Abstract
The increased use of heavy metals in process industries often results in the generation of large quantities of wastewater (WW) and aqueous waste (AW) containing mixtures of heavy metals such as copper and nickel. This research focuses on the electrochemical recovery of copper and nickel from acid pickling solutions used to treat metal surfaces. Using hull cells, beaker plating, and electrolytic cells in pilot scale (capacity 30 L), the most important parameters influencing the process have been identified (temperature, contact time, and current density). In total, about 60 tests were carried out on AW containing nickel and copper. The results of the tests carried out with copper-containing AW shows that removal yields are often higher than 50%; while the energy consumption is less than 15 kWh kg−1 of metal deposited. The best removal efficiency (100%) was achieved by applying a current density of 6 A dm−2 and the energy consumption was 2 kWh kg−1. The tests carried out with AW containing nickel point out very low removal yields (< 20%) and very high energy consumption (even exceeding 300 kWh kg−1). The best removal yield obtained, applying a current density of 3 A dm−2, is 6.7% with an energy consumption of 40 kWh kg−1 of metal removed. A costs analysis based on Metal Exchange value was carried out. The cost analysis suggests that the results, in terms of removal and recovery, obtained for these metals, in particular for copper, are very promising for an industrial application.
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References
Ahmed Basha, C., Bhadrinarayana, N. S., Anantharaman, N., & Meera Sheriffa Begum, K. M. (2008). Heavy metal removal from copper smelting effluent using electrochemical cylindrical flow reactor. Journal of Hazardous Materials, 152(1), 71–78. https://doi.org/10.1016/j.jhazmat.2007.06.069.
APHA. (2012). Standard methods for the examination of water and wastewater. American Public Health Association, American Water Works Association, Water Environment Federation (22nd Editi.). https://www.mwa.co.th/download/file_upload/SMWW_1000-3000.pdf. Accessed 30 October 2018.
ARERA. (2018). Relazione Annuale sullo stato dei servizi e sull’attività svolta - Volume 1| Stato dei Servizi. Milano. https://www.arera.it/allegati/relaz_ann/18/RAvolumeI_2018.pdf.
Awual, M. R. (2015). A novel facial composite adsorbent for enhanced copper (II) detection and removal from wastewater. Chemical Engineering Journal, 266, 368–375. https://doi.org/10.1016/j.cej.2014.12.094.
Balaji, R. (2006). Preparation and characterization of electrodeposits form methane sulphonic acid bath | PhD thesis. Tamil Nadu: Central Electrochemical Research Institute.
Barakat, M. A. (2011). New trends in removing heavy metals from industrial wastewater. Arabian Journal of Chemistry, 4(4), 361–377. https://doi.org/10.1016/j.arabjc.2010.07.019.
Beverskog, B. (1997). Revised Pourbaix diagrams for copper at 25 to 300°C. Journal of the Electrochemical Society, 144(10), 3476. https://doi.org/10.1149/1.1838036.
Beverskog, B., & Puigdomenech, I. (1997). Revised Pourbaix diagrams for nickel at 25–300 °C. Corrosion Science, 39(5), 969–980. https://doi.org/10.1016/S0010-938X(97)00002-4.
Borges Porto, M., Barbosa Alvim, L., & de Almeida Neto, A. F. (2017). Nickel removal from wastewater by induced co-deposition using tungsten to formation of metallic alloys. Journal of Cleaner Production, 142(4), 3293–3299 https://www.sciencedirect.com/science/article/pii/S0959652616317711.
Bourechech, Z., Abdelmalek, F., Ghezzar, M., & Addou, A. (2018). Treatment of leachate from municipal solid waste of Mostaganem district in Algeria: decision support for advising a process treatment. Waste Management & Research, 36(1), 68–78. https://doi.org/10.1177/0734242X17739970.
Britto-Costa, P. H., & Ruotolo, L. A. M. (2015). Copper electrowinning using a spouted-bed electrochemical reactor. Química Nova, 38(5), 657–662. https://doi.org/10.5935/0100-4042.20150068.
Britto-Costa, P. H., Pereira-Filho, E. R., & Ruotolo, L. A. M. (2014). Copper electrowinning using a pulsed bed three-dimensional electrode. Hydrometallurgy, 144–145, 15–22. https://doi.org/10.1016/j.hydromet.2014.01.014.
Brooks, C. S. (2018). Metal recovery from industrial waste. Taylor and Francis Ltd.
Chaudhary, A. J., Grimes, S. M., & Mukhtar-ul-Hassan. (2001). Simultaneous recovery of copper and degradation of 2,4-dichlorophenoxyacetic acid in aqueous systems by a combination of electrolytic and photolytic processes. Chemosphere, 44(5), 1223–1230. doi:https://doi.org/10.1016/S0045-6535(00)00350-7.
Chellammal, S., Raghu, S., Kalaiselvi, P., & Subramanian, G. (2010). Electrolytic recovery of dilute copper from a mixed industrial effluent of high strength COD. Journal of Hazardous Materials, 180(1–3), 91–97. https://doi.org/10.1016/j.jhazmat.2010.03.103.
Collivignarelli, M. C., Abbà, A., Padovani, S., Frascarolo, M., Sciunnach, D., Turconi, M., & Orlando, M. (2015a). Recovery of sewage sludge on agricultural land in Lombardy: current issues and regulatory scenarios. Environmental Engineering and Management Journal, 14(7), 1477–1486. https://doi.org/10.30638/eemj.2015.159.
Collivignarelli, M. C., Bertanza, G., Sordi, M., & Pedrazzani, R. (2015b). High-strength wastewater treatment in a pure oxygen thermophilic process: 11-year operation and monitoring of different plant configurations. Water Science and Technology, 71(4), 588–596. https://doi.org/10.2166/wst.2015.008.
Collivignarelli, M. C., Abbà, A., Bertanza, G., & Barbieri, G. (2017a). Treatment of high strength aqueous wastes in a thermophilic aerobic membrane reactor (TAMR): performance and resilience. Water Science and Technology, 76(12), 3236–3245. https://doi.org/10.2166/wst.2017.492.
Collivignarelli, M. C., Castagnola, F., Sordi, M., & Bertanza, G. (2017b). Sewage sludge treatment in a thermophilic membrane reactor (TMR): factors affecting foam formation. Environmental Science and Pollution Research, 24(3), 2316–2325. https://doi.org/10.1007/s11356-016-7983-4.
Collivignarelli, M. C., Pedrazzani, R., Sorlini, S., Abbà, A., & Bertanza, G. (2017c). H2O2 based oxidation processes for the treatment of real high strength aqueous wastes. Sustainability, 9(2), 244. https://doi.org/10.3390/su9020244.
Collivignarelli, M. C., Abbà, A., Bertanza, G., Setti, M., Barbieri, G., & Frattarola, A. (2018). Integrating novel (thermophilic aerobic membrane reactor-TAMR) and conventional (conventional activated sludge-CAS) biological processes for the treatment of high strength aqueous wastes. Bioresource Technology, 255, 213–219. https://doi.org/10.1016/j.biortech.2018.01.112.
Collivignarelli, M. C., Abbà, A., Carnevale Miino, M., & Damiani, S. (2019). Treatments for color removal from wastewater: state of the art. Journal of Environmental Management, 236, 727–745. https://doi.org/10.1016/j.jenvman.2018.11.094.
Coman, V., Robotin, B., & Ilea, P. (2013). Nickel recovery/removal from industrial wastes: a review. Resources, Conservation and Recycling, 73, 229–238. https://doi.org/10.1016/j.resconrec.2013.01.019.
de Freitas, F., Battirola, L. D., & de Andrade, R. L. T. (2018). Adsorption of Cu2+ and Pb2+ Ions by Pontederia rotundifolia (L.f.) (Pontederiaceae) and Salvinia biloba Raddi (Salviniaceae) Biomass. Water, Air, & Soil Pollution, 229(11), 349. https://doi.org/10.1007/s11270-018-4005-9.
Dermentzis, K., Marmanis, D., Christoforidis, A., Kokkinos, N., & Stergiopoulos, D. K. (2016). Recovery of metallic nickel from waste sludge produced by electrocoagulation of nickel bearing electroplating effluents. In 4th international conference on sustainable solid waste management (pp. 23–25).
EC. (2010). Environmental, economic and social impacts of the use of sewage sludge on land | part II: report on options and impacts. http://ec.europa.eu/environment/archives/waste/sludge/pdf/part_ii_report.pdf
EC. (2018). Circular economy: implementation of the circular economy action plan. European Commission. http://ec.europa.eu/environment/circular-economy/index_en.htm. Accessed 31 October 2018.
ECB. (2018). Euro reference exchange rate: US dollar (USD). European Central Bank. https://www.ecb.europa.eu/stats/policy_and_exchange_rates/euro_reference_exchange_rates/html/eurofxref-graph-usd.en.html. Accessed 23 October 2018.
Erdoğan, M., Karakaya, E., Aras, M. S., Karagül, S. Ç., Ersoy, M. K., Öztürk, A., & Karakaya, İ. (2018). Removal of trace amounts of copper from concentrated hydrochloric acid solutions. International Journal of Electrochemical Science, 10934–10947. https://doi.org/10.20964/2018.11.75.
Fu, F., & Wang, Q. (2011). Removal of heavy metal ions from wastewaters: a review. Journal of Environmental Management, 92(3), 407–418. https://doi.org/10.1016/j.jenvman.2010.11.011.
Gunatilake, S. K. (2015). Methods of removing heavy metals from industrial wastewater. Journal of Multidisciplinary Engineering Science Studies, 1(1), 12–18 http://www.jmess.org/wp-content/uploads/2015/11/JMESSP13420004.pdf.
Ishak, A. R., Hamid, F. S., Mohamad, S., & Tay, K. S. (2018). Stabilized landfill leachate treatment by coagulation-flocculation coupled with UV-based sulfate radical oxidation process. Waste Management, 76, 575–581. https://doi.org/10.1016/j.wasman.2018.02.047.
Karakaya, E., Aras, M. S., Erdoğan, M., Karagül, S. Ç., Ersoy, M. K., & Karakaya, İ. (2018). An electrochemical procedure for copper removal from regenerated pickling solutions of steel plants (pp. 275–281). doi:https://doi.org/10.1007/978-3-319-72362-4_24.
Lavelaine, H., & Allanore, A. (2009). Optimized design of an iron electrowinning cell. Revue de Métallurgie, 106(10), 460–471. https://doi.org/10.1051/metal/2009079.
Liu, Y., Wu, X., Yuan, D., & Yan, J. (2013). Removal of nickel from aqueous solution using cathodic deposition of nickel hydroxide at a modified electrode. Journal of Chemical Technology & Biotechnology, 88(12), 2193–2200. https://doi.org/10.1002/jctb.4085.
LME. (2018). Copper and nickel prices. London Metal Exchange. https://www.lme.com/. Accessed 23 October 2018.
Lou, W., Cai, W., Li, P., Su, J., Zheng, S., Zhang, Y., & Jin, W. (2018). Additives-assisted electrodeposition of fine spherical copper powder from sulfuric acid solution. Powder Technology, 326, 84–88. https://doi.org/10.1016/j.powtec.2017.12.060.
Luo, H., Qin, B., Liu, G., Zhang, R., Tang, Y., & Hou, Y. (2015). Selective recovery of Cu2+ and Ni2+ from wastewater using bioelectrochemical system. Frontiers of Environmental Science & Engineering, 9(3), 522–527. https://doi.org/10.1007/s11783-014-0633-5.
Maarof, H. I., Daud, W. M. A. W., & Aroua, M. K. (2017). Recent trends in removal and recovery of heavy metals from wastewater by electrochemical technologies. Reviews in Chemical Engineering, 33(4). https://doi.org/10.1515/revce-2016-0021.
Malamis, S., Katsou, E., & Haralambous, K. J. (2011). Study of Ni(II), Cu(II), Pb(II), and Zn(II) removal using sludge and minerals followed by MF/UF. Water, Air, & Soil Pollution, 218(1–4), 81–92. https://doi.org/10.1007/s11270-010-0625-4.
Min, X., Luo, X., Deng, F., Shao, P., Wu, X., & Dionysiou, D. D. (2018). Combination of multi-oxidation process and electrolysis for pretreatment of PCB industry wastewater and recovery of highly-purified copper. Chemical Engineering Journal, 354, 228–236. https://doi.org/10.1016/j.cej.2018.07.212.
Orhan, G., Arslan, C., Bombach, H., & Stelter, M. (2002). Nickel recovery from the rinse waters of plating baths. Hydrometallurgy, 65(1), 1–8. https://doi.org/10.1016/S0304-386X(02)00038-5.
Orhan, G., Gurmen, S., & Timur, S. (2004). The behavior of organic components in copper recovery from electroless plating bath effluents using 3D electrode systems. Journal of Hazardous Materials, 112(3), 261–267. https://doi.org/10.1016/j.jhazmat.2004.05.012.
Peng, C., Jin, R., Li, G., Li, F., & Gu, Q. (2014). Recovery of nickel and water from wastewater with electrochemical combination process. Separation and Purification Technology, 136, 42–49. https://doi.org/10.1016/j.seppur.2014.08.025.
Pletcher, D., & Walsh, F. C. (1993). Industrial electrochemistry. Dordrecht: Springer Netherlands. https://doi.org/10.1007/978-94-011-2154-5.
Renou, S., Givaudan, J. G., Poulain, S., Dirassouyan, F., & Moulin, P. (2008). Landfill leachate treatment: review and opportunity. Journal of Hazardous Materials, 150(3), 468–493. https://doi.org/10.1016/j.jhazmat.2007.09.077.
Rodenas Motos, P., ter Heijne, A., van der Weijden, R., Saakes, M., Buisman, C. J. N., & Sleutels, T. H. J. A. (2015). High rate copper and energy recovery in microbial fuel cells. Frontiers in Microbiology, 6. https://doi.org/10.3389/fmicb.2015.00527.
Rodenas Motos, P., Molina, G., ter Heijne, A., Sleutels, T., Saakes, M., & Buisman, C. (2017). Prototype of a scaled-up microbial fuel cell for copper recovery. Journal of Chemical Technology & Biotechnology, 92(11), 2817–2824. https://doi.org/10.1002/jctb.5353.
Sharma, B., Sarkar, A., Singh, P., & Singh, R. P. (2017). Agricultural utilization of biosolids: a review on potential effects on soil and plant grown. Waste Management, 64, 117–132. https://doi.org/10.1016/j.wasman.2017.03.002.
Sorlini, S., Collivignarelli, M. C., & Canato, M. (2015). Effectiveness in chlorite removal by two activated carbons under different working conditions: a laboratory study. Journal of Water Supply: Research and Technology-AQUA, 64(4), 450–461. https://doi.org/10.2166/aqua.2015.132.
Su, F., & Ye, S. (2017). Zinc and copper recovery from smelter waste stream case study. Geo-Resources Environment and Engineering. https://doi.org/10.15273/gree.2017.02.012.
Tiwari, A. K., Singh, P. K., Singh, A. K., & De Maio, M. (2016). Estimation of heavy metal contamination in groundwater and development of a heavy metal pollution index by using GIS technique. Bulletin of Environmental Contamination and Toxicology, 96(4), 508–515. https://doi.org/10.1007/s00128-016-1750-6.
Wang, H., & Ren, Z. J. (2014). Bioelectrochemical metal recovery from wastewater: a review. Water Research, 66, 219–232. https://doi.org/10.1016/j.watres.2014.08.013.
Wang, C.-T., Chou, W.-L., & Kuo, Y.-M. (2009). Removal of COD from laundry wastewater by electrocoagulation/electroflotation. Journal of Hazardous Materials, 164(1), 81–86. https://doi.org/10.1016/j.jhazmat.2008.07.122.
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The authors are grateful to IdroClean s.r.l. and LabioLab s.r.l. for providing technical assistance.
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The authors are grateful to IdroClean s.r.l. and LabioLab s.r.l. for providing financial support.
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Collivignarelli, M.C., Abbà, A., Bestetti, M. et al. Electrolytic Recovery of Nickel and Copper from Acid Pickling Solutions Used to Treat Metal Surfaces. Water Air Soil Pollut 230, 101 (2019). https://doi.org/10.1007/s11270-019-4158-1
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DOI: https://doi.org/10.1007/s11270-019-4158-1