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

Figures(6)

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
1. [1]
  Yuanpei ZHANG , Jiahong WANG , Jinming HUANG , Zhi HU . Preparation of magnetic mesoporous carbon loaded nano zero-valent iron for removal of Cr(Ⅲ) organic complexes from high-salt wastewater. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1731-1742. doi: 10.11862/CJIC.20240077
2. [2]
  Endong YANG , Haoze TIAN , Ke ZHANG , Yongbing LOU . Efficient oxygen evolution reaction of CuCo₂O₄/NiFe-layered bimetallic hydroxide core-shell nanoflower sphere arrays. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 930-940. doi: 10.11862/CJIC.20230369
3. [3]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
4. [4]
  Jinfeng Chu , Yicheng Wang , Ji Qi , Yulin Liu , Yan Li , Lan Jin , Lei He , Yufei Song . Comprehensive Chemical Experiment Design: Convenient Preparation and Characterization of an Oxygen-Bridged Trinuclear Iron(III) Complex. University Chemistry, 2024, 39(7): 299-306. doi: 10.3866/PKU.DXHX202310105
5. [5]
  Xin Han , Zhihao Cheng , Jinfeng Zhang , Jie Liu , Cheng Zhong , Wenbin Hu . Design of Amorphous High-Entropy FeCoCrMnBS (Oxy) Hydroxides for Boosting Oxygen Evolution Reaction. Acta Physico-Chimica Sinica, 2025, 41(4): 100033-. doi: 10.3866/PKU.WHXB202404023
6. [6]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
7. [7]
  Pengcheng Yan , Peng Wang , Jing Huang , Zhao Mo , Li Xu , Yun Chen , Yu Zhang , Zhichong Qi , Hui Xu , Henan Li . Engineering Multiple Optimization Strategy on Bismuth Oxyhalide Photoactive Materials for Efficient Photoelectrochemical Applications. Acta Physico-Chimica Sinica, 2025, 41(2): 100014-. doi: 10.3866/PKU.WHXB202309047
8. [8]
  Hao XU , Ruopeng LI , Peixia YANG , Anmin LIU , Jie BAI . Regulation mechanism of halogen axial coordination atoms on the oxygen reduction activity of Fe-N₄ site: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 695-701. doi: 10.11862/CJIC.20240302
9. [9]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 693-700. doi: 10.11862/CJIC.20230402
10. [10]
  Zongfei YANG , Xiaosen ZHAO , Jing LI , Wenchang ZHUANG . Research advances in heteropolyoxoniobates. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 465-480. doi: 10.11862/CJIC.20230306
11. [11]
  Chunmei GUO , Weihan YIN , Jingyi SHI , Jianhang ZHAO , Ying CHEN , Quli FAN . Facile construction and peroxidase-like activity of single-atom platinum nanozyme. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1633-1639. doi: 10.11862/CJIC.20240162
12. [12]
  Weihan Zhang , Menglu Wang , Ankang Jia , Wei Deng , Shuxing Bai . 表面硫物种对钯-硫纳米片加氢性能的影响. Acta Physico-Chimica Sinica, 2024, 40(11): 2309043-. doi: 10.3866/PKU.WHXB202309043
13. [13]
  Wenyan Dan , Weijie Li , Xiaogang Wang . The Technical Analysis of Visual Software ShelXle for Refinement of Small Molecular Crystal Structure. University Chemistry, 2024, 39(3): 63-69. doi: 10.3866/PKU.DXHX202302060
14. [14]
  Cen Zhou , Biqiong Hong , Yiting Chen . Application of Electrochemical Techniques in Supramolecular Chemistry. University Chemistry, 2025, 40(3): 308-317. doi: 10.12461/PKU.DXHX202406086
15. [15]
  Jianjun LI , Mingjie REN , Lili ZHANG , Lingling ZENG , Huiling WANG , Xiangwu MENG . UV-assisted degradation of tetracycline hydrochloride by MnFe₂O₄@activated carbon activated persulfate. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1869-1880. doi: 10.11862/CJIC.20240187
16. [16]
  Yang WANG , Xiaoqin ZHENG , Yang LIU , Kai ZHANG , Jiahui KOU , Linbing SUN . Mn single-atom catalysts based on confined space: Fabrication and the electrocatalytic oxygen evolution reaction performance. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2175-2185. doi: 10.11862/CJIC.20240165
17. [17]
  Qinjin DAI , Shan FAN , Pengyang FAN , Xiaoying ZHENG , Wei DONG , Mengxue WANG , Yong ZHANG . Performance of oxygen vacancy-rich V-doped MnO₂ for high-performance aqueous zinc ion battery. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 453-460. doi: 10.11862/CJIC.20240326
18. [18]
  Yongjie ZHANG , Bintong HUANG , Yueming ZHAI . Research progress of formation mechanism and characterization techniques of protein corona on the surface of nanoparticles. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2318-2334. doi: 10.11862/CJIC.20240247
19. [19]
  Zijuan LI , Xuan LÜ , Jiaojiao CHEN , Haiyang ZHAO , Shuo SUN , Zhiwu ZHANG , Jianlong ZHANG , Yanling MA , Jie LI , Zixian FENG , Jiahui LIU . Synthesis of visual fluorescence emission CdSe nanocrystals based on ligand regulation. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 308-320. doi: 10.11862/CJIC.20240138
20. [20]
  Lu XU , Chengyu ZHANG , Wenjuan JI , Haiying YANG , Yunlong FU . Zinc metal-organic framework with high-density free carboxyl oxygen functionalized pore walls for targeted electrochemical sensing of paracetamol. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 907-918. doi: 10.11862/CJIC.20230431

Get Citation

PDF

XML

Metrics

PDF Downloads(114)
Abstract views(4578)
HTML views(1620)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142