Abstract
In this study, stabilised nano zero-valent iron (nZVI) was used to investigate the simultaneous removal of Cd(II), Cu(II), Pb(II), and Zn(II) from their aqueous solution over a 32-day period. The concentration of each metal used in the solution was 50 mg/L, and the applied nZVI doses were 0.25, 0.50, 1.0, and 2 g/L. The experiments were carried out using multi-metal solutions with initial pH values of 3 and 5. The results of the study showed that the overall metal removal efficiency followed the sequence: Pb > Cu > Zn > Cd. When 2.0 g/L of nZVI was applied to the multi-metal solutions, a high level of Pb(II) removal efficiency was achieved over a 32-day period, i.e. Pb(II) removal from the solutions with an initial pH of 3.0 and 5.0 was in the range 94.6–99.5% and 97.9–99.6%, respectively. Meanwhile, at the same dose of nZVI and both the initial solution pH values, high removal efficiencies of Cu (99.6–99.9%), Zn (62.8–82.2%), and Cd (52.2–67.1%) were achieved only over 2.5 h of contact time, and later substantially decreased. The initial pH of the multi-metal solutions did not have a considerable effect on the removal of metals at the initial contact time (0.5 h). However, the impact of pH on metal removal increased with an increase in contact time. Lower nZVI corrosion and therefore superior long-term treatment efficiency was achieved for solutions with an initial pH of 5 compared to that in solutions with an initial pH of 3.
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The datasets generated during and/or analysed during the current study are available from the corresponding author on reasonable request.
References
Ahmed, M. A., Bishay, S. T., Ahmed, F. M., & El-Dek, S. I. (2017). Effective Pb2+ removal from water using nanozerovalent iron stored 10 months. Applied Nanoscience (switzerland), 7(7), 407–416. https://doi.org/10.1007/s13204-017-0581-z
Baragaño, D., Alonso, J., Gallego, J. R., Lobo, M. C., & Gil-Díaz, M. (2020). Zero valent iron and goethite nanoparticles as new promising remediation techniques for As-polluted soils. Chemosphere, 238, 124624.
Baragaño, D., Forján, R., Fernández, B., Ayala, J., Afif, E., & Gallego, J. L. R. (2020). Application of biochar, compost and ZVI nanoparticles for the remediation of As, Cu, Pb and Zn polluted soil. Environmental Science and Pollution Research. https://doi.org/10.1007/s11356-020-09586-3
Boparai, H. K., Joseph, M., & O’Carroll, D. M. (2011). Kinetics and thermodynamics of cadmium ion removal by adsorption onto nano zerovalent iron particles. Journal of Hazardous Materials, 186(1), 458–465. https://doi.org/10.1016/j.jhazmat.2010.11.029
Calderon, B., & Fullana, A. (2015). Heavy metal release due to aging effect during zero valent iron nanoparticles remediation. Water Research, 83, 1–9. https://doi.org/10.1016/j.watres.2015.06.004
Cheng, Y., Dong, H., & Hao, T. (2021). CaCO3 coated nanoscale zero-valent iron (nZVI) for the removal of chromium(VI) in aqueous solution. Separation and Purification Technology, 257, 117967. https://doi.org/10.1016/j.seppur.2020.117967
Danila, V., Kumpiene, J., Kasiuliene, A., & Vasarevičius, S. (2020). Immobilisation of metal(loid)s in two contaminated soils using micro and nano zerovalent iron particles: Evaluating the long-term stability. Chemosphere. https://doi.org/10.1016/j.chemosphere.2020.126054
Eljamal, O., Khalil, A. M. E., Sugihara, Y., & Matsunaga, N. (2016). Phosphorus Removal from Aqueous Solution by Nanoscale Zero Valent Iron in the Presence of Copper Chloride. https://doi.org/10.1016/j.cej.2016.02.052
Fajardo, C., Costa, G., Nande, M., Martín, C., Martín, M., & Sánchez-Fortún, S. (2019). Heavy metals immobilization capability of two iron-based nanoparticles (nZVI and Fe3O4): Soil and freshwater bioassays to assess ecotoxicological impact. Science of the Total Environment, 656, 421–432. https://doi.org/10.1016/j.scitotenv.2018.11.323
Fang, Z., Chen, J., Qiu, X., Qiu, X., Cheng, W., & Zhu, L. (2011). Effective removal of antibiotic metronidazole from water by nanoscale zero-valent iron particles. Desalination, 268(1–3), 60–67. https://doi.org/10.1016/j.desal.2010.09.051
Fu, Z., & Xi, S. (2020). March). Toxicology Mechanisms and Methods. Taylor and Francis Ltd. https://doi.org/10.1080/15376516.2019.1701594
Gil-Díaz, M., Rodríguez-Alonso, J., Maffiotte, C. A., Baragaño, D., Millán, R., & Lobo, M. C. (2021). Iron nanoparticles are efficient at removing mercury from polluted waters. Journal of Cleaner Production, 315, 128272.
Gil-Díaz, M., Álvarez, M. A., Alonso, J., & Lobo, M. C. (2020). Effectiveness of nanoscale zero-valent iron for the immobilization of Cu and/or Ni in water and soil samples. Scientific Reports, 10(1), 1–10.
Karabelli, D., Çaǧri, Ü., Shahwan, T., Eroǧlu, A. E., Scott, T. B., Hallam, K. R., & Lieberwirth, I. (2008). Batch removal of aqueous Cu2+ ions using nanoparticles of zero-valent iron: A study of the capacity and mechanism of uptake. Industrial and Engineering Chemistry Research. https://doi.org/10.1021/ie800081s
Kharisov, B. I., Dias, H. V. R., & Kharissova, O. V. (2014). Nanotechnology-based remediation of petroleum impurities from water. Journal of Petroleum Science and Engineering, 122, 705–718. https://doi.org/10.1016/j.petrol.2014.09.013
Kim, S. A., Kamala-Kannan, S., Lee, K. J., Park, Y. J., Shea, P. J., Lee, W. H., et al. (2013). Removal of Pb(II) from aqueous solution by a zeolite-nanoscale zero-valent iron composite. Chemical Engineering Journal, 217, 54–60. https://doi.org/10.1016/j.cej.2012.11.097
Li, X. Q., & Zhang, W. X. (2006). Iron nanoparticles: The core-shell structure and unique properties for Ni(II) sequestration. Langmuir. https://doi.org/10.1021/la060057k
Li, S., Wang, W., Liang, F., & Zhang, W. X. (2017). Heavy metal removal using nanoscale zero-valent iron (nZVI): Theory and application. Journal of Hazardous Materials, 322, 163–171.
Lian, J. J., Yang, M., Wang, H. L., Zhong, Y., Chen, B., Huang, W. L., & Peng, P. A. (2021). Enhanced molybdenum(VI) removal using sulfide-modified nanoscale zerovalent iron: Kinetics and influencing factors. Water Science and Technology. https://doi.org/10.2166/wst.2020.570
Liang, L., Li, X., Guo, Y., Lin, Z., Su, X., & Liu, B. (2021). The removal of heavy metal cations by sulfidated nanoscale zero-valent iron (S-nZVI): The reaction mechanisms and the role of sulfur. Journal of Hazardous Materials, 404, 124057. https://doi.org/10.1016/j.jhazmat.2020.124057
Liang, L., Li, X., Lin, Z., Tian, C., & Guo, Y. (2020). The removal of Cd by sulfidated nanoscale zero-valent iron: The structural, chemical bonding evolution and the reaction kinetics. Chemical Engineering Journal, 382, 122933.
Liang, W., Dai, C., Zhou, X., & Zhang, Y. (2014). Application of zero-valent iron nanoparticles for the removal of queous zinc ions under various experimental conditions. PLoS ONE, 9(1), e85686. https://doi.org/10.1371/journal.pone.0085686
Lien, H.-L., Jhuo, Y.-S., & Chen, L.-H. (2007). Effect of heavy metals on dechlorination of carbon tetrachloride by iron nanoparticles. Environmental Engineering Science, 24(1), 21–30. https://doi.org/10.1089/ees.2007.24.21
Liu, A., Liu, J., & Zhang, W. (2015). Transformation and composition evolution of nanoscale zero valent iron (nZVI) synthesized by borohydride reduction in static water. Chemosphere, 119, 1068–1074. https://doi.org/10.1016/j.chemosphere.2014.09.026
Lv, D., Zhou, J., Cao, Z., Xu, J., Liu, Y., Li, Y., et al. (2019). Mechanism and influence factors of chromium(VI) removal by sulfide-modified nanoscale zerovalent iron. Chemosphere, 224, 306–315. https://doi.org/10.1016/j.chemosphere.2019.02.109
Lv, D., Zhou, X., Zhou, J., Liu, Y., Li, Y., Yang, K., et al. (2018). Design and characterization of sulfide-modified nanoscale zerovalent iron for cadmium(II) removal from aqueous solutions. Applied Surface Science, 442, 114–123. https://doi.org/10.1016/j.apsusc.2018.02.085
Makaras, T., Razumienė, J., Gurevičienė, V., Šakinytė, I., Stankevičiūtė, M., & Kazlauskienė, N. (2020). A new approach of stress evaluation in fish using β-D-Glucose measurement in fish holding-water. Ecological Indicators, 109, 105829. https://doi.org/10.1016/j.ecolind.2019.105829
Mondino, F., Piscitello, A., Bianco, C., Gallo, A., de Folly D’Auris, A., Tosco, T., et al. (2020). Injection of zerovalent iron gels for aquifer nanoremediation: Lab experiments and modeling. Water, 12(3), 826. https://doi.org/10.3390/w12030826
O’Carroll, D., Sleep, B., Krol, M., Boparai, H., & Kocur, C. (2013). Nanoscale zero valent iron and bimetallic particles for contaminated site remediation. Advances in Water Resources, 51, 104–122. https://doi.org/10.1016/j.advwatres.2012.02.005
Song, S., Su, Y., Adeleye, A. S., Zhang, Y., & Zhou, X. (2017). Optimal design and characterization of sulfide-modified nanoscale zerovalent iron for diclofenac removal. Applied Catalysis b: Environmental, 201, 211–220. https://doi.org/10.1016/j.apcatb.2016.07.055
Suzuki, T., Moribe, M., Oyama, Y., & Niinae, M. (2012). Mechanism of nitrate reduction by zero-valent iron: Equilibrium and kinetics studies. Chemical Engineering Journal, 183, 271–277. https://doi.org/10.1016/j.cej.2011.12.074
Tiberg, C., Sjöstedt, C., Persson, I., & Gustafsson, J. P. (2013). Phosphate effects on copper(II) and lead(II) sorption to ferrihydrite. Geochimica Et Cosmochimica Acta, 120, 140–157. https://doi.org/10.1016/j.gca.2013.06.012
Üzüm, Ç., Shahwan, T., Eroǧlu, A. E., Hallam, K. R., Scott, T. B., & Lieberwirth, I. (2009). Synthesis and characterization of kaolinite-supported zero-valent iron nanoparticles and their application for the removal of aqueous Cu2+ and Co2+ ions. Applied Clay Science. https://doi.org/10.1016/j.clay.2008.07.030
Vasarevičius, S., Danila, V., & Januševičius, T. (2020). Immobilisation of cadmium, copper, lead, and nickel in soil using nano zerovalent iron particles: Ageing effect on heavy metal retention. Water, Air, & Soil Pollution, 231(10), 496. https://doi.org/10.1007/s11270-020-04864-9
Vasarevičius, S., Danila, V., & Paliulis, D. (2019). Application of stabilized nano zero valent iron particles for immobilization of available Cd2+, Cu2+, Ni2+, and Pb2+ ions in soil. International Journal of Environmental Research. https://doi.org/10.1007/s41742-019-00187-8
Vítková, M., Rákosová, S., Michálková, Z., & Komárek, M. (2017). Metal(loid)s behaviour in soils amended with nano zero-valent iron as a function of pH and time. Journal of Environmental Management. https://doi.org/10.1016/j.jenvman.2016.06.003
Wang, Y., Liu, Y., Su, G., Yang, K., & Lin, D. (2021). Transformation and implication of nanoparticulate zero valent iron in soils. Journal of Hazardous Materials, 412, 125207. https://doi.org/10.1016/j.jhazmat.2021.125207
Wu, Y., Yue, Q., Gao, Y., Ren, Z., & Gao, B. (2018). Performance of bimetallic nanoscale zero-valent iron particles for removal of oxytetracycline. Journal of Environmental Sciences (china), 69, 173–182. https://doi.org/10.1016/j.jes.2017.10.006
Yan, W., Herzing, A. A., Kiely, C. J., & Zhang, W. X. (2010). Nanoscale zero-valent iron (nZVI): Aspects of the core-shell structure and reactions with inorganic species in water. Journal of Contaminant Hydrology, 118(3–4), 96–104. https://doi.org/10.1016/j.jconhyd.2010.09.003
Zhang, J., Zhu, Q., & Xing, Z. (2020). Preparation of new materials by ethylene glycol modification and Al(OH)3 coating NZVI to remove sulfides in water. Journal of Hazardous Materials, 390, 122049. https://doi.org/10.1016/j.jhazmat.2020.122049
Zhang, Y., Su, Y., Zhou, X., Dai, C., & Keller, A. A. (2013). A new insight on the core-shell structure of zerovalent iron nanoparticles and its application for Pb(II) sequestration. Journal of Hazardous Materials. https://doi.org/10.1016/j.jhazmat.2013.10.031
Zou, Y., Wang, X., Khan, A., Wang, P., Liu, Y., Alsaedi, A., et al. (2016). Environmental remediation and application of nanoscale zero-valent iron and its composites for the removal of heavy metal ions: A review. Environmental Science & Technology, 50(14), 7290–7304. https://doi.org/10.1021/acs.est.6b01897
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Danila, V., Šerevičienė, V. Simultaneous Removal of Cd(II), Cu(II), Pb(II), and Zn(II) from Aqueous Solution Using Nano Zero-valent Iron: Effect of Contact Time, Fe(0) Loading, and pH. Water Air Soil Pollut 232, 453 (2021). https://doi.org/10.1007/s11270-021-05415-6
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DOI: https://doi.org/10.1007/s11270-021-05415-6