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Effects of crystallization reagent and pH on the sulfide crystallization of Cu and Ni in fluidized bed reactor

유동층 반응기를 이용한 구리와 니켈의 황화물 결정화에 결정화 시약 및 pH가 미치는 영향

  • Jeong, Eunhoo (Center for Water Resources Cycle Research, Korea Institute of Science and Technology) ;
  • Shim, Soojin (Center for Water Resources Cycle Research, Korea Institute of Science and Technology) ;
  • Yun, Seong Taek (Korea University Graduate School of Energy, Environment Policy&Technology) ;
  • Hong, Seok Won (Center for Water Resources Cycle Research, Korea Institute of Science and Technology)
  • 정은후 (한국과학기술연구원 녹색도시기술연구소 물자원순환연구단) ;
  • 심수진 (한국과학기술연구원 녹색도시기술연구소 물자원순환연구단) ;
  • 윤성택 (고려대학교 그린스쿨 대학원) ;
  • 홍석원 (한국과학기술연구원 녹색도시기술연구소 물자원순환연구단)
  • Received : 2014.03.24
  • Accepted : 2014.04.10
  • Published : 2014.04.15

Abstract

Wastewater containing heavy metals such as copper (Cu) and nickel (Ni) is harmful to humans and the environment due to its high toxicity. Crystallization in a fluidized bed reactor (FBR) has recently received significant attention for heavy metal removal and recovery. It is necessary to find optimum reaction conditions to enhance crystallization efficacy. In this study, the effects of crystallization reagent and pH were investigated to maximize crystallization efficacy of Cu-S and Ni-S in a FBR. CaS and $Na_2S{\cdot}9H_2O$ were used as crystallization reagent, and pH were varied in the range of 1 to 7. Additionally, each optimum crystallization condition for Cu and Ni were sequentially employed in two FBRs for their selective removal from the mixture of Cu and Ni. As major results, the crystallization of Cu was most effective in the range of pH 1-2 for both CaS and $Na_2S{\cdot}9H_2O$ reagents. At pH 1, Cu was completely removed within five minutes. Ni showed a superior reactivity with S in $Na_2S{\cdot}9H_2O$ compared to that in CaS at pH 7. When applying each optimum crystallization condition sequentially, only Cu was firstly crystallized at pH 1 with CaS, and then, in the second FBR, the residual Ni was completely removed at pH 7 with $Na_2S{\cdot}9H_2O$. Each crystal recovered from two different FBRs was mainly composed of CuxSy and NiS, respectively. Our results revealed that Cu and Ni can be selectively recovered as reusable resources from the mixture by controlling pH and choosing crystallization reagent accordingly.

Keywords

References

  1. Aderhold, D., Williams, C.J. and Edyvean, R.G.J. (1996) The Removal of Heavy-metal Ions by Seaweeds and their Derivatives. Biores. Tech., 58(1), 1-6. https://doi.org/10.1016/S0960-8524(96)00072-7
  2. Ahmed Basha, C., Bhadrinarayana, N.S., Anantharaman, N. and Meera Sheriffa Begum, K.M. (2008) Heavy Metal Removal from Copper Smelting Effluent using Electrochemical Cylindrical Flow Reactor, J. Hazard. Mater., 152(1), 71-78. https://doi.org/10.1016/j.jhazmat.2007.06.069
  3. Akbal, F. and Camci, S. (2011) Copper, Chromium and Nickel Removal from Metal Plating Wastewater by Electrocoagulation, DESALINATION, 269(1-3), 214-222. https://doi.org/10.1016/j.desal.2010.11.001
  4. Armenante, P.M. (1997) Precipitation of heavy metals from wastewaters, p.1-43, NJIT, New Jersey.
  5. Ayres, R.U. (1997) Metals Recycling: Economic and Environmental Implications, Res. Cons. and Recycl., 21(3), 145-173. https://doi.org/10.1016/S0921-3449(97)00033-5
  6. Bebie, J., Schoonen, M.A.A., Fuhrmann, M. and Strongin, D.R. (1998) Surface Charge Development on Transition Metal Sulfides: An Electrokinetic Study, Geochim. Cosmochim. Acta, 62(4), 633-642. https://doi.org/10.1016/S0016-7037(98)00058-1
  7. Crini, G. (2005) Recent Developments in Polysaccharide-based Materials Used as Adsorbents in Wastewater Treatment, Prog. Polym. Sci., 30(1), 38-70. https://doi.org/10.1016/j.progpolymsci.2004.11.002
  8. EPA, USA, http://cfpub.epa.gov/ecotox/blackbox/help/ecotoxsop.pdf
  9. Espinoza, E., Escudero, R. and Tavera, F.J. (2012) Waste Water Treatment by Precipitating Copper, Lead and Nickel Species, Res. J. Recent. Sci., 1(10), 1-6. https://doi.org/10.5530/jscires.2012.1.1
  10. Fujimoto, N., Mizuochi, T. and Togami, Y. (1991) Phosphorus Fixation in the Sludge Treatment System of a Biological Phosphorus Removal Process, Water Sci. & Tech., 23(4-6), 635-640.
  11. Kongscricharoern, N. and Polprasert. C. (1995) Electrochemical Precipitation of Chromium($Cr^{6+}$) from an Electroplating Wastewater, Water Sci. & Tech., 31(9), 109-117.
  12. Lee. C. I., Yang, W.F. and Hsieh, C.I. (2004) Removal of Cu(II) from Aqueous Solution in a Fluidized-bed Reactor, Chemosphere, 57(9), 1173-1180. https://doi.org/10.1016/j.chemosphere.2004.08.028
  13. Lee. C. I. and Yang, W.F. (2005) Heavy Metal Removal from Aqueous Solution in Sequential Fluidized-bed Reactors, Environ. Technol., 26(12), 1345-1354. https://doi.org/10.1080/09593332608618613
  14. Lewis, A.E. (2010) Rewiew of Metal sulfide Precipitation, Hydrometallurgy, 104(2), 222-234. https://doi.org/10.1016/j.hydromet.2010.06.010
  15. Madoni, P. (2000) The Acute Toxicity of Nickel to Freshwater Ciliates, Environ. Pollut., 109(1), 53-59. https://doi.org/10.1016/S0269-7491(99)00226-2
  16. Ministry of Environment. (2009) Countermeasure against Recycling Metal Waste Resources, p.1-33, Ministry of Strategy and Finance, Ministry of Education, Science and Technology, Ministry of Defence, Ministry of Knowledge Economy, Ministry of Environment and Ministry of Land, Transport and Maritime Affairs, Sejong.
  17. Ministry of Environment. (2010) Detailed Implementation Plan against Recycling Metal Waste Resources, p.1-92, Ministry of environment, Sejong.
  18. Mohan, D. and Pittman Jr, C.U. (2007) Arsenic Removal from Water/Wastewater Using Adsorbents-A Critical Review, J. Hazard. Mater., 142(1-2), 1-53. https://doi.org/10.1016/j.jhazmat.2007.01.006
  19. Momberg, G.A. and Oellermann, R.A. (1992) The Removal of Phosphate by Hydroxyapatite and Struvite Crystallization in South Africa, Water Sci. & Tech., 26(5-6), 987-996.
  20. Mokone, T.P., van Hille, R.P. and Lewis, A.E. (2012) Metal sulfides from Wastewater: Assessing the Impact of Supersaturation Control strategies, Water Res., 46(7), 2088-2100. https://doi.org/10.1016/j.watres.2012.01.027
  21. Nduna, M.K., Lewis, A.E. and Nortier, P. (2014) A Model for the Zeta Potential of Copper sulfide, Colloids and Surfaces A: Physicochem. Eng. Aspects, 441(20), 643-652. https://doi.org/10.1016/j.colsurfa.2013.10.024
  22. Scholler, M., Dijk, J.C., Wilms, D. (1987) Env. Technol., p.294-303, Springer, Netherlands.
  23. Soya, K., Mihara, N., Kuchar, D., Kubota, M., Matsuda, H. and Fukuta, T. (2008) Selective Sulfidation of Copper, Zinc and Nickel in Plating Wastewater Using Calcium Sulfide, WASET, 44, 356-360.
  24. van Hille, R.P., Peterson, K.A. and Lewis, A.E. (2005) Copper sulfide Precipitation in a Fluidised Bed Reactor, Chem. Eng. Sci., 60(10), 2571-2578. https://doi.org/10.1016/j.ces.2004.11.052
  25. Veeken, A.H.M., de Vries, S., van der Mark, A. and Rulkens, W.H. (2003) Selective Precipitation of Heavy Metals as Controlled by a Sulfide-Selective Electrode, Sep. Sci. and Technol., 38(1), 1-19. https://doi.org/10.1081/SS-120016695