Abstract
Chlorinated ethene contaminations are a widespread environmental hazard and a threat to drinking water supplies. Electrochemical methods for in situ degradation of the chlorinated ethenes in the plume are under development. In laboratory, complete electrochemical removal of chlorinated ethenes in undivided flow-through reactors is reported when using palladized iron (Fe) cathodes (C) and cast Fe anodes (A). The cost of the electrodes depends on the Fe purity. In this study, 99.95%, 99.8% and 98+% palladized Fe cathodes, and 99.8% Fe and cast Fe anodes were investigated. The surfaces of the palladized Fe electrodes were examined by scanning electron microscopy. Deposition of palladium by electroless plating onto the Fe surfaces was uneven and disconnected. The less pure the Fe material, the higher the degree of oxide coverage of the cathode’s surface during electroless plating. Electrochemical application via Fe electrodes installed in a flow-through reactor of field-extracted groundwater and sandy sediment was studied for three-electrode configurations of A–A–C and C–C–A. The anodes of 99.8% Fe and cast Fe demonstrated different corrosion patterns; uniform corrosion and graphitization, respectively. Corrosion products clogged the sandy matrix. The corrosion product compositions differed between the A–A–C and C–C–A electrode configurations. The groundwater pH of 7.35 ± 0.05 changed downgradient to the electrochemical zone to 9.5 and 6.2 for the A–A–C and C–C–A reactors, respectively. The response of the hydrogeochemical settings to the established redox zones showed that the C–C–A electrode configuration was less intrusive to the surrounding environment.
Similar content being viewed by others
References
Bass, D. H., et al. (2000). Performance of air sparging systems: a review of case studies. Journal of Hazardous Materials, 72(2–3), 101–119. https://doi.org/10.1016/S0304-3894(99)00136-3.
Brewster, J. H. (1954). Mechanisms of reductions at metal surfaces. I. A general working hypothesis. Journal of the American Chemical Society, 76(24), 6361–6363. https://doi.org/10.1021/ja01653a034.
Carter, K. E., & Farrell, J. (2009). Electrochemical oxidation of trichloroethylene using boron-doped diamond film electrodes. Environmental Science and Technology, 43(21), 8350–8354. https://doi.org/10.1021/es9017738.
Chakhmouradian, A. R., et al. (2016). Calcite and dolomite in intrusive carbonatites. II. Trace-element variations. Mineralogy and Petrology, 110(2–3), 361–377. https://doi.org/10.1007/s00710-015-0392-4.
Cheng, I. F. (1997). Electrochemical dechlorination of 4-chlorophenol to phenol. Environmental Science and Technology, 31(4), 1074–1078. https://doi.org/10.1021/es960602b.
Fallahpour, N., et al. (2016). Hydrodechlorination of TCE in a circulated electrolytic column at high flow rate. Chemosphere, 144, 59–64. https://doi.org/10.1016/j.chemosphere.2015.08.037.
Fallahpour, N., et al. (2017). Electrochemical dechlorination of trichloroethylene in the presence of natural organic matter, metal ions and nitrates in a simulated karst media. Journal of Environmental Chemical Engineering, 5(1), 240–245. https://doi.org/10.1016/j.jece.2016.11.046.
Gilbert, D., et al. (2010). In situ remediation of chlorinated solvent plumes, in situ remediation of chlorinated solvent plumes. In H. F. Stroo & C. H. Ward (Eds.), SERDP/ESTCP environmental remediation technology. New York: Springer New York. https://doi.org/10.1007/978-1-4419-1401-9.
He, Y. T., et al. (2015). Review of abiotic degradation of chlorinated solvents by reactive iron minerals in aquifers. Groundwater Monitoring and Remediation, 35(3), 57–75. https://doi.org/10.1111/gwmr.12111.
Heystek, H., & Haul, R. A. W. (1951). Differential thermal analysis of the dolomite decomposition. American Mineralogist, 37(3), 165–178.
Hyldegaard, B. H., et al. (2019). Challenges in electrochemical remediation of chlorinated solvents in natural groundwater aquifer settings. Journal of Hazardous Materials, 368, 680–688. https://doi.org/10.1016/j.jhazmat.2018.12.064.
Interstate Technology & Regulatory Council. (2005). Permeable reactive barriers: lessons learned/new directions. Washington: PRB-4, Interstate Technology & Regulatory Council, Permeable Reactive Barrier Team.
Interstate Technology & Regulatory Council. (2011). Integrated DNAPL site strategy. Washington: Available at: http://www.itrcweb.org. Accesssed 15 May 2019.
Järvinen, L., et al. (2014). Core level studies of calcite and dolomite. Surface and Interface Analysis, 46(6), 399–406. https://doi.org/10.1002/sia.5511.
Jovanovic, G. N., et al. (2005). Dechlorination of P-chlorophenol in a microreactor with bimetallic Pd/Fe catalyst. Industrial and Engineering Chemistry Research, 44(14), 5099–5106. https://doi.org/10.1021/ie049496+.
Kemp, S. J. et al. (2010) Low level detection and quantification of carbonate species using thermogravimetric and differential thermal analysis. Report IR/09/074. Keyworth, UK.
Kueper, B. H., et al. (2003). An illustrated handbook of DNAPL transport and fate in the subsurface—environment agency R&D publication 133. Bristol: Environment Agency Available at: http://www.environment-agency.gov.uk. Accessed 15 May 2019.
Kueper, B. H., et al. (2014). Chlorinated solvent source zone remediation. New York: Springer. https://doi.org/10.1007/978-1-4614-6922-3.
Mackay, D. M., & Cherry, J. A. (1989). Groundwater contamination: pump-and-treat remediation. Environmental Science and Technology, 23(6), 630–636. https://doi.org/10.1021/es00064a001.
Mao, X., et al. (2011). Redox control for electrochemical dechlorination of trichloroethylene in bicarbonate aqueous media. Environmental Science and Technology, 45(15), 6517–6523. https://doi.org/10.1021/es200943z.
Mao, X., et al. (2012). Electrochemically induced dual reactive barriers for transformation of TCE and mixture of contaminants in groundwater. Environmental Science and Technology, 46(21), 12003–12011. https://doi.org/10.1021/es301711a.
Mao, X., et al. (2015). Iron electrocoagulation with enhanced cathodic reduction for the removal of aqueous contaminant mixtures. Environmental Engineering and Management Journal, 14(12), 2905–2911.
Marselli, B., et al. (2003). Electrogeneration of hydroxyl radicals on boron-doped diamond electrodes. Journal of the Electrochemical Society, 150(3), 79–83. https://doi.org/10.1149/1.1553790.
Mattsson, E. (2001). Types of corrosion. In E. Mattsson (Ed.), Basic corrosion technology for scientists and engineers (2nd ed., pp. 37–63). Wandsworth: The Chameleon Press, Ltd..
Pamukcu, S., et al. (2014). Reduction of contaminants in soil and water by direct electric current. In G. V. Chilingar & M. Haroun (Eds.), Electrokinetics for petroleum and environmental engineers (pp. 33–101). Wiley.
Pankow, J. F., et al. (1996). In J. Pankow (Ed.), Dense chlorinated solvents and other DNAPLs in groundwater: history, behavior, and remediation. Portland: Waterloo Press.
Parker, B. L., et al. (2003). Review and analysis of chlorinated solvent dense nonaqueous phase liquid distributions in five sandy aquifers. Vadose Zone Journal, 2(2), 116–137. https://doi.org/10.2136/vzj2003.1160.
Parkinson, G. S. (2016). Iron oxide surfaces. Surface Science Reports, 71(1), 272–365. https://doi.org/10.1016/j.surfrep.2016.02.001.
Rajic, L., et al. (2014). Electrochemical transformation of trichloroethylene in aqueous solution by electrode polarity reversal. Water Research. Elsevier Ltd, 67, 267–275. https://doi.org/10.1016/j.watres.2014.09.017.
Rajic, L., et al. (2015a). Electrochemical transformation of thichloroethylene in groundwater by Ni-containing cathodes. Electrochimica Acta, 181, 118–122. https://doi.org/10.1016/j.electacta.2015.03.112.
Rajic, L., et al. (2015b). Influence of humic substances on electrochemical degradation of trichloroethylene in limestone aquifers. Electrochimica Acta, 181, 123–129. https://doi.org/10.1016/j.electacta.2015.03.121.
Rajic, L., et al. (2015c). Impact of electrode sequence on electrochemical removal of trichloroethylene from aqueous solution. Applied Catalysis B: Environmental, 174–175, 427–434. https://doi.org/10.1016/j.apcatb.2015.03.018.
Rajic, L., et al. (2016a). Electrochemical degradation of trichloroethylene in aqueous solution by bipolar graphite electrodes. Journal of Environmental Chemical Engineering, 4(1), 197–202. https://doi.org/10.1016/j.jece.2015.10.030.
Rajic, L., et al. (2016b). The influence of cathode material on electrochemical degradation of trichloroethylene in aqueous solution. Chemosphere, 147, 98–104. https://doi.org/10.1016/j.chemosphere.2015.12.095.
Rudén, C. (2006). Science and policy in risk assessments of chlorinated ethenes. Annals of the New York Academy of Sciences, 1076, 191–206. https://doi.org/10.1196/annals.1371.046.
Ruder, A. M. (2006). Potential health effects of occupational chlorinated solvent exposure. Annals of the New York Academy of Sciences, 1076, 207–227. https://doi.org/10.1196/annals.1371.050.
Sáez, V., et al. (2010). Electrochemical degradation of perchloroethylene in aqueous media: influence of the electrochemical operational variables in the viability of the process. Industrial and Engineering Chemistry Research, 49(9), 4123–4131. https://doi.org/10.1021/ie100134t.
Sarin, P., et al. (2004). Iron release from corroded iron pipes in drinking water distribution systems: effect of dissolved oxygen. Water Research, 38(5), 1259–1269. https://doi.org/10.1016/j.watres.2003.11.022.
Scheutz, C., et al. (2010). Field evaluation of biological enhanced reductive dechlorination of chloroethenes in clayey till. Environmental Science and Technology, 44(13), 5134–5141. https://doi.org/10.1021/es1003044.
Siegrist, R. L., et al. (2012). Advances in groundwater remediation: achieving effective in situ delivery of chemical oxidants and amendments. In F. F. Quercia & D. Vidojevic (Eds.), Clean soil and safe water (pp. 197–212). Dordrecht: Springer. https://doi.org/10.1007/978-94-007-2240-8_22.
Stenzel, M. H., & Gupta, U. S. (1985). Treatment of contaminated groundwaters with granular activated carbon and air stripping. Journal of the Air Pollution Control Association, 35(12), 1304–1309. https://doi.org/10.1080/00022470.1985.10466035.
Stroo, H. F., et al. (2012). Chlorinated ethene source remediation: lessons learned. Environmental Science and Technology, 46(12), 6438–6447. https://doi.org/10.1021/es204714w.
Urano, K., et al. (1991). Adsorption of chlorinated organic compounds on activated carbon from water. Water Research, 25(12), 1459–1464. https://doi.org/10.1016/j.arabjc.2015.04.013.
Valverde, J. M., et al. (2015). Thermal decomposition of dolomite under CO2: insights from TGA and in situ XRD analysis. Physical Chemistry Chemical Physics, 17(44), 30162–30176. https://doi.org/10.1039/c5cp05596b.
WHO (2019) World Health Organization (WHO), international programme on chemical safety—environmental health criteria. Available at: https://www.who.int/ipcs/publications/ehc/en/ (Accessed: 22 June 2019).
Yuan, S., et al. (2013). A three-electrode column for Pd-catalytic oxidation of TCE in groundwater with automatic pH-regulation and resistance to reduced sulfur compound foiling. Water Research, 47(1), 269–278. https://doi.org/10.1016/j.watres.2012.10.009.
Zhou, W., et al. (2019). Efficient H2O2 electrogeneration at graphite felt modified via electrode polarity reversal: utilization for organic pollutants degradation. Chemical Engineering Journal, 364, 428–439. https://doi.org/10.1016/j.cej.2019.01.175.
Funding
This work was funded by the Innovation Fund Denmark (grant number 5016-00165B), COWIfonden (grant number C-131.01), the Capital Region of Denmark (grant number 14002102), COWI A/S, and the Technical University of Denmark. A special thanks to Dr. David Gent, US Army Corps of Engineers, Engineer Research and Development Centers Environmental Laboratory, for access to the acrylic column for customization to comply with the lab work requirements of this study. The sandy sediment was kindly donated by Nymølle Stenindustrier A/S, Denmark. The cast iron was kindly donated by Velamp A/S.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of Interest
The authors declare that they have no conflict of interest.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Hyldegaard, B.H., Ottosen, L.M. Selecting Electrode Materials and Sequence for Electrochemical Removal of Chlorinated Ethenes in Groundwater. Water Air Soil Pollut 231, 290 (2020). https://doi.org/10.1007/s11270-020-04641-8
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s11270-020-04641-8