Recovery of zinc granules from synthetic electroplating wastewater using fluidized-bed homogeneous crystallization process

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In the present work, the recovery of zinc granules from synthetic electroplating wastewater was evaluated using fluidized-bed homogeneous crystallization. The effect of carbonate-to-zinc ([CO32−]/[Zn2+]) molar ratio (1.0–2.0), precipitant pH (10.30–11.20), initial zinc concentration (100–500 mg/L), and anions (Cl, F, and NO3) on the removal and granulation efficiencies of zinc was investigated. Results show that the highest granulation efficiency of 96.70% was attained at an influent zinc concentration of 300 mg/L, precipitant pH of 10.60 and [CO32−]/[Zn2+] of 1.2. Meanwhile, the highest removal efficiency of 99.90% was obtained at a precipitant pH of 10.60, [CO32−]/[Zn2+] of 1.2, and influent zinc concentration of 100 mg/L. Moreover, the residual zinc concentration of 0.15 mg/L was attained in the treated effluent, which is within the maximum contaminant level of 5.0 mg/L set by the US Environmental Protection Agency and World Health Organization. The presence of anions had little but insignificant effect on the removal where the treated effluent has a residual zinc concentration of 0.44 mg/L. Based on the X-ray diffraction analysis, zinc granules were recovered in the form of smithsonite and hydrozincite with rhombohedral-hexagonal and monoclinic structures, respectively. A broad size distribution was displayed by zinc granules where majority of the pellet diameters fall within the range of 0.149–2.000 mm. Overall, fluidized-bed homogeneous crystallization produced higher-purity pellets and proved to be an effective alternative to seeded crystallization technology.

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  1. Andalib M, Elbeshbishy E, Mustafa N, Hafez H, Nakhla G, Zhu J (2014) Performance of an anaerobic fluidized bed bioreactor (AnFBR) for digestion of primary municipal wastewater treatment biosolids and bioethanol thin stillage. Renew Energy 71:276–285

  2. Ballesteros FC, Salcedo AFS, Vilando AC, Huang YH, Lu MC (2016) Removal of nickel by homogeneous granulation in a fluidized-bed reactor. Chemosphere 164:59–67

  3. Boryczko B, Hołda A, Kolenda Z (2014) Depletion of the non-renewable natural resource reserves in copper, zinc, lead and aluminium production. J Clean Prod 84:313–321

  4. Brackin MJ, Mckenzie DE, Hughes BM, Heitkamp MA (1996) Laboratory-scale evaluation of fluidized bed reactor technology for biotreatment of maleic anhydride process wastewater. J Ind Microbiol 16:216–223

  5. Chen CS, Shih YJ, Huang YH (2015) Remediation of lead (Pb(II)) wastewater through recovery of lead carbonate in a fluidized-bed homogenous crystallization (FBHC) system. Chem Eng J 279:120–128

  6. Chen X, Ren P, Li T, Trembly JP, Liu X (2018) Zinc removal from model wastewater by electrocoagulation: processing, kinetics and mechanism. Chem Eng J 349:358–367

  7. Chicagov AV, Belonozhko AB, Lopatin AL, Dokina TN, Samokhvalova OL, Ushakovskaya TV, Shilova ZV (1990) Information-calculating system on crystal structure data for minerals (MINICRYST). Kristallografiya 35:610–616

  8. Chung J, Jeong E, Choi JW, Yun ST, Maeng SK, Hong SW (2015) Factors affecting crystallization on copper sulfide in fed-batch fluidized bed reactor. Hydrometallurgy 152:107–112

  9. Downs B, Swaminathan R, Bartelmehs K (1993) Crystallographic tables for the rhombohedral carbonates. Am Mineral 78:1104–1107

  10. Ghnimi SM, Frini-Srasra N (2018) A comparison of single and mixed pillared clays for zinc and chromium cations removal. Appl Clay Sci 158:150–157

  11. Ghose S (1964) The crystal structure of hydrozincite, Zn5(OH)6(CO3)2. Acta Cryst 17:1051–1057

  12. Guevara HPR, Ballesteros FC, Vilando AC, de Luna MDG, Lu MC (2017) Recovery of oxalate from bauxite wastewater using fluidized-bed homogeneous granulation process. J Clean Prod 154:130–138

  13. Guillard D, Lewis AE (2001) Nickel carbonate precipitation in a fluidized-bed reactor. Ind Eng Chem Res 40:5564–5569

  14. Hambidge KM, Krebs NF (2007) Zinc deficiency: a special challenge. J Nutr 137:1101–1105

  15. Hosseini SS, Bringas E, Tan NR, Ortiz I, Ghahramani M, Shahmirzadi MAA (2016) Recent progress in the development of high performance polymeric membranes and materials for metal plating wastewater treatment: a review. J Water Process Eng 9:78–110

  16. Kobya M, Demirbas E, Ozyonar F, Sirtbas G, Gengec E (2017) Treatments of alkaline non-cyanide, alkaline cyanide and acidic zinc electroplating wastewaters by electrocoagulation. Process Saf Environ Prot 105:373–385

  17. Kunicky Z, Jandova J, Dostal J, Dvorak J (2008) Zinc recovery from wastes using spent acid from scrapped lead acid batteries. The Southern African Institute of Mining and Metallurgy. Accessed 11 June 2019

  18. Lee CI, Yang WF (2005) Heavy metal removal from aqueous solution in sequential fluidized-bed reactors. Environ Technol 26:1345–1354

  19. Lee C, Yang W, Hsieh C (2004) Removal of Cu (II) from aqueous solution in a fluidized-bed reactor. Chemosphere 57:1173–1180

  20. Martín-Lara MA, Blázquez G, Trujillo MC, Pérez A, Calero M (2014) New treatment of real electroplating wastewater containing heavy metal ions by adsorption onto olive stone. J Clean Prod 81:120–129

  21. Mokone TP, van Hille RP, Lewis AE (2012) Metal sulphides from wastewater: assessing the impact of supersaturation control strategies. Water Res 46:2088–2100

  22. Moussavi G, Talebi S (2012) Comparing the efficacy of a novel waste-based adsorbent with PAC for the simultaneous removal of Cr(VI) and cyanide from electroplating wastewater. Chem Eng Res Des 90:960–966

  23. Naito W, Kamo M, Tsushima K, Iwasaki Y (2010) Exposure and risk assessment of zinc in Japanese surface waters. Sci Total Environ 408:4271–4284

  24. Nriagu J (2011) Encyclopedia of environmental health: zinc toxicity in humans. Elsevier, Amsterdam.

  25. Park Y, Kim SH, Matalon S, Wang NHL, Franses EI (2009) Effect of phosphate salts concentrations, supporting electrolytes, and calcium phosphate salt precipitation on the pH of phosphate buffer solutions. Fluid Phase Equilib 278:76–84

  26. Patterson JW, Allen HE, Scala JJ (1977) Carbonate precipitation for heavy metals pollutants. J Water Pollut Control Fed 49:2397–2410

  27. Peng ZX, He HJ, Yang CP, Zeng GM, Wen S, Yan Z, Xiang HH, Cheng Y, Tarre S, Green M (2017) Biological treatment of wastewater with high concentrations of zinc and sulfate ions from zinc pyrithione synthesis. Trans Nonferrous Met Soc China 27:2481–2491

  28. Pereira FV, Gurgel LVA, Gil LF (2010) Removal of Zn2+ from aqueous single metal solutions and electroplating wastewater with wood sawdust and sugarcane bagasse modified with EDTA dianhydride (EDTAD). J Hazard Mater 176:856–863

  29. Plum LM, Rink L, Hajo H (2010) The essential toxin: impact of zinc on human health. Int J Environ Res Public Health 7:1342–1365

  30. Rubio J, Tessele F (1997) Removal of heavy metal ions by adsorptive particulate flotation. Min Eng 10:671–679

  31. Sanna R, Medas D, Podda F, Meneghini C, Casu M, Lattanzi P, Scoriapino MA, Floris C, Cannas C, de Giudici G (2015) Binding of bis-(2-ethylhexyl)phthalate at the surface of hydrozincite nanocrystals: an example of organic molecules absorption onto nanocrystalline minerals. J Colloid Interface Sci 457:298–306

  32. Senthilkumar R, Vijayaraghavan K, Thilakavathi M, Iyer PVR, Velan M (2006) Seaweeds for the remediation of wastewaters contaminated with zinc(II) ions. J Hazard Mater 136:791–799

  33. Shimizu Y, Hirasawa I (2013) Impurities effect on carbonate reactive crystallization for the wastewater. ISRN Chem Eng 1–8

  34. Sönmez S, Aktas S, Açma E (2003) A study on the treatment of wastes in hot dip galvanizing plants. Can Metall Q 42:289–300

  35. Stefanidou M, Maravelias C, Dona A, Spiliopoulou C (2008) Zinc: a multipurpose trace element. Cancer Sci 99:1515–1522

  36. Stoilova D, Koleva V, Vasileva V (2002) Infrared study of some synthetic phases of malachite (Cu2(OH)2CO3)-hydrozincite (Zn5(OH)6(CO3)2) series. Spectrochim Acta, Part A 58:2051–2059

  37. Tai CY, Chien WC, Chen CY (1999) Crystal growth kinetics of calcite in a dense fluidized-bed crystallizer. Am Inst Chem Eng J 45:1605–1614

  38. Tai CY, Chen PC, Tsao TM (2006) Growth kinetics of CaF2 in a pH-stat fluidized-bed crystallizer. J Cryst Growth 290:576–584

  39. US Environmental Protection Agency (2014) Guidelines for Water Reuse. US Agency for International Development, Washington

  40. Van Dijk JC, Van Ammers M, Graveland A, Nuhn PANM (1986) State of the art of pellet softening in The Netherlands. Water Supply 4:223–235

  41. Vilando AC, Caparanga AR, Huang YH, Lu MC (2017) Tohdite recovery from water by fluidized-bed homogeneous granulation process. Desalin Water Treat 96:224–230

  42. World Health Organization (2011) Guidelines for drinking-water quality, 4th edn. WHO Press, Geneva, pp 433–434

  43. Ye X, Ye ZL, Lou Y, Pan S, Wang X, Wang MK, Chen S (2016) A comprehensive understanding of saturation index and upflow velocity in a pilot-scale fluidized bed reactor for struvite recovery from swine wastewater. Powder Technol 295:16–26

  44. Zhang J, Xu Y, Zhou J, Liang Y, Chen C, Liu Q, Qian G, Xu ZP (2013) Magnetic nanomaterials recovered from co-treatment of CN-containing electroplating wastewaters and pickle acid liquor. Sep Purif Technol 120:186–190

  45. Zumdahl SS (2009) Chemical Principles, 6th edn. Massachusetts, Boston

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This work was supported by the Ministry of Science and Technology, Taiwan, under Grant MOST 102-2221-E-041-001-MY3 and National Research Foundation (NRF) of Korea through Ministry of Education under Grant 2016R1A6A1A03012812.

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Correspondence to M. C. Lu.

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Editorial responsibility: J Aravind.

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de Luna, M.D.G., Paulino, L.H.S., Futalan, C.M. et al. Recovery of zinc granules from synthetic electroplating wastewater using fluidized-bed homogeneous crystallization process. Int. J. Environ. Sci. Technol. 17, 129–142 (2020).

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  • Granulation efficiency
  • Hydrozincite
  • Smithsonite
  • Solubility diagram