species' chemical conversion. The results showed that the residual corrosion products on the surface of ZVI were more and the corrosion products were mainly Fe₃O₄ and Fe₂O₃ after reaction in the ZVI/H₂O₂ system. However, in the ZVI/H₂O₂-Cu system, the corrosion effect of ZVI was more significant, but the residual corrosion products of ZVI surface were less, and the proportion of Fe₃O₄ increased. In addition, the main reduction product of Cu²⁺ was Cu⁰, which was accompanied by the generation of CuO. Furthermore, the effects of pH on the removal of pollutants from the five systems (ZVI, ZVI-Cu, H₂O₂-Cu, ZVI/H₂O₂ and ZVI/H₂O₂-Cu) were compared and the changes in TCu and TFe concentrations under different pH conditions were monitored. The results indicated that the ZVI/H₂O₂-Cu system not only simultaneous effectively remove MB and TCu compared with other three systems, but also enlarged the effective pH range (pH=2.5~5.5) of ZVI-Fenton system. In addition, free radical capture experiments showed that hydroxyl radicals played an important role in the oxidative degradation of methylene blue, and 10 mmol/L tert-butanol could completely capture hydroxyl radicals in the system. Finally, the mechanism of synergistic removal of TCu and MB degradation by ZVI-Fenton system was revealed. The substitution reaction between ZVI and Cu²⁺, the action of Cu⁰ and ZVI galvanic cells, the acid corrosion effect, and the redox cycle of iron and copper together accelerate the degradation of MB by the system and promote the conversion of ZVI surface substances. This study provides a theoretical basis for collaborative treatment of industrial complex pollutants.
- zero-valent iron powder,
- heterogeneous Fenton,
- cyclic catalysis,
- synergism,
- micro surface transformation
1. [1]
  Fu, F.; Dionysiou, D. D.; Liu, H. J. Hazard. Mater. 2014, 267, 194. doi: 10.1016/j.jhazmat.2013.12.062
2. [2]
  Yamaguchi, R.; Kurosu, S.; Suzuki, M.; Kawase, Y. Chem. Eng. J. 2018, 334, 1537. doi: 10.1016/j.cej.2017.10.154
3. [3]
  Wei, X. Y.; Gao, N. Y.; Li, C. J.; Deng, Y.; Zhou, S. Q.; Li, L. Chem. Eng. J. 2016, 285, 660. doi: 10.1016/j.cej.2015.08.120
4. [4]
  Mirzaei, A.; Chen, Z.; Haghighat, F.; Yerushalmi, L. Chemosphere 2017, 174, 665. doi: 10.1016/j.chemosphere.2017.02.019
5. [5]
  Ling, R.; Chen, J. P.; Shao, J.; Reinhard, M. Water Res. 2018, 134, 44. doi: 10.1016/j.watres.2018.01.065
6. [6]
  Liu, J.; Ou, C.; Han, W.; Faheem, F.; Shen, J.; Bi, H.; Sun, X.; Li, J.; Wang, L. RSC Adv. 2015, 5, 57444. doi: 10.1039/C5RA08487C
7. [7]
  Cho, Y.; Choi, S. I. Chemosphere 2010, 81, 940. doi: 10.1016/j.chemosphere.2010.07.054
8. [8]
  Zheng, Z. Q.; Lu, G. N.; Wang, R.; Huang, K. B.; Tao, X. Q.; Yang, Y. L.; Zou, M. Y.; Xie, Y. Y.; Yin, H. Environ. Pollut. 2019, 245, 780. doi: 10.1016/j.envpol.2018.11.064
9. [9]
  Gu, T. H.; Shi, J. M.; Hua, Y. L.; Liu, J.; Wang, W.; Zhang, W. X. Acta Chim. Sinica 2017, 75, 991.
10. [10]
  Li, Z.; Luo, S. Q.; Yang, Y.; Chen, J. W. Chemosphere 2019, 216, 499. doi: 10.1016/j.chemosphere.2018.10.133
11. [11]
  Cai, C.; Wang, L. G.; Gao, H.; Hou, L. W.; Zhang, H. J. Environ. Sci. 2014, 26, 1267. doi: 10.1016/S1001-0742(13)60598-7
12. [12]
  Cao, C. J.; Liu, X. G.; Ju, X. R.; Chen, X. R. Acta Phys.-Chim. Sin. 2013, 29, 2475. doi: 10.3866/PKU.WHXB201310101
13. [13]
  Huang, X. Y.; Wang, W.; Lin, L.; Zhang, W. X. Acta Chim. Sinica 2017, 75, 529.
14. [14]
  Liu, J.; Gu, T. H.; Wang, W.; Liu, A. R.; Zhang, W. X. Acta Chim. Sinica 2019, 77, 121. doi: 10.3969/j.issn.0253-2409.2019.01.016
15. [15]
  Li, J. H.; Lin, C. F.; Qin, W.; Xiao, X. B.; Wei, L. Acta Phys.-Chim. Sin. 2016, 32, 2717. doi: 10.3866/PKU.WHXB201607271
16. [16]
  Jiang, X.; Qiao, J.; Lo, I. M.; Wang, L.; Guan, X.; Lu, Z.; Zhou, G.; Xu, C. J. Hazard. Mater. 2015, 283, 880. doi: 10.1016/j.jhazmat.2014.10.044
17. [17]
  Fu, R. B.; Yang, Y. P.; Xu, Z.; Zhang, X.; Guo, X. P.; Bi, D. S. Chemosphere 2015, 138, 726. doi: 10.1016/j.chemosphere.2015.07.051
18. [18]
  Diao, Z.-H.; Xu, X.-R.; Jiang, D.; Liu, J.-J.; Kong, L.-J.; Li, G.; Zuo, L.-Z.; Wu, Q.-H. Chem. Eng. J. 2017, 315, 167. doi: 10.1016/j.cej.2017.01.006
19. [19]
  Liu, C. M.; Diao, Z. H.; Huo, W. Y.; Kong, L. J.; Du, J. J. Environ. Pollut. 2018, 239, 698. doi: 10.1016/j.envpol.2018.04.084
20. [20]
  Sleiman, N.; Deluchat, V.; Wazne, M.; Mallet, M.; Courtin-Nomade, A.; Kazpard, V.; Baudu, M. Colloids Surf., A 2017, 514, 1. doi: 10.1016/j.colsurfa.2016.11.014
21. [21]
  Li, H.; Wan, J.; Ma, Y.; Wang, Y.; Huang, M. Chem. Eng. J. 2014, 237, 487. doi: 10.1016/j.cej.2013.10.035
22. [22]
  Xu, C. H.; Zhang, B. L.; Wang, Y. H.; Shao, Q. Q.; Zhou, W. Z.; Fan, D. M.; Bandstra, J. Z.; Shi, Z. Q.; Tratnyek, P. G. Environ. Sci. Technol. 2016, 50, 11879. doi: 10.1021/acs.est.6b03184
23. [23]
  Zhang, L.; Shao, Q.; Xu, C. J. Clean. Prod. 2019, 213, 753. doi: 10.1016/j.jclepro.2018.12.183
24. [24]
  Liu, W.; Sun, W.; Borthwick, A. G. L.; Wang, T.; Li, F.; Guan, Y. J. Hazard. Mater. 2016, 317, 385. doi: 10.1016/j.jhazmat.2016.06.002
25. [25]
  Grosvenor, A. P.; Kobe, B. A.; Biesinger, M. C.; McIntyre, N. S. Surf. Interface Anal. 2004, 36, 1564. doi: 10.1002/sia.1984
26. [26]
  Choi, K.; Lee, W. J. Hazard. Mater. 2012, 211-212, 146. doi: 10.1016/j.jhazmat.2011.10.056
27. [27]
  Luo, F.; Chen, Z.; Megharaj, M.; Naidu, R. Chem. Eng. J. 2016, 294, 290. doi: 10.1016/j.cej.2016.03.005
28. [28]
  Gao, Y. Y.; Li, H. X.; Ou, Z. Z.; Hao, P.; Li, Y.; Yang, G. Q. Acta Phys.-Chim. Sin. 2011, 27, 2469. doi: 10.3866/PKU.WHXB20110939
29. [29]
  Gotic, M.; Music, S. J. Mol. Struct. 2007, 834, 445.
30. [30]
  Dong, H.; He, Q.; Zeng, G.; Tang, L.; Zhang, L.; Xie, Y.; Zeng, Y.; Zhao, F. Chem. Eng. J. 2017, 316, 410. doi: 10.1016/j.cej.2017.01.118
31. [31]
  Cai, X.; Gao, Y.; Sun, Q.; Chen, Z.; Megharaj, M.; Naidu, R. Chem. Eng. J. 2014, 244, 19. doi: 10.1016/j.cej.2014.01.040
32. [32]
  Guan, X.; Sun, Y.; Qin, H.; Li, J.; Lo, I. M.; He, D.; Dong, Water Res. 2015, 75, 224. doi: 10.1016/j.watres.2015.02.034
33. [33]
  Wang, N.; Zheng, T.; Jiang, J.; Wang, P. Chem. Eng. J. 2015, 260, 386. doi: 10.1016/j.cej.2014.09.002
34. [34]
  Zhou, P.; Zhang, J.; Zhang, Y.; Zhang, G.; Li, W.; Wei, C.; Liang, J.; Liu, Y.; Shu, S. J. Hazard. Mater. 2018, 344, 1209. doi: 10.1016/j.jhazmat.2017.11.023
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