Field Application of Iron and Iron–Nickel Nanoparticles for the Ex Situ Remediation of a Uranium-Bearing Mine Water Effluent
Publication: Journal of Environmental Engineering
Volume 141, Issue 8
Abstract
In this work, sodium borohydride reduced nanoscale zero-valent iron (nZVI–BR), sodium borohydride reduced nanoscale zero-valent iron–nickel (nZVIN–BR), nanoscale zero-valent iron sourced from NanoIron, s.r.o. (nZVI–Star), and nanoscale zero-valent iron sourced from Toda Kogyo Corporation (nZVI–RNIP) have been tested for the ex situ removal of aqueous uranium (U) from a bicarbonate-rich mine water effluent. Laboratory scale (2 L) batch treatment systems containing the mine water and comparator uranyl solutions were tested to compare U removal efficacy and aqueous corrosion behavior of the different nanopowders. The two commercially sourced nanopowders were also tested for the removal of U from 2,500 L batch systems to determine the nature of any differential behavior exhibited by the nanopowders when deployed at commercial scale. Analysis of aqueous samples taken at periodic intervals throughout the 96 h reaction period using inductively coupled plasma mass spectroscopy recorded aqueous U removal within 15 min by the sodium borohydride reduced nanopowders in all systems studied. Similar behavior was exhibited by the commercially sourced nanopowders for the uranyl-only solutions; however, a maximum of only 30.0 and 43.2% removal was recorded for the 2 L mine water effluent by nZVI–Star and nZVI–RNIP, respectively. Similar U uptake behavior was exhibited by the commercially sourced nanopowders for the 2,500 L batch treatment systems; however, a redox and U removal gradient as a function of depth was recorded, compared to a homogenous distribution recorded for the 2 L experiments. Analysis of reacted nanoparticulate solids using X-ray diffraction determined only minor aqueous corrosion of the two commercial nanopowders whereas near-total conversion to iron (hydr)oxides was recorded for the sodium borohydride reduced nanopowders. Results therefore demonstrate that in order for effective U removal from waters containing appreciable concentrations of complexing agents, highly reactive forms of iron and iron–nickel nanoparticles are required. In addition, the performance of such materials in commercial scale applications is likely to be lower than in laboratory-scale experiments due to the significant technical challenge of homogenous mixing/dispersion of the nanopowder with the aqueous phase.
Get full access to this article
View all available purchase options and get full access to this article.
Acknowledgments
The National Company Uranium (Romania) is thanked for providing access to the Ciudanovita site for the experiments. Dragos Curelea and all other scientists from the National Institute for Metals and Radioactive Resources, Bucharest, Romania, are also thanked for help with arranging and conducting the fieldwork. Finally, Dr. David Morgan of the Cardiff Catalysis Institute, School of Chemistry, Cardiff University is thanked for performing the XPS analysis. The research reported in this paper was funded by the Engineering and Physical Sciences Research Council and North Atlantic Treaty Organization (NATO) through the Cooperative Science and Technology Subprogram (CLG982551).
References
Caré, S., Crane, R. A., Calabro, P. S., Ghauch, A., Temgoua, E., and Noubactep, C. (2012). “Modelling the permeability loss of metallic iron water filtration systems.” Clean Soil Air Water, 41(3), 275–282.
Crane, R. A., Dickinson, M., Popescu, I. C., and Scott, T. B. (2011). “Magnetite and zero-valent iron nanoparticles for the remediation of uranium contaminated environmental water.” Water Res., 45(9), 2931–2942.
Crane, R. A., Dickinson, M., and Scott, T. B. (2015). “Nanoscale zero-valent iron particles for the remediation of plutonium and uranium contaminated solutions.” Chem. Eng. J., 262, 319–325.
Crane, R. A., and Noubactep, C. (2012). “Elemental metals for environmental remediation: Lessons from hydrometallurgy.” Fresenius Environ. Bull., 21(5), 1192–1196.
Crane, R. A., and Scott, T. B. (2012). “Nanoscale zero-valent iron: Future prospects for an emerging water treatment technology.” J. Hazard. Mater., 15, 211–212.
Crane, R. A., and Scott, T. B. (2013). “The effect of vacuum annealing of magnetite and zero-valent iron nanoparticles on the removal of aqueous uranium.” J. Nanotechnol., 2013(1), 1–11.
Crane, R. A., and Scott, T. B. (2014). “The removal of uranium onto nanoscale zero-valent iron particles in anoxic batch systems.” J. Nanomater., 2014(1), 1–9.
Dickinson, M., and Scott, T. B. (2010). “The application of zero-valent iron nanoparticles for the remediation of a uranium-contaminated waste effluent.” J. Hazard. Mater., 178(1–3), 171–179.
Filip, J., et al. (2007). “Environmental applications of chemically pure natural ferrihydrite.” Environ. Sci. Technol., 41(12), 4367–4374.
Glavee, G. N., Klabunde, K. J., Sorensen, C. M., and Hadjipanayis, G. C. (1995). “Chemistry of borohydride reduction of iron (II) and iron (III) irons in aqueous and nonaqueous media, formation of nanoscale Fe, FeB and Fe2B Powders.” Inorg. Chem., 34(1), 28–35.
Hoch, L. B., Mack, E. J., Hydutsky, B. W., Hershman, J. M., Skluzacek, J. M., and Mallouk, T. E. (2008). “Carbothermal synthesis of carbon-supported nanoscale zero-valent iron particles for the remediation of hexavalent chromium.” Environ. Sci. Technol., 42(7), 2600–2605.
Hsi, C. D., and Langmuir, D. (1985). “Adsorption of uranyl onto ferric oxyhydroxides. Application of the surface complexation site-binding model.” Geochim. Cosmochim. Acta., 49(9), 1931–1941.
Klimkova, S., Cernik, M., Lacinova, L., Filip, J., Jancik, D., and Zboril, R. (2011). “Zero-valent iron nanoparticles in treatment of acid mine water from in situ uranium leaching.” Chemosphere, 82(8), 1178–1184.
Lenhart, J. J., and Honeyman, B. D. (1999). “Uranium (VI) sorption to haematite in the presence of humic acid.” Geochim. Cosmochim. Acta., 63(19–20), 2891–2901.
MacFarlane, J. W., Tesh, S. J., Crane, R. A., Hallam, K. R., and Scott, T. B. (2014). “Synthesis of nano-composite surfaces via the co-deposition of metallic salts and nano particles.” Mater. Sci. Eng.: B., 182, 59–68.
Müeller, N. C., and Nowack, B. (2010). “Nano zero valent iron—The solution for water and soil remediation?” 〈http://www.observatorynano.eu〉 (Jun. 23, 2014).
Noubactep, C., Caré, S., and Crane, R. A. (2012). “Nanoscale metallic iron for environmental remediation: Prospects and limitations.” Water Air Soil Pollut., 223(3), 1363–1382.
Nurmi, J. T., et al. (2004). “Characterization and properties of metallic iron nanoparticles: Spectroscopy, electrochemistry, and kinetics.” Environ. Sci. Technol., 39(5), 1221–1230.
Popescu, I. C., Filip, P., Humelnicu, D., Humelnicu, I., Scott, T. B., and Crane, R. A. (2013). “Removal of uranium (VI) from aqueous systems by nanoscale zero-valent iron particles suspended in carboxy-methyl cellulose.” J. Nucl. Mater., 443(1–3), 250–255.
Riba, O., Scott, T. B., Ragnarsdottir, K. V., and Allen, G. C. (2008). “Reaction mechanism of uranyl in the presence of zero-valent iron nanoparticles.” Geochim. Cosmochim. Acta., 72(16), 4047–4057.
Scott, T. B., Dickinson, M., Crane, R. A., Riba, O., Hughes, G. M., and Allen, G. C. (2010). “The effects of vacuum annealing on the structure and surface chemistry of iron nanoparticles.” J. Nanopart. Res., 12(5), 1765–1775.
Scott, T. B., Popescu, I. C., Crane, R. A., and Noubactep, C. (2011). “Nano-scale metallic iron for the treatment of solutions containing multiple inorganic contaminants.” J. Hazard. Mater., 186(1), 280–287.
Wang, C. B., and Zhang, W. (1997). “Synthesizing nanoscale iron particles for rapid and complete dechlorination of TCE and PCBs.” Environ. Sci. Technol., 31(7), 2154–2156.
Wang, Q., Snyder, S., Kim, J., and Choi, H. (2009). “Aqueous ethanol modified nanoscale zerovalent iron in bromate reduction: Synthesis, characterization, and reactivity.” Environ. Sci. Technol., 43(9), 3292–3299.
Yan, S., Hua, B., Bao, Z., Yang, J., Liu, C., and Deng, B. (2010). “Uranium(VI) removal by nanoscale zerovalent iron in anoxic batch systems.” Environ. Sci. Technol., 44(20), 7783–7789.
Yunfei, X., Mallavarapu, M., and Ravendra, N. (2010). “Reduction and adsorption of in aqueous solution by nano zero-valent iron: A SEM, TEM and XPS study.” Mater. Res. Bull., 45(10), 1361–1367.
Zhang, W.-X. (2003). “Nanoscale iron particles for environmental remediation: An overview.” J. Nano. Res., 5(3–4), 323–332.
Information & Authors
Information
Published In
Copyright
© 2015 American Society of Civil Engineers.
History
Received: Dec 2, 2013
Accepted: Dec 8, 2014
Published online: Feb 4, 2015
Discussion open until: Jul 4, 2015
Published in print: Aug 1, 2015
Authors
Metrics & Citations
Metrics
Citations
Download citation
If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.