-NTA-Catalyzed Homogenous Fenton-Like Degradation of Trichloroethylene in Groundwater at Natural pH (): Efficacy, By-Products, and Utilization
Publication: Journal of Environmental Engineering
Volume 148, Issue 1
Abstract
The ferric-nitrilotriacetate ()-catalyzed homogenous Fenton-like reaction (i.e., ) has received increasing interest for environmental applications, but its potential in degrading trichloroethylene (TCE) in groundwater still is not well known. The results of this study showed that was more effective than other processes (e.g., including ethylenediaminetetraacetate, ethylenediamine--disuccinate, citrate, malonate, and tartrate) in degrading TCE in groundwater at natural pH (). The effects of important parameters including the ratio of , and the dosages of and were investigated. Greater than 98% degradation efficiency of TCE in actual groundwater was obtained after 60 min of reaction time under the given conditions of , , , and pH 8.0. Hydroxyl radical () was responsible for the degradation of TCE, and the by-products were identified as formic acid and chloride ion (). Greater than 90% degradation efficiency of TCE in a sand column was achieved under dynamic conditions [ (), , and hydraulic retention time of 4 h], resulting in stoichiometric ratios of and of and 4%, respectively. Compared with iron mineral (e.g., magnetite)-catalyzed Fenton-like processes, led to much smaller consumption of (at least 1 order of magnitude smaller). In addition, the buffering capacity of bicarbonate anions () in groundwater had a positive effect on the degradation of TCE by .
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Data Availability Statement
All data, models, and code generated or used during the study appear in the published article.
Acknowledgments
The authors thank the financial support from the Major Science and Technology Program of Ningbo National Hi-tech Zone (New Materials Science and Technology City) (No. 20181CX050011), the National Natural Science Foundation of China (No. 21507096), and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD) (No. Q410900314).
References
Ahile, U. J., R. A. Wuana, A. U. Itodo, R. Sha’Ato, and R. F. Dantas. 2020. “A review on the use of chelating agents as an alternative to promote photo-Fenton at neutral pH: Current trends, knowledge gap and future studies.” Sci. Total Environ. 710 (25): 134872. https://doi.org/10.1016/j.scitotenv.2019.134872.
Baskaran, D., and R. Rajamanickam. 2019. “Aerobic biodegradation of trichloroethylene by consortium microorganism from turkey litter compost.” J. Environ. Chem. Eng. 7 (4): 103260. https://doi.org/10.1016/j.jece.2019.103260.
Bucheli-Witschel, M., and T. Egli. 2001. “Environmental fate and microbial degradation of aminopolycarboxylic acids.” FEMS Microbiol. Rev. 25 (1): 69–106. https://doi.org/10.1111/j.1574-6976.2001.tb00572.x.
Buxton, G. V., C. L. Greenstock, W. P. Helman, and A. B. Ross. 1988. “Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals ( in aqueous solution.” J. Phys. Chem. Ref. Data 17 (2): 513–886. https://doi.org/10.1063/1.555805.
Che, H., S. Bae, and W. Lee. 2011. “Degradation of trichloroethylene by Fenton reaction in pyrite suspension.” J. Hazard. Mater. 185 (2–3): 1355–1361. https://doi.org/10.1016/j.jhazmat.2010.10.055.
Chen, G., G. E. Hoag, P. Chedda, F. Nadim, B. A. Woody, and G. M. Dobbs. 2001. “The mechanism and applicability of in situ oxidation of trichloroethylene with Fenton’s reagent.” J. Hazard. Mater. 87 (1–3): 171–186. https://doi.org/10.1016/S0304-3894(01)00263-1.
Clément, J.-L., N. Ferré, D. Siri, H. Karoui, A. Rockenbauer, and P. Tordo. 2005. “Assignment of the EPR spectrum of 5,5-dimethyl-1-pyrroline -oxide (DMPO) superoxide spin adduct.” J. Org. Chem. 70 (4): 1198–1203. https://doi.org/10.1021/jo048518z.
Czinnerová, M., O. Vološčuková, K. Marková, A. Ševců, M. Černík, and J. Nosek. 2020. “Combining nanoscale zero-valent iron with electrokinetic treatment for remediation of chlorinated ethenes and promoting biodegradation: A long-term field study.” Water Res. 175 (May): 115692. https://doi.org/10.1016/j.watres.2020.115692.
Dao, Y. H., and J. De Laat. 2011. “Hydroxyl radical involvement in the decomposition of hydrogen peroxide by ferrous and ferric-nitrilotriacetate complexes at neutral pH.” Water Res. 45 (11): 3309–3317. https://doi.org/10.1016/j.watres.2011.03.043.
De Laat, J., Y. H. Dao, N. Hamdi El Najjar, and C. Daou. 2011. “Effect of some parameters on the rate of the catalysed decomposition of hydrogen peroxide by iron(III)-nitrilotriacetate in water.” Water Res. 45 (17): 5654–5664. https://doi.org/10.1016/j.watres.2011.08.028.
De Luca, A., R. F. Dantas, and S. Esplugas. 2014. “Assessment of iron chelates efficiency for photo-Fenton at neutral pH.” Water Res. 61 (Sep): 232–242. https://doi.org/10.1016/j.watres.2014.05.033.
Dong, H., K. Hou, W. Qiao, Y. Cheng, L. Zhang, B. Wang, L. Li, Y. Wang, Q. Ning, and G. Zeng. 2019a. “Insights into enhanced removal of TCE utilizing sulfide-modified nanoscale zero-valent iron activated persulfate.” Chem. Eng. J. 359 (Mar): 1046–1055. https://doi.org/10.1016/j.cej.2018.11.080.
Dong, W., Y. Jin, K. Zhou, S.-P. Sun, Y. Li, and X. D. Chen. 2019b. “Efficient degradation of pharmaceutical micropollutants in water and wastewater by -NTA-catalyzed neutral photo-Fenton process.” Sci. Total Environ. 688 (Oct): 513–520. https://doi.org/10.1016/j.scitotenv.2019.06.315.
Gaza, S., K. R. Schmidt, P. Weigold, M. Heidinger, and A. Tiehm. 2019. “Aerobic metabolic trichloroethene biodegradation under field-relevant conditions.” Water Res. 151 (Mar): 343–348. https://doi.org/10.1016/j.watres.2018.12.022.
Goldstone, J. V., M. J. Pullin, S. Bertilsson, and B. M. Voelker. 2002. “Reactions of hydroxyl radical with humic substances: Bleaching, mineralization, and production of bioavailable carbon substrates.” Environ. Sci. Technol. 36 (3): 364–372. https://doi.org/10.1021/es0109646.
Huang, L., Z. Yang, B. Li, J. Hu, W. Zhang, and W.-C. Ying. 2011. “Granular activated carbon adsorption process for removing trichloroethylene from groundwater.” AIChE J. 57 (2): 542–550. https://doi.org/10.1002/aic.12273.
Huang, W., M. Brigante, F. Wu, C. Mousty, K. Hanna, and G. Mailhot. 2013. “Assessment of the Fe(III)–EDDS complex in Fenton-like processes: From the radical formation to the degradation of bisphenol A.” Environ. Sci. Technol. 47 (4): 1952–1959. https://doi.org/10.1021/es304502y.
Jia, D., S.-P. Sun, Z. Wu, N. Wang, Y. Jin, W. Dong, X. D. Chen, and Q. Ke. 2018. “TCE degradation in groundwater by chelators-assisted Fenton-like reaction of magnetite: Sand columns demonstration.” J. Hazard. Mater. 346 (Mar): 124–132. https://doi.org/10.1016/j.jhazmat.2017.12.031.
Kormann, C., D. W. Bahnemann, and M. R. Hoffmann. 1988. “Photocatalytic production of hydrogen peroxides and organic peroxides in aqueous suspensions of titanium dioxide, zinc oxide, and desert sand.” Environ. Sci. Technol. 22 (7): 798–806. https://doi.org/10.1021/es00172a009.
Lewis, S., A. Lynch, L. Bachas, S. Hampson, L. Ormsbee, and D. Bhattacharyya. 2009. “Chelate-modified Fenton reaction for the degradation of trichloroethylene in aqueous and two-phase systems.” Environ. Eng. Sci. 26 (4): 849–859. https://doi.org/10.1089/ees.2008.0277.
Li, Y., J. Sun, and S.-P. Sun. 2016. “Mn2+-mediated homogeneous Fenton-like reaction of Fe(III)-NTA complex for efficient degradation of organic contaminants under neutral conditions.” J. Hazard. Mater. 313 (Aug): 193–200. https://doi.org/10.1016/j.jhazmat.2016.04.003.
Liang, S., W. Zheng, L. Zhu, W. Duan, C. Wei, and C. Feng. 2019. “One-step treatment of phosphite-laden wastewater: A single electrochemical reactor integrating superoxide radical-induced oxidation and electrocoagulation.” Environ. Sci. Technol. 53 (9): 5328–5336. https://doi.org/10.1021/acs.est.9b00841.
Liang, S. H., K. F. Chen, C. S. Wu, Y. H. Lin, and C. M. Kao. 2014. “Development of -releasing composites for in situ chemical oxidation of TCE-contaminated groundwater.” Water Res. 54 (May): 149–158. https://doi.org/10.1016/j.watres.2014.01.068.
Mejri, A., P. Soriano-Molina, S. Miralles-Cuevas, and J. A. Sánchez Pérez. 2020. “Fe3+-NTA as iron source for solar photo-Fenton at neutral pH in raceway pond reactors.” Sci. Total Environ. 736 (Sep): 139617. https://doi.org/10.1016/j.scitotenv.2020.139617.
Moran, M. J., J. S. Zogorski, and P. J. Squillace. 2007. “Chlorinated solvents in groundwater of the United States.” Environ. Sci. Technol. 41 (1): 74–81. https://doi.org/10.1021/es061553y.
Motekaitis, R. J., and A. E. Martell. 1994. “The iron(III) and iron(II) complexes of nitrilotriacetic acid.” J. Coord. Chem. 31 (1): 67–78. https://doi.org/10.1080/00958979408022546.
Pham, A. L.-T., F. M. Doyle, and D. L. Sedlak. 2012. “Kinetics and efficiency of activation by iron-containing minerals and aquifer materials.” Water Res. 46 (19): 6454–6462. https://doi.org/10.1016/j.watres.2012.09.020.
Pham, H. T., K. Suto, and C. Inoue. 2009. “Trichloroethylene transformation in aerobic pyrite suspension: Pathways and kinetic modeling.” Environ. Sci. Technol. 43 (17): 6744–6749. https://doi.org/10.1021/es900623u.
Ren, T., S. Yang, Y. Jiang, X. Sun, and Y. Zhang. 2018. “Enhancing surface corrosion of zero-valent aluminum (ZVAl) and electron transfer process for the degradation of trichloroethylene with the presence of persulfate.” Chem. Eng. J. 348 (Sep): 350–360. https://doi.org/10.1016/j.cej.2018.04.216.
Ren, T., S. Yang, S. Wu, M. Wang, and Y. Xue. 2019. “High-energy ball milling enhancing the reactivity of microscale zero-valent aluminum toward the activation of persulfate and the degradation of trichloroethylene.” Chem. Eng. J. 374 (9): 100–111. https://doi.org/10.1016/j.cej.2019.05.172.
Richardson, D. E., H. Yao, K. M. Frank, and D. A. Bennett. 2000. “Equilibria, kinetics, and mechanism in the bicarbonate activation of hydrogen peroxide: Oxidation of sulfides by peroxymonocarbonate.” J. Am. Chem. Soc. 122 (8): 1729–1739. https://doi.org/10.1021/ja9927467.
Salvadó, V., X. Ribas, V. Zelano, G. Ostacoli, and M. Valiente. 1989. “The chemistry of iron in biosystems—III. Complex formation between and malonic acid in aqueous solutions.” Polyhedron 8 (6): 813–818. https://doi.org/10.1016/S0277-5387(00)83851-6.
Seibert, D., T. Diel, J. B. Welter, A. L. de Souza, A. N. Módenes, F. R. Espinoza-Quiñones, and F. H. Borba. 2017. “Performance of photo-Fenton process mediated by Fe (III)-carboxylate complexes applied to degradation of landfill leachate.” J. Environ. Chem. Eng. 5 (5): 4462–4470. https://doi.org/10.1016/j.jece.2017.08.043.
Seol, Y., and I. Javandel. 2008. “Citric acid-modified Fenton’s reaction for the oxidation of chlorinated ethylenes in soil solution systems.” Chemosphere 72 (4): 537–542. https://doi.org/10.1016/j.chemosphere.2008.03.052.
Shukla, A. K., S. N. Upadhyay, and S. K. Dubey. 2014. “Current trends in trichloroethylene biodegradation: A review.” Crit. Rev. Biotechnol. 34 (2): 101–114. https://doi.org/10.3109/07388551.2012.727080.
Stroo, H. F., et al. 2012. “Chlorinated ethene source remediation: Lessons learned.” Environ. Sci. Technol. 46 (12): 6438–6447. https://doi.org/10.1021/es204714w.
Su, A.-Q., L. Han, J.-C. Yan, L.-B. Qian, D. Ouyang, and M.-F. Chen. 2018. “Risk assessment of chlorinated solvents in groundwater based on health and water environment.” [In Chinese.] Environ. Eng. 36 (10): 138–143. https://doi.org/10.13205/j.hjgc.201807028.
Sun, S.-P., X. Zeng, and A. T. Lemley. 2013. “Kinetics and mechanism of carbamazepine degradation by a modified Fenton-like reaction with ferric-nitrilotriacetate complexes.” J. Hazard. Mater. 252–253 (3): 155–165. https://doi.org/10.1016/j.jhazmat.2013.02.045.
Teel, A. L., C. R. Warberg, D. A. Atkinson, and R. J. Watts. 2001. “Comparison of mineral and soluble iron Fenton’s catalysts for the treatment of trichloroethylene.” Water Res. 35 (4): 977–984. https://doi.org/10.1016/S0043-1354(00)00332-8.
Walling, C. 1975. “Fenton’s reagent revisited.” Acc. Chem. Res. 8 (4): 125–131. https://doi.org/10.1021/ar50088a003.
Wang, N., D. Jia, Y. Jin, S.-P. Sun, and Q. Ke. 2017. “Enhanced Fenton-like degradation of TCE in sand suspensions with magnetite by NTA/EDTA at circumneutral pH.” Environ. Sci. Pollut. Res. 24 (21): 17598–17605. https://doi.org/10.1007/s11356-017-9387-5.
Watts, R. J., D. D. Finn, L. M. Cutler, J. T. Schmidt, and A. L. Teel. 2007. “Enhanced stability of hydrogen peroxide in the presence of subsurface solids.” J. Contam. Hydrol. 91 (3–4): 312–326. https://doi.org/10.1016/j.jconhyd.2006.11.004.
Watts, R. J., and A. L. Teel. 2019. “Hydroxyl radical and non-hydroxyl radical pathways for trichloroethylene and perchloroethylene degradation in catalyzed propagation systems.” Water Res. 159 (2): 46–54. https://doi.org/10.1016/j.watres.2019.05.001.
Wilkin, R. T., T. R. Lee, M. R. Sexton, S. D. Acree, R. W. Puls, D. W. Blowes, C. Kalinowski, J. M. Tilton, and L. L. Woods. 2019. “Geochemical and isotope study of trichloroethene degradation in a zero-valent iron permeable reactive barrier: A twenty-two-year performance evaluation.” Environ. Sci. Technol. 53 (1): 296–306. https://doi.org/10.1021/acs.est.8b04081.
Xu, X., and N. R. Thomson. 2007. “An evaluation of the green chelant EDDS to enhance the stability of hydrogen peroxide in the presence of aquifer solids.” Thomson Chemosphere 69 (5): 755–762. https://doi.org/10.1016/j.chemosphere.2007.05.008.
Yang, X., J. Cai, X. Wang, Y. Li, Z. Wu, W. D. Wu, X. D. Chen, J. Sun, S.-P. Sun, and Z. Wang. 2020. “A bimetallic Fe–Mn oxide-activated oxone for in situ chemical oxidation (ISCO) of trichloroethylene in groundwater: Efficiency, sustained activity, and mechanism investigation.” Environ. Sci. Technol. 54 (6): 3714–3724. https://doi.org/10.1021/acs.est.0c00151.
Yuan, S., X. Mao, and A. N. Alshawabkeh. 2012. “Efficient degradation of TCE in groundwater using Pd and electro-generated and : A shift in pathway from hydrodechlorination to oxidation in the presence of ferrous ions.” Environ. Sci. Technol. 46 (6): 3398–3405. https://doi.org/10.1021/es204546u.
Zhang, X., X. Gu, S. Lu, Z. Miao, M. Xu, X. Fu, Z. Qiu, and Q. Sui. 2016a. “Application of calcium peroxide activated with Fe(II)-EDDS complex in trichloroethylene degradation.” Chemosphere 160 (Oct): 1–6. https://doi.org/10.1016/j.chemosphere.2016.06.067.
Zhang, Y., N. Klamerth, and M. Gamal El-Din. 2016b. “Degradation of a model naphthenic acid by nitrilotriacetic acid—Modified Fenton process.” Chem. Eng. J. 292 (6): 340–347. https://doi.org/10.1016/j.cej.2016.02.045.
Zhang, Y., N. Klamerth, S. A. Messele, P. Chelme-Ayala, and M. Gamal El-Din. 2016c. “Kinetics study on the degradation of a model naphthenic acid by ethylenediamine-N,N’-disuccinic acid-modified Fenton process.” J. Hazard. Mater. 318 (2): 371–378. https://doi.org/10.1016/j.jhazmat.2016.06.063.
Zhang, Y., Q. Zhang, S. Zuo, M. Zhou, Y. Pan, G. Ren, Y. Li, and Y. Zhang. 2019. “A highly efficient flow-through electro-Fenton system enhanced with nitrilotriacetic acid for phenol removal at neutral pH.” Sci. Total Environ. 697 (9): 134173. https://doi.org/10.1016/j.scitotenv.2019.134173.
Zhang, Y., and M. Zhou. 2019. “A critical review of the application of chelating agents to enable Fenton and Fenton-like reactions at high pH values.” J. Hazard. Mater. 362 (Sep): 436–450. https://doi.org/10.1016/j.jhazmat.2018.09.035.
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Received: Jun 10, 2021
Accepted: Aug 30, 2021
Published online: Oct 21, 2021
Published in print: Jan 1, 2022
Discussion open until: Mar 21, 2022
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