Synthesis of Ferrate(VI) in Two Cathodes and One Anode Cell: Enhanced Efficiency and Treatment of Thiocyanate in Wastewater
Publication: Journal of Environmental Engineering
Volume 144, Issue 10
Abstract
Ferrate(VI) () is a greener oxidant in the treatment of wastewater. This paper presents electrochemical synthesis using two titanium ruthenium sheets as cathodes and a gray cast iron sheet as anode (two cathodes/one anode cell configuration). This electrolytic cell was demonstrated to produce more Fe(VI) than a one cathode/one anode cell configuration ( versus ). In the cell, hydroxide ion concentration (), current density (), distance between cathodes and anode (), and electrolyte NaCl concentration were varied to obtain optimum conditions to generate Fe(VI) efficiently. The optimum NaOH concentration was determined to be in using applied , , , , and . The efficiency of Fe(VI) to remove in petroleum wastewater was tested in the pH range from 7.0 to 12.0. Additions of coagulants, polyaluminum chloride (PAC), and polyacrylamide (PAM) to petroleum wastewater under alkaline conditions eliminated the large particles present in the wastewater. Fe(VI) treatment of particle-free wastewater showed almost complete removal of at pH 7.0–9.0 using . At of the reaction mixture of Fe(VI) and wastewater, incomplete removal of in wastewater was observed.
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Acknowledgments
The authors greatly appreciated the financial support from the Key Projects of Enterprise and University Cooperation in Fujian (Grant No. 2018Y4010), the Program for the Natural Science Foundation of China (Grant No. 51678255), and the National Science and Technology Support Program of China (Grant No. 2015BAL01B01).
References
Alsheyab, M., J. Q. Jiang, and C. Stanford. 2009. “On-line production of ferrate with an electrochemical method and its potential application for wastewater treatment: A review.” J. Environ. Manage. 90 (3): 1350–1356. https://doi.org/10.1016/j.jenvman.2008.10.001.
Alsheyab, M., J. Q. Jiang, and C. Stanford. 2010. “Electrochemical generation of ferrate (VI): Determination of optimum conditions.” Desalination 254 (1–3): 175–178. https://doi.org/10.1016/j.desal.2009.11.035.
Barışçı, S., F. Ulu, H. Särkkä, A. Dimoglo, and M. Sillanpää. 2014. “Electrosynthesis of Ferrate (VI) ion using high purity iron electrodes: Optimization of Influencing parameters on the process and investigating its stability.” Int. J. Electrochem. Sci. 9 (6): 3099–3117.
Barışçı, S., F. Ulu, M. Sillanpää, and A. Dimoglo. 2015. “Evaluation of flurbiprofen removal from aqueous solution by electrosynthesized ferrate(VI) ion and electrocoagulation process.” Chem. Eng. J. 262: 1218–1225. https://doi.org/10.1016/j.cej.2014.10.083.
Chen, Q. Q., H. Chen, Z. Z. Zhang, L. X. Guo, and R. C. Jin. 2017. “Effects of thiocyanate on granule-based anammox process and implications for regulation.” J. Hazard. Mater. 321: 81–91. https://doi.org/10.1016/j.jhazmat.2016.08.044.
Cho, K. B., H. Hirao, S. Shaik, and W. Nam. 2016. “To rebound or dissociate? This is the mechanistic question in C-H hydroxylation by heme and nonheme metal-oxo complexes.” Chem. Soc. Rev. 45 (5): 1197–1210. https://doi.org/10.1039/C5CS00566C.
Cussó, O., M. Cianfanelli, X. Ribas, R. J. M. Klein Gebbink, and M. Costas. 2016. “Iron catalyzed highly enantioselective epoxidation of cyclic aliphatic enones with aqueous .” J. Am. Chem. Soc. 138 (8): 2732–2738. https://doi.org/10.1021/jacs.5b12681.
Ding, L., T. X. Liu, and X. Z. Li. 2014. “Removal of with in-situ generated ferrate(VI) in a wet-scrubbing reactor.” J. Chem. Technol. Biotechnol. 89 (3): 455–461. https://doi.org/10.1002/jctb.4139.
Ding, Z., C. Yang, and Q. Wu. 2004. “The electrochemical generation of ferrate at porous magnetite electrode.” Electrochim. Acta 49 (19): 3155–3159. https://doi.org/10.1016/j.electacta.2004.01.031.
Feng, M., X. Wang, J. Chen, R. Qu, Y. Sui, L. Cizmas, Z. Wang, and V. K. Sharma. 2016. “Degradation of fluoroquinolone antibiotics by ferrate(VI): Effects of water constituents and oxidized products.” Water Res 103: 48–57. https://doi.org/10.1016/j.watres.2016.07.014.
Gonzalez-Merchan, C., T. Genty, B. Bussière, R. Potvin, M. Paquin, M. Benhammadi, and C. M. Neculita. 2016. “Ferrates performance in thiocyanates and ammonia degradation in gold mine effluents.” Miner. Eng 95: 124–130. https://doi.org/10.1016/j.mineng.2016.06.022.
Groves, J. T. 2014. “Enzymatic C-H bond activation: Using push to get pull.” Nat. Chem. 6 (2): 89–91. https://doi.org/10.1038/nchem.1855.
He, W., J. Wang, C. Yang, and J. Zhang. 2006. “The rapid electrochemical preparation of dissolved ferrate(VI): Effects of various operating parameters.” Electrochim. Acta. 51 (10): 1967–1973. https://doi.org/10.1016/j.electacta.2005.03.077.
Jiang, J. Q. 2014. “The role of ferrate(VI) in the remediation of emerging micropollutants: A review” Desalin. Water Treat. 55 (3): 828–835. https://doi.org/10.1080/19443994.2014.932713.
Jiang, W., L. Chen, S. R. Batchu, P. R. Gardinali, L. Jasa, B. Marsalek, R. Zboril, D. D. Dionysiou, K. E. O’shea, and V. K. Sharma. 2014. “Oxidation of microcystin-LR by ferrate(VI): Kinetics, degradation pathways, and toxicity assessment.” Environ. Sci. Technol. 48 (20): 12164–12172. https://doi.org/10.1021/es5030355.
Jiang, Y., J. E. Goodwill, J. E. Tobiason, and D. A. Reckhow. 2016. “Impacts of ferrate oxidation on natural organic matter and disinfection byproduct precursors.” Water Res 96: 114–125. https://doi.org/10.1016/j.watres.2016.03.052.
Kim, C., V. R. Panditi, P. R. Gardinali, R. S. Varma, H. Kim, and V. K. Sharma. 2015. “Ferrate promoted oxidative cleavage of sulfonamides: Kinetics and product formation under acidic conditions.” Chem. Eng. J. 279: 307–316. https://doi.org/10.1016/j.cej.2015.04.139.
Kralchevska, R. P., R. Prucek, J. Kolarík, J. Tucek, L. Machala, J. Filip, V. K. Sharma, and R. Zboril. 2016. “Remarkable efficiency of phosphate removal: Ferrate(VI)-induced in situ sorption on core-shell nanoparticles.” Water Res. 103: 83–91. https://doi.org/10.1016/j.watres.2016.07.021.
Lee, D. G., and H. Gai. 1993. “Kinetics and mechanism of the oxidation of alcohols by ferrate ion.” Can. J. Chem. 71 (9): 1394–1400. https://doi.org/10.1139/v93-180.
Lin, H., N. Oturan, J. Wu, H. Zhang, and M. A. Oturan. 2017. “Cold incineration of sucralose in aqueous solution by electro-Fenton process.” Sep. Purif. Technol. 173: 218–225. https://doi.org/10.1016/j.seppur.2016.09.028.
Luo, Z., M. Strouse, J. Q. Jiang, and V. K. Sharma. 2011. “Methodologies for the analytical determination of ferrate(VI): A Review.” J. Environ. Sci. Health Part A Toxic/Hazard. Subs. Environ. Eng. 46 (5): 453–460. https://doi.org/10.1080/10934529.2011.551723.
Mácová, Z., and K. Bouzek. 2012. “The influence of electrolyte composition on electrochemical ferrate(VI) synthesis. Part III: Anodic dissolution kinetics of a white cast iron anode rich in iron carbide.” J. Appl. Electrochem. 42 (8): 615–626. https://doi.org/10.1007/s10800-012-0438-9.
Mácová, Z., K. Bouzek, J. Hives, V. K. Sharma, R. J. Terryn, and J. C. Baum. 2009. “Research progress in the electrochemical synthesis of ferrate(VI).” Electrochim. Acta. 54 (10): 2673–2683. https://doi.org/10.1016/j.electacta.2008.11.034.
Mills, M. R., A. C. Weitz, M. P. Hendrich, A. D. Ryabov, and T. J. Collins. 2016. “NaClO-generated iron(IV) oxo ad iron(V)oxo TAML in pure water.” J. Am. Chem. Soc. 138 (42): 13866–13869. https://doi.org/10.1021/jacs.6b09572.
Oulego, P., S. Collado, A. Laca, and M. Díaz. 2014. “Simultaneous oxidation of cyanide and thiocyanate at high pressure and temperature.” J. Hazard. Mater. 280: 570–578. https://doi.org/10.1016/j.jhazmat.2014.08.051.
Prucek, R., J. Tucek, J. Kolarik, I. Huskova, J. Filip, R. S. Varma, V. K. Sharma, and R. Zboril. 2015. “Ferrate(VI)-prompted removal of metals in aqueous media: Mechanistic delineation of enhanced efficiency via metal entrenchment in magnetic oxides.” Environ. Sci. Technol. 49 (4): 2319–2327. https://doi.org/10.1021/es5048683.
Ray, K., F. Heims, M. Schwalbe, and W. Nam. 2015. “High-valent metal-oxo intermediates in energy demanding processes: From dioxygen reduction to water splitting.” Curr. Opin. Chem. Biol. 25: 159–171. https://doi.org/10.1016/j.cbpa.2015.01.014.
Sharma, V. K. 2007. “Disinfection performance of Fe(VI) in water and wastewater: A review.” Water Sci. Technol. 55 (1–2): 225–232. https://doi.org/10.2166/wst.2007.019.
Sharma, V. K., C. R. Burnett, D. B. O’Connor, and D. Cabelli. 2002. “Iron(VI) and iron(V) oxidation of thiocyanate.” Environ. Sci. Technol. 36 (19): 4182–4186. https://doi.org/10.1021/es020570u.
Sharma, V. K., L. Chen, and R. Zboril. 2015. “A review on high valent (ferrate): A sustainable green oxidant in organic chemistry and transformation of pharmaceuticals.” ACS Sustainable Chem. Eng. 4 (1): 18–34. https://doi.org/10.1021/acssuschemeng.5b01202.
Sharma, V. K., N. Johnson, L. Cizmas, T. J. McDonald, and H. Kim. 2016. “A review of the influence of treatment strategies on antibiotic resistant bacteria and antibiotic resistance genes.” Chemosphere 150: 702–714. https://doi.org/10.1016/j.chemosphere.2015.12.084.
Sharma, V. K., F. Kazama, Y. H. Jiang, and A. K. Ray. 2005. “Ferrates (iron(VI) and iron(V)): Environmentally friendly oxidants and disinfectants.” J. Water Health. 3 (1): 45–58. https://doi.org/10.2166/wh.2005.0005.
Sharma, V. K., S. Mácová, K. Bouzek, and F. J. Millero. 2010. “Solubility of ferrate(VI) in NaOH-KOH mixtures at different temperatures.” J. Chem. Eng. Data. 55 (12): 5594–5597. https://doi.org/10.1021/je100417d.
Sharma, V. K., R. A. Yngard, D. E. Cabelli, and J. C. Baum. 2008. “Ferrate(VI) and ferrate(V) oxidation of cyanide, thiocyanate, and copper(I) cyanide.” Radiat. Phys. Chem. 77 (6): 761–767. https://doi.org/10.1016/j.radphyschem.2007.11.004.
Sharma, V. K., and R. Zboril. 2015. “Ferryl and ferrate species: Mössbauer spectroscopy investigation.” Croat. Chem. Acta. 88 (4): 363–368. https://doi.org/10.5562/cca2686.
Sharma, V. K., R. Zboril, and R. S. Varma. 2015. “Ferrates: Greener oxidants with multimodal action in water treatment technologies.” Acc. Chem. Res. 48 (2): 182–191. https://doi.org/10.1021/ar5004219.
Sun, X., Q. Zhang, H. Liang, L. Ying, M. X. Xu, and V. K. Sharma. 2016. “Ferrate(VI) as a greener oxidant: Electrochemical generation and treatment of phenol.” J. Hazard. Mater. 319: 130–136. https://doi.org/10.1016/j.jhazmat.2015.12.020.
Xie, Y., H. Dong, G. Zeng, L. Tang, Z. Jiang, C. Zhang, J. Deng, L. Zhang, and Y. Zhang. 2017. “The interactions between nanoscale zero-valent iron and microbes in the subsurface environment: A review.” J. Hazard. Mater. 321 (5): 390–407. https://doi.org/10.1016/j.jhazmat.2016.09.028.
Zhang, W., H. Gao, J. He, P. Yang, D. Wang, T. Ma, H. Xia, and X. Xu. 2017. “Removal of norfloxacin using coupled synthesized nanoscale zero-valent iron (nZVI) with system: Optimization of operating conditions and degradation pathway.” Sep. Purif. Technol. 172: 158–167. https://doi.org/10.1016/j.seppur.2016.08.008.
Zhou, Z., and J. Q. Jiang. 2015. “Treatment of selected pharmaceuticals by ferrate(VI): Performance, kinetic studies and identification of oxidation products.” J. Pharm. Biomed. Anal. 106: 37–45. https://doi.org/10.1016/j.jpba.2014.06.032.
Zou, J. Y., and D. T. Chin. 1988. “Anodic behaviour of carbon steel in concentrated NaOH solutions.” Electrochim. Acta. 33 (4): 477–485. https://doi.org/10.1016/0013-4686(88)80164-6.
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©2018 American Society of Civil Engineers.
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Received: Dec 12, 2017
Accepted: Mar 30, 2018
Published online: Aug 2, 2018
Published in print: Oct 1, 2018
Discussion open until: Jan 2, 2019
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