Arsenate adsorption onto hematite nanoparticles under alkaline conditions: effects of aging

  • Soumya Das
  • Joseph Essilfie-Dughan
  • M. Jim Hendry
Research Paper

Abstract

Arsenate adsorption onto freshly synthesized hematite nanoparticles was carried out under highly alkaline conditions (~pH 10) at room temperature (21 °C). Dynamic light scattering measurements of hydrated hematite colloids ranged from 43 to 106 nm (~96 %). The measured zeta potential was 28.1 mV (±5.85) suggesting that the hematite nanoparticles were moderately stable. X-ray diffraction and Raman spectroscopy data showed that hematite was stable under the conditions tested, with no crystal modification evident at the completion of the experiment (9 days). An additional band position at ~826 cm−1 in the Raman spectra represented arsenate adsorbed onto hematite. The pH of the slurry dropped from ~10 to ~8 during the experiment; this was coincident with a drop in the aqueous concentration of arsenic (from ~121 to ~92 mg/L) as determined via inductively coupled plasma mass spectrometry (ICP-MS). ICP-MS analyses on the solid samples indicated a significant amount of arsenic partitioned to the solid phase during aging, corroborating the results of aqueous analyses. X-ray absorption spectroscopic analyses revealed that the bonding environment remained the same irrespective of the pH and the amount of arsenate adsorbed. Arsenate adsorbed onto hematite through a strong inner-sphere bidentate-mononuclear complex both before (0 days) and after (9 days) aging. These results are valuable for understanding the fate of potential contaminants in alkaline mine tailings environments where 2-line ferrihydrite frequently transforms to hematite rather than goethite.

Keywords

Arsenate Hematite Adsorption Aging Mine tailings Environmental contaminants 

Notes

Acknowledgments

The authors acknowledge the assistance of Tom Bonli, Virginia Chostner, Jianzhong Fan, and Waleed Mohammed-Saeid with XRD, BET, ICM-MS, and DLS-zeta potential analyses conducted at the University of Saskatchewan. The authors also acknowledge the assistance of Mert Çelikin with TEM analyses conducted at McGill University. Funding was provided by the Natural Sciences and Engineering Research Council of Canada (NSERC) and Cameco Corporation (MJH).

References

  1. Anderson PR, Benjamin MM (1985) Effects of silicon on the crystallization and adsorption properties of ferric oxides. Environ Sci Technol 19:1048–1053CrossRefGoogle Scholar
  2. Arai Y, Sparks DL, Davis JA (2004) Effects of dissolved carbonate on arsenate adsorption and surface speciation at the hematite–water interface. Environ Sci Technol 38:817–824CrossRefGoogle Scholar
  3. Brady KS, Bigham JM, Jaynes WF, Logan TJ (1986) Influence of sulfate on Fe-oxide formation: comparisons with a stream receiving acid mine drainage. Clays Clay Miner 34:266–274CrossRefGoogle Scholar
  4. Breeuwsma A, Lyklema J (1973) Physical and chemical adsorption of ions in the electrical double layer of hematite (α-Fe2O3). J Colloid Interface Sci 43:437–448CrossRefGoogle Scholar
  5. Carlson L, Schwertmann U (1981) Natural ferrihydrites in surface deposits from Finland and their association with silica. Geochim Cosmochim Acta 45:421–429CrossRefGoogle Scholar
  6. Carlson L, Bigham JM, Schwertmann U, Kyek A, Wagner F (2002) Scavenging of As from acid mine drainage by schwertmannite and ferrihydrite: a comparison with synthetic analogues. Environ Sci Technol 36:1712–1719CrossRefGoogle Scholar
  7. Christl I, Kretzschmar R (2001) Interaction of copper and fulvic acid at the hematite–water interface. Geochim Cosmochim Acta 65:3435–3442CrossRefGoogle Scholar
  8. Cornell RM, Giovanoli R, Schindler PW (1987) Effect of silicate species on the transformation of ferrihydrite into goethite and hematite in alkaline media. Clays Clay Miner 35:21–28CrossRefGoogle Scholar
  9. Das S, Hendry MJ (2013) Adsorption of molybdate by synthetic hematite under alkaline conditions: effects of aging. Appl Geochem 28:194–201CrossRefGoogle Scholar
  10. Das S, Hendry MJ, Essilfie-Dughan J (2011) Effects of adsorbed arsenate on the rate of transformation of 2-line ferrihydrite at pH 10. Environ Sci Technol 45:5557–5563CrossRefGoogle Scholar
  11. de Faria DLA, Lopes FN (2007) Heated goethite and natural hematite: can Raman spectroscopy be used to differentiate them? Vib Spec 45:117–121CrossRefGoogle Scholar
  12. de Faria DLA, Silva SV, de Oliveira MT (1997) Raman microspectroscopy of some iron oxides and oxyhydroxides. J Raman Spectrosc 28:873–878CrossRefGoogle Scholar
  13. Degen A, Kosec M (2000) Effect of pH and impurities on the surface charge of zinc oxide in aqueous solution. J Eur Ceram Soc 20:667–673CrossRefGoogle Scholar
  14. Dzombak DA, Morel FMM (1990) Surface complexation modelling—hydrous ferric oxide. Wiley, New YorkGoogle Scholar
  15. Environmental Protection Agency (EPA) (2001) National primary drinking water regulations; arsenic and clarifications to compliance and new source contaminants monitoringGoogle Scholar
  16. Essilfie-Dughan J, Hendry MJ, Warner J, Kotzer T (2012) Microscale mineralogical characterization of As, Fe, and Ni in uranium mine tailings. Geochim Cosmochim Acta 96:336–352CrossRefGoogle Scholar
  17. Essilfie-Dughan J, Hendry MJ, Warner J, Kotzer T (2013) Arsenic and iron speciation in uranium mine tailings using X-ray absorption spectroscopy. Appl Geochem 28:11–18CrossRefGoogle Scholar
  18. Fendorf S, Eick MJ, Grossl P, Sparks DL (1997) Arsenate and chromate retention mechanisms on goethite. 1. Surface structure. Environ Sci Technol 31:315–320CrossRefGoogle Scholar
  19. Ferris FG, Tazaki K, Fyfe WS (1989) Iron oxides in acid mine drainage environments and their association with bacteria. Chem Geol 74:321–330CrossRefGoogle Scholar
  20. Fischer WR, Schwertmann U (1975) The formation of hematite from amorphous iron(III) hydroxide. Clays Clay Miner 23:33–37CrossRefGoogle Scholar
  21. Ford RG (2002) Rates of hydrous ferric oxide crystallization and the influence on coprecipitated arsenate. Environ Sci Technol 36:2459–2463CrossRefGoogle Scholar
  22. Fuller CC, Davis JA, Waychunas GA (1993) Surface chemistry of ferrihydrite: Part 2. Kinetics of arsenate adsorption and coprecipitation. Geochim Cosmochim Acta 57:2271–2282CrossRefGoogle Scholar
  23. Galvez N, Barron V, Torrent J (1999) Effect of phosphate on the crystallization of hematite, goethite, and lepidocrocite from ferrihydrite. Clays Clay Miner 47:304–311CrossRefGoogle Scholar
  24. Giménez J, Martínez M, de Pablo J, Rovira M, Duro L (2007) Arsenic sorption onto natural hematite, magnetite, and goethite. J Hazard Mater 141:575–580CrossRefGoogle Scholar
  25. Goldberg S, Johnston CT (2001) Mechanisms of arsenic adsorption on amorphous oxides evaluated using macroscopic measurements, vibrational spectroscopy, and surface complexation modeling. J Colloid Interface Sci 234:204–216CrossRefGoogle Scholar
  26. Goldberg S, Forster HS, Godfrey CL (1996) Molybdenum adsorption on oxides, clay minerals, and soils. Soil Sci Soc Am J 60:425–432CrossRefGoogle Scholar
  27. Grover VA, Hu J, Engates KE, Shipley HJ (2012) Adsorption and desorption of bivalent metals to hematite nanoparticles. Environ Toxicol Chem 31:86–92CrossRefGoogle Scholar
  28. Hanesch M (2009) Raman spectroscopy of iron oxides and oxy(hydroxides) at lower laser power and possible application in environmental magnetic studies. Geophys J Int 177:941–948CrossRefGoogle Scholar
  29. Horányi G, Joó P (2002) Some peculiarities in the specific adsorption of phosphate ions on hematite and gamma-Al2O3 as reflected by radiotracer studies. J Colloid Interface Sci 247:12–17CrossRefGoogle Scholar
  30. Horányi G, Kálmán E (2004) Anion specific adsorption on Fe2O3 and AlOOH nanoparticles in aqueous solutions: comparison with hematite and gamma-Al2O3. J Colloid Interface Sci 269:315–319CrossRefGoogle Scholar
  31. Hsi C-KD, Langmuir D (1985) Adsorption of uranyl onto ferric oxyhydroxides: application of surface complexation site-binding model. Geochim Cosmochim Acta 49:1931–1941CrossRefGoogle Scholar
  32. Jain A, Raven KP, Loeppert RH (1999) Arsenite and arsenate adsorption on ferrihydrite: surface charge reduction and net OH release stoichiometry. Environ Sci Technol 33:1179–1184CrossRefGoogle Scholar
  33. Janusz W, Sędłak A (2011) Specific adsorption of carbonate ions at the hematite/aqueous electrolyte solution interface. Physicochem Probl Miner Process 46:65–72Google Scholar
  34. Kim M-J, Jang M (2010) Adsorption of molybdate onto hematite: kinetics and equilibrium. Water Geosci 30:170–173Google Scholar
  35. Ladeira ACQ, Ciminelli VST, Duarte HA, Alves MCM, Ramos AY (2001) Mechanism of anion retention from EXAFS and density functional calculations: arsenic(V) adsorbed on gibbsite. Geochim Cosmochim Acta 65:1211–1217CrossRefGoogle Scholar
  36. Legodi MA, de Waal D (2007) The preparation of magnetite, goethite, hematite and maghemite of pigment quality from mill scale iron waste. Dyes Pigment 74:161–168CrossRefGoogle Scholar
  37. Livesey NT, Huang PM (1981) Adsorption of arsenate by soils and its relation to selected chemical properties and anions. Soil Sci 131:88–94CrossRefGoogle Scholar
  38. Lloyd JR, Oremland RS (2006) Microbial transformations of arsenic in the environment: from soda lake to aquifers. Elements 2:85–90CrossRefGoogle Scholar
  39. Lumsdon DG, Fraser AR, Russell JD, Livesey NT (1984) New infrared band assignments for the arsenate ion adsorbed on synthetic goethite (α-FeOOH). J Soil Sci 35:381–386CrossRefGoogle Scholar
  40. Mamindy-Pajany Y, Hurel C, Marmier N, Roméo M (2009) Arsenic adsorption on hematite and goethite. C R Chim 12:876–881CrossRefGoogle Scholar
  41. Mengisite AA, Rao TS, Rao AVP, Singanan M (2008) Removal of Pb(II) ions from aqueous solution using activated carbon from Militia ferruginea plant leaves. Bull Chem Soc Ethiop 22:349–360Google Scholar
  42. Moldovan BJ, Jiang DT, Hendry MJ (2003) Mineralogical characterization of arsenic in uranium mine tailings precipitated from iron-rich hydrometallurgical solutions. Environ Sci Technol 37:873–879CrossRefGoogle Scholar
  43. Müller K, Ciminelli VST, Dantas MSS (2010) A comparative study of As(III) and As(V) in aqueous solutions and adsorbed on iron oxy-hydroxides by Raman spectroscopy. Water Res 44:5660–5672CrossRefGoogle Scholar
  44. Myneni SCB, Traina SJ, Waychunas GA, Logan TJ (1998) Experimental and theoretical vibrational spectroscopic evaluation of arsenate coordination in aqueous solutions and solids. Geochim Cosmochim Acta 62:3285–3300CrossRefGoogle Scholar
  45. Oh SH, Cook DC, Townsend HE (1998) Characterization of iron-oxides commonly formed as corrosion products on steel. Hyperfine Interact 112:59–65CrossRefGoogle Scholar
  46. Opiso E, Charnock J, Sato T, Ankraku S, Numako C, Yoneda T (2010) Incorporation of arsenic during the formation of Mg-bearing minerals at alkaline conditions. Miner Eng 23:230–237CrossRefGoogle Scholar
  47. Paige CR, Snodgrass WJ, Nicholson RV, Scharer JM (1996) The crystallization of arsenate-contaminated iron hydroxide solids at high pH. Water Environ Res 68:981–987CrossRefGoogle Scholar
  48. Paige CR, Snodgrass WJ, Nicholson RV, Scharer JM (1997a) An arsenate effect on ferrihydrite dissolution kinetics under acidic oxic conditions. Water Res 31:2370–2382CrossRefGoogle Scholar
  49. Paige CR, Snodgrass WJ, Nicholson RV, Scharer JM (1997b) The effect of phosphate on the transformation of ferrihydrite into crystalline products in alkaline media. Water Air Soil Pollut 97:397–412Google Scholar
  50. Peak D, Sparks DL (2002) Mechanisms of selenate adsorption on iron oxides and hydroxides. Environ Sci Technol 36:1460–1466CrossRefGoogle Scholar
  51. Pochard I, Denoyel R, Couchot P, Foissy A (2002) Adsorption of barium and calcium chloride onto negatively charged α-Fe2O3 particles. J Colloid Interface Sci 255:27–35CrossRefGoogle Scholar
  52. Ravel B, Newville M (2005) ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT. J Synchrotron Rad 12:537–541CrossRefGoogle Scholar
  53. Rehr JJ, Albers RC, Zabinsky SI (1992) High-order multiple-scattering calculations of X-ray absorption fine structure. Phys Rev Lett 69:3397–3430CrossRefGoogle Scholar
  54. Rull F, Martinez-Frias J, Sansano A, Medina J, Edwards HGM (2004) Comparative micro-Raman study of the Nakhla and Vaca Muerta meteorites. J Raman Spectrosc 35:497–503CrossRefGoogle Scholar
  55. Russel N (2001) Arsenic and old waste: U.S. Congress Debates Bush Environmental Policy; International Committee of the Fourth International (ICFI)Google Scholar
  56. Schwertmann U, Cornell RM (1991) Iron oxides in the laboratory-preparation and characterization. VCH, New YorkGoogle Scholar
  57. Schwertmann U, Murad E (1983) The effect of pH on the formation of goethite and hematite from ferrihydrite. Clays Clay Miner 31:277–284CrossRefGoogle Scholar
  58. Shaw SA, Hendry MJ, Essilfie-Dughan J, Kotzer T, Wallschläger D (2012) Distribution, characterization, and controls on elements of concern in uranium mine tailings, Key Lake, Saskatchewan, Canada. Appl Gechem 26:2044–2056CrossRefGoogle Scholar
  59. Suarez DL, Goldberg S, Su C (1999) Evaluation of oxyanion adsorption mechanisms on oxides using FTIR spectroscopy and electrophoretic mobility. Am Chem Soc Symp Ser 715:136–178Google Scholar
  60. Sun XH, Doner HE (1996) An investigation of arsenate and arsenite bonding structures on goethite by FTIR. Soil Sci 161:865–872CrossRefGoogle Scholar
  61. Sun T, Paige CR, Snodgrass WJ (1999) Combined effect of arsenic and cadmium on the transformation of ferrihydrite onto crystalline products. J Univ Sci Technol 3:168–173Google Scholar
  62. Thibeau RH, Brown CW, Heidersbach RH (1978) Raman spectra of possible corrosion products of iron. Appl Spectrosc 32:532–535CrossRefGoogle Scholar
  63. Todorović M, Milonjić SK, Čomor JJ, Gal IJ (1992) Adsorption of radioactive ions 137Cs+, 85Sr2+, and 60Co2+ on natural magnetite and hematite. Sep Sci Technol 27:671–679CrossRefGoogle Scholar
  64. Torrent J, Guzman R (1982) Crystallization of Fe(III)-oxides from ferrihydrite in salt solutions: osmotic and specific ion effects. Clay Miner 17:463–469CrossRefGoogle Scholar
  65. Vaughan DJ (2006) Arsenic. Elements 2:71–75CrossRefGoogle Scholar
  66. Waychunas GA, Rea BA, Fuller CC, Davis JA (1993) Surface chemistry of ferrihydrite: Part 1. EXAFS studies of the geometry of coprecipitated and adsorbed arsenate. Geochim Cosmochim Acta 57:2251–2269CrossRefGoogle Scholar
  67. Waychunas GA, Kim CS, Banfield JF (2005) Nanoparticulate iron oxide minerals in soils and sediments: unique properties and contaminant scavenging mechanisms. J Nanopart Res 7:409–433CrossRefGoogle Scholar
  68. ZhangLei H, Chen L, Zhang L, Yu X (2011) Impact of environmental conditions on the adsorption behavior of radionuclide Ni(II) onto hematite. J Radioanal Nucl Chem 287:357–365CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media Dordrecht 2014

Authors and Affiliations

  • Soumya Das
    • 1
  • Joseph Essilfie-Dughan
    • 1
  • M. Jim Hendry
    • 1
  1. 1.Department of Geological SciencesUniversity of SaskatchewanSaskatoonCanada

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