Citation: Mu Yi, Jia Falong, Ai Zhihui, Zhang Lizhi. Molecular Oxygen Activation with Nano Zero-valent Iron for Aerobic Degradation of Organic Contaminants and the Performance Enhancement[J]. Acta Chimica Sinica, ;2017, 75(6): 538-543. doi: 10.6023/A17020047 shu

Molecular Oxygen Activation with Nano Zero-valent Iron for Aerobic Degradation of Organic Contaminants and the Performance Enhancement

Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Applied & Environmental Chemistry, Central China Normal University, Wuhan 430079

Corresponding author: Ai Zhihui, jennifer.ai@mail.ccnu.edu.cn Zhang Lizhi, zhanglz@mail.ccnu.edu.cn
Received Date: 10 February 2017

Fund Project: the National Key Research and Development Program of China 2016YFA0203000Self-Determined Research Funds of CCNU from the Colleges' Basic Research and Operation of MOE CCNU16A04005National Natural Science Foundation of China 21477044Excellent Doctorial Dissertation Cultivation Grant from Central China Normal University 2016YBZZ031National Natural Science Foundation of China 51472100National Natural Science Foundation of China 21425728National Natural Science Foundation of China 21173093Self-Determined Research Funds of CCNU from the Colleges' Basic Research and Operation of MOE CCNU16A02029National Natural Science Foundation of China 21177048Excellent Doctorial Dissertation Cultivation Grant from Central China Normal University 2015YBZD024

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Nano zero-valent iron (nZVI) is a special kind of iron with large specific surface area, strong reduction activity, and the environmental friendliness. nZVI was usually used to reductively degrade organic pollutants, but its long-term performance was poor and the organic pollutants could not be mineralized. Nano zero-valent iron can reductively activate molecular oxygen to generate reactive oxygen species for oxidation or even mineralization of organic pollutants. Recently, we found the core-shell structure dependent aerobic degradation of organic pollutants by nZVI and proposed a new physical insight into the molecular oxygen activation mechanism of the aerobic nZVI process, where the outward electrons transfer from the iron core initiate the two-electron molecular oxygen activation and surface bound ferrous ions on iron oxide shell favor the single-electron molecular oxygen activation. Several strategies have also been proposed to enhance the production of reactive oxidants by nZVI-induced oxygen activation. We confirmed that addition of extra ferrous ions into the nZVI/O₂ system could generate more surface bound ferrous ions for significantly enhancing the generation of reactive oxygen species. Meanwhile, the introduction of some inorganic or organic ligands in the aerobic nZVI system could also improve the active oxygen species generation efficiency. Finally main typical environmental factors including of the pH value, coexisting ions, natural organic matter on the organic pollutants degradation with the aerobic nZVI were discussed. By the way, we also investigated the anoxic Cr(Ⅵ) removal with nZVI. It was found the Cr(Ⅵ) removal rate constant was mainly attributed to the reduction of Cr(Ⅵ) by the surface bound Fe(Ⅱ) besides the reduction of Cr(Ⅵ) adsorbed on the iron oxide shell via the electrons transferred from the iron core. We also demonstrated that the presence of oxygen molecule can inhibit Cr(Ⅵ) removal with nZVI, which was attributed to that the oxygen molecular activation could compete with Cr(Ⅵ) for the consumption of surface bond Fe(Ⅱ) and donor electrons transferred from Fe⁰ core.
- nano zero-valent iron,
- molecular oxygen activation,
- reactive oxygen species,
- advanced oxidation technology
1. [1]
  Phillips, D. H.; Nooten, T. V.; Bastiaens, L.; Russell, M. I.; Dickson, K.; Plant, S.; Ahad, J. M. E.; Newton, T.; Elliot, T.; Kalin, R. M. Environ. Sci. Technol. 2010, 44, 3861. doi: 10.1021/es902737t
2. [2]
  Yin, W.; Wu, J.; Li, P.; Wang, X.; Zhu, N.; Wu, P.; Yang, B. Chem. Eng. J. 2012, 184, 198. doi: 10.1016/j.cej.2012.01.030
3. [3]
  Mu, Y.; Ai, Z.; Zhang, L.; Song, F. ACS Appl. Mater. Inter. 2015, 7, 1997. doi: 10.1021/am507815t
4. [4]
  Li, X. Q.; Elliott, D. W.; Zhang, W. X. Crit. Rev. Solid State Mater. Sci. 2006, 31, 111. doi: 10.1080/10408430601057611
5. [5]
  Ona-Nguema, G.; Morin, G.; Wang, Y.; Foster, A. L.; Juillot, F.; Calas, G.; Brown, G. E. Environ. Sci. Technol. 2010, 44, 5416. doi: 10.1021/es1000616
6. [6]
  Joo, S. H.; Feitz, A. J.; Waite, T. D. Environ. Sci. Technol. 2004, 38, 2242. doi: 10.1021/es035157g
7. [7]
  Keenan, C. R.; Sedlak, D. L. Environ. Sci. Technol. 2008, 42, 1262. doi: 10.1021/es7025664
8. [8]
  Zečević, S.; Dražić, D. M.; Gojković, S. J. Electroanal. Chem. 1989, 265, 179. doi: 10.1016/0022-0728(89)80188-3
9. [9]
  Fu, F.; Dionysiou, D. D.; Liu, H. J. Hazard. Mater. 2014, 267, 194. doi: 10.1016/j.jhazmat.2013.12.062
10. [10]
  Stumm, W.; Lee, G. F. Ind. Eng. Chem. 1961, 53, 143. doi: 10.1021/ie50614a030
11. [11]
  Lu, L.; Ai, Z.; Li, J.; Zheng, Z.; Li, Q.; Zhang, L. Cryst. Growth Des. 2007, 7, 459. doi: 10.1021/cg060633a
12. [12]
  Ai, Z.; Gao, Z.; Zhang, L.; He, W.; Yin, J. J. Environ. Sci. Technol. 2013, 47, 5344. doi: 10.1021/es4005202
13. [13]
  Keenan, C. R.; Sedlak, D. L. Environ. Sci. Technol. 2008, 42, 6936. doi: 10.1021/es801438f
14. [14]
  Lee, H.; Lee, H. J.; Kim, H. E.; Kweon, J.; Lee, B. D.; Lee, C. J. Hazard. Mater. 2014, 265, 201. doi: 10.1016/j.jhazmat.2013.11.066
15. [15]
  Ai, Z.; Lu, L.; Li, J.; Zhang, L.; Qiu, J.; Wu, M. J. Phys. Chem. C 2007, 111, 7430. doi: 10.1021/jp070412v
16. [16]
  Ai, Z.; Mei, T.; Liu, J.; Li, J.; Jia, F.; Zhang, L.; Qiu, J. J. Phys. Chem. C 2007, 111, 14799. doi: 10.1021/jp073617c
17. [17]
  Liu, W.; Ai, Z.; Cao, M.; Zhang, L. Appl. Catal., B 2014, 150-151, 1. doi: 10.1016/j.apcatb.2013.11.034
18. [18]
  Pecher, K.; Haderlein, S. B.; Schwarzenbach, R. P. Environ. Sci. Technol. 2002, 36, 1734. doi: 10.1021/es011191o
19. [19]
  Amonette, J. E.; Workman, D. J.; Kennedy, D. W.; Fruchter, J. S.; Gorby, Y. A. Environ. Sci. Technol. 2000, 34, 4606. doi: 10.1021/es9913582
20. [20]
  Noradoun, C.; Engelmann, M. D.; McLaughlin, M.; Hutcheson, R.; Breen, K.; Paszczynski, A.; Cheng, I. F. Ind. Eng. Chem. Res. 2003, 42, 5024. doi: 10.1021/ie030076e
21. [21]
  Huang, Q.; Cao, M.; Ai, Z.; Zhang, L. Appl. Catal., B 2015, 162, 326.
22. [22]
  Lee, C.; Keenan, C. R.; Sedlak, D. L. Environ. Sci. Technol. 2008, 42, 4921. doi: 10.1021/es800317j
23. [23]
  Lee, J.; Kim, J.; Choi, W. Environ. Sci. Technol. 2007, 41, 3335. doi: 10.1021/es062430g
24. [24]
  Wang, L.; Cao, M.; Ai, Z.; Zhang, L. Environ. Sci. Technol. 2014, 48, 3354. doi: 10.1021/es404741x
25. [25]
  Kim, H. H.; Lee, H.; Kim, H. E.; Seo, J.; Hong, S. W.; Lee, J. Y.; Lee, C. Water Res. 2015, 86, 66. doi: 10.1016/j.watres.2015.06.016
26. [26]
  Cwiertny, D. M.; Bransfield, S. J.; Roberts, A. L. Environ. Sci. Technol. 2007, 41, 3734. doi: 10.1021/es062993s
27. [27]
  Lee, C.; Sedlak, D. L. Environ. Sci. Technol. 2008, 42, 8528. doi: 10.1021/es801947h
28. [28]
  Ai, Z.; Jia, F.; Zhang, L. Environ. Chem. 2016, 35, 1977.
29. [29]
  King, D. W.; Lounsbury, H. A.; Millero, F. J. Environ. Sci. Technol. 1995, 29, 818. doi: 10.1021/es00003a033
30. [30]
  Liu, T.; Li, X.; Waite, T. D. Environ. Sci. Technol. 2014, 48, 14564. doi: 10.1021/es503777a
31. [31]
  Liu, T.; Li, X.; Waite, T. D. Environ. Sci. Technol. 2013, 47, 7350. doi: 10.1021/es400362w
32. [32]
  Liu, Y.; Phenrat, T.; Lowry, G. V. Environ. Sci. Technol. 2007, 41, 7881. doi: 10.1021/es0711967
33. [33]
  Wittbrodt, P. R.; Palmer, C. D. Environ. Sci. Technol. 1995, 29, 255. doi: 10.1021/es00001a033
34. [34]
  Wang, Z.; Zhang, L.; Zhao, J.; Xing, B. Environ. Sci.-Nano 2016, 3, 240. doi: 10.1039/C5EN00230C
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