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Environmental Science and Pollution Research

, Volume 25, Issue 23, pp 22710–22724 | Cite as

Hydrothermal synthesis of a magnetic adsorbent from wasted iron mud for effective removal of heavy metals from smelting wastewater

  • Suiyi Zhu
  • Ge Dong
  • Yang Yu
  • Jiakuan Yang
  • Wu YangEmail author
  • Wei Fan
  • Dandan ZhouEmail author
  • Jiancong Liu
  • Leilei Zhang
  • Mingxin Huo
  • Yi Wang
Research Article

Abstract

A magnetic adsorbent (MA) was synthesized from wasted iron mud of a groundwater treatment plant using a novel one-step hydrothermal method. The results showed that Fe content of MA was 41.8 wt%, 2.5 times higher than that of iron mud, which was caused by hydrothermal dissolution of non-ferrous impurities under alkaline condition, such as quartz and albite, regardless of addition of ascorbic acid or not. Ferrihydrite was 92.7% in dry iron mud before adding ascorbic acid and gradually decreased to 58.1% by increasing the molar ratio of ascorbic acid to Fe following hydrothermal treatment. The strongest saturation magnetization of 16.29 emu/g was observed in the prepared MA-4 when the ascorbic acid to Fe molar ratio was 1. The highest surface site concentration of 1.31 mmol/g was observed in MA-2 when the ratio was 0.02. The mechanism of hydrothermal conversion of wasted iron mud to MA was reductive dissolution of ferrihydrite to form siderite, which was then reoxidized to maghemite. When 12.5 g/L of MA-2 was applied to treat smelting wastewater, over 99% removal of Cu2+, Zn2+, Pb2+, and Cd2+ was achieved. The major mechanisms of Cu2+ and Zn2+ adsorption by the adsorbent were cationic exchange.

Keywords

Groundwater plant Iron mud Hydrothermal synthesis Maghemite Heavy metals Smelting wastewater 

Notes

Funding information

This work was supported by the National Natural Science Foundation of China (Grant Nos. 51578118, 51238001, 51408110, 51678273, 51508079, and 51378098) and the Long-Term Program in “1000 Talent Plan for High-Level Foreign Experts” (Grant No. WQ20142200209).

Supplementary material

11356_2018_2378_MOESM1_ESM.doc (66 kb)
ESM 1 (DOC 65.5 kb)
11356_2018_2378_MOESM2_ESM.doc (58 kb)
ESM 2 (DOC 58.5 kb)
11356_2018_2378_MOESM3_ESM.doc (62 kb)
ESM 3 (DOC 62 kb)

References

  1. Agbenin JO, Olojo LA (2004) Competitive adsorption of copper and zinc by a Bt horizon of a savanna Alfisol as affected by pH and selective removal of hydrous oxides and organic matter. Geoderma 119:85–95CrossRefGoogle Scholar
  2. Ahmad R, Kumar R, Haseeb S (2012) Adsorption of Cu2+ from aqueous solution onto iron oxide coated eggshell powder: evaluation of equilibrium, isotherms, kinetics, and regeneration capacity. Arab J Chem 5:353–359CrossRefGoogle Scholar
  3. Akinwekomi V, Maree JP, Zvinowanda C, Masindi V (2017) Synthesis of magnetite from iron-rich mine water using sodium carbonate. J Environ Chem Eng 5:2699–2707CrossRefGoogle Scholar
  4. Alzaydien AS (2015) Adsorption behavior of methyl orange onto wheat bran: role of surface and pH. Orient J Chem 31:643–651CrossRefGoogle Scholar
  5. Chang Z, Yu Z, Zeng G, Huang B, Dong H, Huang J, Yang Z, Wei J, Liang H, Qi Z (2016) Phase transformation of crystalline iron oxides and their adsorption abilities for Pb and Cd. Chem Eng J 284:247–259CrossRefGoogle Scholar
  6. Chen H, Zhao Y, Wang A (2007) Removal of Cu(II) from aqueous solution by adsorption onto acid-activated palygorskite. J Hazard Mater 149:346–354CrossRefGoogle Scholar
  7. Costa R, Moura F, Oliveira P (2010) Controlled reduction of red mud waste to produce active systems for environmental applications: heterogeneous Fenton reaction and reduction of Cr(VI). Chemosphere 78:1116–1120CrossRefGoogle Scholar
  8. Creutz C (1981) Complexities of ascorbate as a reducing agent. Inorg Chem 20(12):4449–4452CrossRefGoogle Scholar
  9. Debnath S, Hausner DB, Strongin DR, Kubicki J (2010) Reductive dissolution of ferrihydrite by ascorbic acid and the inhibiting effect of phospholipid. J Colloid Interface Sci 341:215–223CrossRefGoogle Scholar
  10. Delalio A, Bajger Z, Balaz P, Castro F (1999) A new treatment process to recover magnetite, zinc and lead from iron and steelmaking dusts and sludges. ECSC Steel Research & Development on Environmental Issues. Universidade do Minho, TecMinho, BilbaoGoogle Scholar
  11. Dixit S, Hering JG (2003) Comparison of arsenic(V) and arsenic(III) sorption onto iron oxide minerals: implications for arsenic mobility. Environ Sci Technol 37:4182–4189CrossRefGoogle Scholar
  12. Elwakeel KZ, Al-Bogami AS, Elgarahy AM (2017a) Efficient retention of chromate from industrial wastewater onto a green magnetic polymer based on shrimp peels. J Polym Environ:1–12Google Scholar
  13. Elwakeel KZ, Daher AM, El-Fatah AILA, Monem HAE, Khalil MMH (2017b) Biosorption of lanthanum from aqueous solutions using magnetic alginate beads. J Disper Sci Technol 38:145–151CrossRefGoogle Scholar
  14. Estes SL, Arai Y, Becker U, Fernando S, Yuan K, Ewing RC, Zhang J, Shibata T, Powell BA (2013) A self-consistent model describing the thermodynamics of Eu(III) adsorption onto hematite. Geochim Cosmochim Acta 122:430–447CrossRefGoogle Scholar
  15. Ford RG (2002) Rates of hydrous ferric oxide crystallization and the influence on coprecipitated arsenate. Environ Sci Technol 36:2459–2463CrossRefGoogle Scholar
  16. Ghosh SK, Gould ES (1989) Electron transfer. 97. The iron-catalyzed reduction of peroxide-bound chromium(IV) with ascorbic acid. Inorg Chem 28:1538–1542CrossRefGoogle Scholar
  17. Gu X, Evans LJ (2007) Modelling the adsorption of Cd(II), Cu(II), Ni(II), Pb(II), and Zn(II) onto Fithian illite. J Colloid Interface Sci 307:317–325CrossRefGoogle Scholar
  18. Han SW, Kim DK, Hwang IG, Bae JH (2002) Development of pellet-type adsorbents for removal of heavy metal ions from aqueous solutions using red mud. J Ind Eng Chem 8:120–125Google Scholar
  19. Ho YS, McKay G (1999) Pseudo-second order model for sorption processes. Process Biochem 34:451–465CrossRefGoogle Scholar
  20. Hokkanen S, Repo E, Suopajärvi T, Liimatainen H, Niinimaa J, Sillanpää M (2014) Adsorption of Ni(II), Cu(II) and Cd(II) from aqueous solutions by amino modified nanostructured microfibrillated cellulose. Cellulose 21:1471–1487CrossRefGoogle Scholar
  21. Hui LI, Xiao DL, Hua HE, Lin R, Zuo PL (2013) Adsorption behavior and adsorption mechanism of Cu(II) ions on amino-functionalized magnetic nanoparticles. Trans Nonferrous Metals Soc China 23:2657–2665CrossRefGoogle Scholar
  22. Iakovleva E, Sillanpää M (2013) The use of low-cost adsorbents for wastewater purification in mining industries. Environ Sci Pollut Res 20:7878–7899CrossRefGoogle Scholar
  23. Jianmin Z (1994) Ferrihydrite: surface structure and its effects on phase transformation. Clay Clay Miner 42:737–746CrossRefGoogle Scholar
  24. Juang RS, Shao HJ (2002) Effect of pH on competitive adsorption of Cu(II), Ni(II), and Zn(II) from water onto chitosan beads. Adsorption 8:71–78CrossRefGoogle Scholar
  25. Kabwadzacorner P, Munthali MW, Johan E, Matsue N (2014) Comparative study of copper adsorptivity and selectivity toward zeolites. Am J Anal Chem 5:395–405CrossRefGoogle Scholar
  26. Landtwing MR, Pettke T, Halter WE, Heinrich CA, Redmond PB, Einaudi MT, Kunze K (2005) Copper deposition during quartz dissolution by cooling magmatic–hydrothermal fluids: the Bingham porphyry. Earth Planet Sci Lett 235:229–243CrossRefGoogle Scholar
  27. Lee CH, Ambrosia MS (2013) Kinetics and thermodynamic properties related to the adsorption of copper and zinc onto zeolite synthesized from coal fly ash. J Environ Sci Inter 22:1327–1335CrossRefGoogle Scholar
  28. Li J, Hu J, Sheng G, Zhao G, Huang Q (2009) Effect of pH, ionic strength, foreign ions and temperature on the adsorption of Cu(II) from aqueous solution to GMZ bentonite. Colloids Surf A Physicochem Eng Asp 349:195–201CrossRefGoogle Scholar
  29. Li Y, Yue Q, Gao B (2010) Adsorption kinetics and desorption of Cu(II) and Zn(II) from aqueous solution onto humic acid. J Hazard Mater 178:455–461CrossRefGoogle Scholar
  30. Li J, Zhang S, Chen C, Zhao G, Yang X, Li J, Wang X (2012) Removal of Cu(II) and fulvic acid by graphene oxide nanosheets decorated with Fe3O4 nanoparticles. ACS Appl Mater Interfaces 4:4991–5000CrossRefGoogle Scholar
  31. Li S, Wang W, Liu Y, W-x Z (2014) Zero-valent iron nanoparticles (nZVI) for the treatment of smelting wastewater: a pilot-scale demonstration. Chem Eng J 254:115–123CrossRefGoogle Scholar
  32. Li X, Liu N, Qi T, Wang Y, Zhou Q, Peng Z, Liu G (2015) Conversion of ferric oxide to magnetite by hydrothermal reduction in Bayer digestion process. Trans Nonferrous Metals Soc China 25:3467–3474CrossRefGoogle Scholar
  33. Liu Y, Zhao B, Tang Y, Wan P, Chen Y, Lv Z (2014) Recycling of iron from red mud by magnetic separation after co-roasting with pyrite. Thermochim Acta 588:11–15CrossRefGoogle Scholar
  34. Liu J, Yu Y, Zhu S, Yang J, Song J, Fan W, Yu H, Bian D, Huo M (2018) Synthesis and characterization of a magnetic adsorbent from negatively-valued iron mud for methylene blue adsorption. PLoS One 13:e0191229CrossRefGoogle Scholar
  35. López E, Soto B, Arias M, Núñez A, Rubinos D, Barral MT (1998) Adsorbent properties of red mud and its use for wastewater treatment. Water Res 32:1314–1322Google Scholar
  36. Lu C, Liu C, Rao GP (2008) Comparisons of sorbent cost for the removal of Ni 2+ from aqueous solution by carbon nanotubes and granular activated carbon. J Hazard Mater 151:239–246CrossRefGoogle Scholar
  37. Lucovsky G, Phillips JC (2010) Nano-regime length scales extracted from the first sharp diffraction peak in non-crystalline SiO2 and related materials: device applications. Nanoscale Res Lett 5:550–558CrossRefGoogle Scholar
  38. Man Y, Feng J (2016) Effect of gas composition on reduction behavior in red mud and iron ore pellets. Powder Technol 301:674–678CrossRefGoogle Scholar
  39. Meng Y, Chen D, Sun Y, Jiao D, Zeng D, Liu Z (2015) Adsorption of Cu2+ ions using chitosan-modified magnetic Mn ferrite nanoparticles synthesized by microwave-assisted hydrothermal method. Appl Surf Sci 324:745–750CrossRefGoogle Scholar
  40. Nadaroglu H, Kalkan E, Demir N (2010) Removal of copper from aqueous solution using red mud. Desalination 251:90–95Google Scholar
  41. Ngatenah SNI, Kutty SRM, Isa MH (2010) Optimization of heavy metal removal from aqueous solution using groundwater treatment plant sludge (GWTPS), International Conference on Environment 2010 (ICENV 2010), Penang, MalaysiaGoogle Scholar
  42. Osman SBS, Iqbal F (2014) Possible stabilization of sludge from groundwater treatment plant using electrokinetic method. Appl Mech Mater 567:110–115CrossRefGoogle Scholar
  43. Pan Y, Zhu R, Liu Q, Guo B (1999) Magnetic susceptibility variation and AMS exchange related to thermal treatment of siderite. Chin Sci Bull 44:1135–1139CrossRefGoogle Scholar
  44. Phuengprasop T, Sittiwong J, Unob F (2011) Removal of heavy metal ions by iron oxide coated sewage sludge. J Hazard Mater 186:502–507Google Scholar
  45. Pinto PS, Lanza GD, Souza MN, Ardisson JD, Lago RM (2018) Surface restructuring of red mud to produce FeO × (OH) y sites and mesopores for the efficient complexation/adsorption of β-lactam antibiotics. Environ Sci Pollut Res 25:6762–6771CrossRefGoogle Scholar
  46. Raval NP, Shah PU, Shah NK (2016) Adsorptive amputation of hazardous azo dye Congo red from wastewater: a critical review. Environ Sci Pollut Res 23:14810–14853CrossRefGoogle Scholar
  47. Sahu RC, Patel R, Ray BC (2011) Adsorption of Zn(II) on activated red mud: Neutralized by CO2. Desalination 266:93–97Google Scholar
  48. Schimanke G, Martin M (2000) In situ XRD study of the phase transition of nanocrystalline maghemite (γ-Fe2O3) to hematite (α-Fe2O3). Solid State Ionics 136-137:1235–1240CrossRefGoogle Scholar
  49. Shi L, Peng X, Luan Z, Wei N, Wang Q, Zhao Y (2009) Use of activated red mud to remove phosphate and heavy metals from the effluent of biologically treated swine wastewater. Acta Sci Circumst 29:2282–2288Google Scholar
  50. Simpson GL, Ortwerth BJ (2000) The non-oxidative degradation of ascorbic acid at physiological conditions. Biochim Biophys Acta (BBA) Mol Basis Dis 1501:12–24CrossRefGoogle Scholar
  51. Sushil S, Alabdulrahman AM, Balakrishnan M, Batra VS, Blackley RA, Clapp J, Hargreaves JS, Monaghan A, Pulford ID, Rico JL (2010) Carbon deposition and phase transformations in red mud on exposure to methane. J Hazard Mater 180:409–418CrossRefGoogle Scholar
  52. Swaddle TW, Oltmann P (1980) Kinetics of the magnetite-maghemite-hematite transformation, with special reference to hydrothermal systems. Can J Chem 58:1763–1772CrossRefGoogle Scholar
  53. Tang Y, Martin ST (2011) Siderite dissolution in the presence of chromate. Geochim Cosmochim Acta 75:4951–4962CrossRefGoogle Scholar
  54. Tang C, Zhu J, Zhou Q, Wei J, Zhu R, He H (2014) Surface heterogeneity of SiO2 polymorphs: an XPS investigation of α-quartz and α-cristobalite. J Phys Chem C 118:26249–26257CrossRefGoogle Scholar
  55. Tang C, Zhu J, Li Z, Zhu R, Zhou Q, Wei J, He H, Tao Q (2015) Surface chemistry and reactivity of SiO2 polymorphs: a comparative study on α-quartz and α-cristobalite. Appl Surf Sci 355:1161–1167CrossRefGoogle Scholar
  56. Tarso de S. Costa E, Guilherme L, Lopes G, Marques JJ, Curi N (2014) Effect of equilibrium solution ionic strength on the adsorption of Zn, Cu, Cd, Pb, As, and P on aluminum mining by-product. Water Air Soil Poll 225:1–11Google Scholar
  57. Top A, Ülkü S (2004) Silver, zinc, and copper exchange in a Na-clinoptilolite and resulting effect on antibacterial activity. Appl Clay Sci 27:13–19CrossRefGoogle Scholar
  58. Vempati RK (1989) Influence of structural and adsorbed Si on the transformation of synthetic ferrihydrite1. Clay Clay Miner 37:273–279CrossRefGoogle Scholar
  59. Vempati RK, Loeppert RH, Sittertzbhatkar H, Burghardt RC (1990) Infrared vibrations of hematite formed from aqueous- and dry-thermal incubation of Si-containing ferrihydrite. Clay Clay Miner 38:294–298CrossRefGoogle Scholar
  60. Vu HP, Moreau JW (2015) Thiocyanate adsorption on ferrihydrite and its fate during ferrihydrite transformation to hematite and goethite. Chemosphere 119:987–993CrossRefGoogle Scholar
  61. Wang S, Ang HM, Tadé MO (2008) Novel applications of red mud as coagulant, adsorbent and catalyst for environmentally benign processes. Chemosphere 72:1621–1635CrossRefGoogle Scholar
  62. Wang XS, Zhu L, Lu HJ (2011) Surface chemical properties and adsorption of Cu (II) on nanoscale magnetite in aqueous solutions. Desalination 276:154–160CrossRefGoogle Scholar
  63. Wang F, Luo L, Yi J, Liu F, Zhang Q, Wei J (2016) Adsorption behavior of red mud ceramsite to Cu2+ from simulated acidic wastewater. Chinese. J Environ Eng 10:2440–2446Google Scholar
  64. Wu Z-C, Wang Z-Z, Liu J, Yin J-H, Kuang S-P (2015) A new porous magnetic chitosan modified by melamine for fast and efficient adsorption of Cu(II) ions. Int J Biol Macromol 81:838–846CrossRefGoogle Scholar
  65. Yan L, Huang Y, Cui J, Jing C (2015) Simultaneous As(III) and Cd removal from copper smelting wastewater using granular TiO2 columns. Water Res 68:572–579CrossRefGoogle Scholar
  66. Yang W, Wang H, Zhao X (1996) Study on the complexation reaction of ascorbic acid with Fe (II) by thin layer chromatography in situ absorption spectrometry. Chinese. J Anal Chem:828–831Google Scholar
  67. Zhang MC, Zhou Q, Zhou Y, Li AM, Shuang CD (2012) Efficient adsorption and desorption of Cu2+ by a novel acid-resistant magnetic weak acid resin. Chin Chem Lett 23:1267–1270CrossRefGoogle Scholar
  68. Zhu S, Fang S, Huo M, Yu Y, Chen Y, Yang X, Geng Z, Wang Y, Bian D, Huo H (2015) A novel conversion of the groundwater treatment sludge to magnetic particles for the adsorption of methylene blue. J Hazard Mater 292:173–179CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  1. 1.Science and Technology Innovation Center for Municipal Wastewater Treatment and Water Quality ProtectionNortheast Normal UniversityChangchunChina
  2. 2.Engineering Lab for Water Pollution Control and Resources RecoveryNortheast Normal UniversityChangchunChina
  3. 3.Key Laboratory of Songliao Aquatic Environment (Ministry of Education)Jilin Jianzhu UniversityChangchunChina
  4. 4.School of Environmental Science & EngineeringHuazhong University of Science and TechnologyWuhanChina

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