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In Situ Chemical Oxidation of Contaminated Groundwater by Persulfate: Decomposition by Fe(III)- and Mn(IV)-Containing Oxides and Aquifer Materials
Open accessAbstract
Persulfate (S2O8(2-)) is being used increasingly for in situ chemical oxidation (ISCO) of organic contaminants in groundwater, despite an incomplete understanding of the mechanism through which it is converted into reactive species. In particular, the decomposition of persulfate by naturally occurring mineral surfaces has not been studied in detail. To gain insight into the reaction rates and mechanism of persulfate decomposition in the subsurface, and to identify possible approaches for improving its efficacy, the decomposition of persulfate was investigated in the presence of pure metal oxides, clays, and representative aquifer solids collected from field sites in the presence and absence of benzene. Under conditions typical of groundwater, Fe(III)- and Mn(IV)-oxides catalytically converted persulfate into sulfate radical (SO4(•-)) and hydroxyl radical (HO(•)) over time scales of several weeks at rates that were 2-20 times faster than those observed in metal-free systems. Amorphous ferrihydrite was the most reactive iron mineral with respect to persulfate decomposition, with reaction rates proportional to solid mass and surface area. As a result of radical chain reactions, the rate of persulfate decomposition increased by as much as 100 times when benzene concentrations exceeded 0.1 mM. Due to its relatively slow rate of decomposition in the subsurface, it can be advantageous to inject persulfate into groundwater, allowing it to migrate to zones of low hydraulic conductivity where clays, metal oxides, and contaminants will accelerate its conversion into reactive oxidants.
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Cites
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Fang, G., Liu, C., Gao, J., Dionysiou, D. D., & Zhou, D. (2015) · Environmental Science & Technology · doi:10.1021/es5061512 · Cited by 887
Zhou, Z., Liu, X., Sun, K., Lin, C., Ma, J., He, M., & Ouyang, W. (2019) · Chemical Engineering Journal · doi:10.1016/j.cej.2019.04.213 · Cited by 677
Ushani, U., Lu, X., Wang, J., Zhang, Z., Dai, J., Tan, Y., Wang, S., Li, W., Niu, C., Cai, T., et al. (2020) · Chemical Engineering Journal · doi:10.1016/j.cej.2020.126232 · Cited by 451
Kinetics and Mechanism of Ultrasonic Activation of Persulfate: An in Situ EPR Spin Trapping Study
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Bicarbonate-activated persulfate oxidation of acetaminophen
Jiang, M., Lu, J., Ji, Y., & Kong, D. (2017) · Water Research · doi:10.1016/j.watres.2017.03.043 · Cited by 259
Limitations and Prospects of Sulfate-Radical Based Advanced Oxidation Processes
Duan, X., Yang, S., Wacławek, S., Fang, G., Xiao, R., & Dionysiou, D. D. (2020) · Journal of Environmental Chemical Engineering · doi:10.1016/j.jece.2020.103849 · Cited by 206
Bruton, T. A., & Sedlak, D. L. (2017) · Environmental Science & Technology · doi:10.1021/acs.est.7b03969 · Cited by 183
Self-citationLi, W., Jain, T., Ishida, K., & Liu, H. (2017) · Environmental Science: Water Research & Technology · doi:10.1039/c6ew00242k · Cited by 151
Self-citationElectro-Persulfate Processes for the Treatment of Complex Wastewater Matrices: Present and Future
Fernandes, A., Nunes, M. J., Rodrigues, A. S., Pacheco, M. J., Ciríaco, L., & Lopes, A. (2021) · Molecules · doi:10.3390/molecules26164821 · Cited by 67
Metheniti, M. E., Frontistis, Z., Ribeiro, R. S., Silva, A. M. T., Faria, J. L., Gomes, H. T., & Mantzavinos, D. (2018) · Environmental Science and Pollution Research · doi:10.1007/s11356-017-0178-9 · Cited by 45
Metadata
- Authors
- Liu, H., Bruton, T. A., Doyle, F. M., & Sedlak, D. L.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-08-18
- Volume
- 48
- Issue
- 17
- Pages
- 10330-10336
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W2072187875
- Cited by
- 430
- References
- 2
- FWCI
- 20.07
- Type
- journal article
- Language
- en
- Open access
- hybrid
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