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Journal of Soils and Sediments

, Volume 12, Issue 5, pp 704–712 | Cite as

Organoclays reduce arsenic bioavailability and bioaccessibility in contaminated soils

  • Binoy Sarkar
  • Ravi NaiduEmail author
  • Mohammad Mahmudur Rahman
  • Mallavarapu Megharaj
  • Yunfei Xi
SOILS, SEC 3 • REMEDIATION AND MANAGEMENT OF CONTAMINATED OR DEGRADED LANDS • RESEARCH ARTICLE

Abstract

Purpose

Naturally occurring layer silicate clay minerals can be value added by modifying their surface properties to enhance their efficacy in the remediation of environmental contaminants. Silicate clay minerals modified by the introduction of organic molecules into the mineral structure are known as organoclays and show much promise for environmental remediation applications. The present study assesses the extent of decrease in bioavailable and bioaccessible arsenic (As) via enhanced adsorption by soil treated with organoclays.

Materials and methods

Organoclays were prepared from hexadecyl trimethylammonium bromide (HDTMA) and Arquad® 2HT-75 (Arquad) at surfactant loadings equivalent to twice the cation exchange capacity (CEC) of an Australian bentonite and characterised by X-ray diffraction (XRD). Batch experiments were conducted to evaluate the adsorption of arsenate onto the organoclays from aqueous solutions. Encouraged by these results, the organoclays were applied to As-spiked soils, at 10% and 20% (w/w) rates, to assess their capacity to stabilise soil As. After 1 month of incubation in the laboratory, bioavailable (1 mM Ca(NO3)2 extractable) and bioaccessible (1 M glycine extractable) As from the spiked soils were assessed.

Results and discussion

Both the organobentonites effectively removed As from aqueous solutions. The adsorbent prepared with Arquad adsorbed 23% more As from aqueous phase than adsorbent prepared with HDTMA. Adsorption of As was controlled by anion exchange and electrostatic attraction. When applied to As-contaminated soils, the organoclays reduced the bioavailable As by as much as 81%. The extent of reduction of bioaccessible As was only up to 58%. The adsorbents were not as efficient in reducing bioaccessible As in contaminated soils as compared with bioavailable As. It could be attributed to the extreme pH condition (pH = 3) of the extractant used in the physiologically based extraction test method for assessing bioaccessibility. The greater the loading rate of organoclays, the better was the stabilisation of As in soils.

Conclusions

Organobentonites prepared from HDTMA and Arquad at surfactant loadings greater than the CEC of the bentonite effectively remove As from aqueous solutions. Also, when applied to As-contaminated soils, both the organoclays reduce the bioavailability of soil As. The Arquad-modified bentonite performs better than HDTMA-modified bentonite. Data from this initial study can be used to further improve the stabilisation of soil As by using organoclays.

Keywords

Adsorption Arsenic stabilisation in soil Bioaccessibility Bioavailability Organoclay Remediation 

Notes

Acknowledgements

Dr. Binoy Sarkar is thankful to the University of South Australia for the award of a University President Scholarship (UPS) and CRC CARE for Ph.D. fellowship. The authors would like to acknowledge the financial and infrastructural support from the Centre for Environmental Risk Assessment and Remediation (CERAR), University of South Australia. The authors would also like to thank Dr. Dane Lamb and Mr. Phil Thomas for their kind editing of the manuscript and two anonymous reviewers for their valuable suggestions to improve the quality of the manuscript.

References

  1. Bate B, Burns SE (2010) Effect of total organic carbon content and structure on the electrokinetic behavior of organoclay suspensions. J Colloid Interface Sci 343:58–64CrossRefGoogle Scholar
  2. Benhammou A, Yaacoubi A, Nibou L, Tanouti B (2005) Adsorption of metal ions onto Moroccan stevensite: kinetic and isotherm studies. J Colloid Interface Sci 282:320–326CrossRefGoogle Scholar
  3. Boisson J, Ruttens A, Mench M, Vangronsveld J (1999) Evaluation of hydroxyapatite as a metal immobilizing soil additive for the remediation of polluted soils. Part 1. Influence of hydroxyapatite on metal exchangeability in soil, plant growth and plant metal accumulation. Environ Pollut 104:225–233CrossRefGoogle Scholar
  4. Borden D, Giese RF (2001) Baseline studies of the clay minerals society source clays: cation exchange capacity measurements by the ammonia-electrode method. Clays Clay Miner 49:444–445CrossRefGoogle Scholar
  5. Boyd SA, Shaobai S, Lee JF, Mortland MM (1988) Pentachlorophenol sorption by organo-clays. Clays Clay Miner 36:125–130CrossRefGoogle Scholar
  6. Cao X, Ma LQ (2004) Effects of compost and phosphate on plant arsenic accumulation from soils near pressure-treated wood. Environ Pollut 132:435–442CrossRefGoogle Scholar
  7. Chakraborti D, Mukherjee SC, Pati S, Sengupta MK, Rahman MM, Chowdhury UK, Lodh D, Chanda CR, Chakraborti AK, Basu GK (2003) Arsenic groundwater contamination in Middle Ganga Plain, Bihar, India: a future danger? Environ Health Perspect 111:1194–1201CrossRefGoogle Scholar
  8. Dubinin MM, Radushkevich LV (1947) Equation of the characteristic curve of activated charcoal. Proc Acad Sci Phys Chem Sec USSR 55:331–333Google Scholar
  9. Fendorf S, La Force MJ, Li G (2004) Temporal changes in soil partitioning and bioaccessibility of arsenic, chromium, and lead. J Environ Qual 33:2049–2055CrossRefGoogle Scholar
  10. Freundlich H (1906) Über die adsorption in lösungen. Z Phys Chem (Leipzig) 57:385–470Google Scholar
  11. Frost RL, Zhoua Q, He H, Xi Y (2008) An infrared study of adsorption of para-nitrophenol on mono-, di- and tri-alkyl surfactant intercalated organoclays. Spectrochim Acta Part A 69:239–244CrossRefGoogle Scholar
  12. Hartley W, Edwards R, Lepp NW (2004) Arsenic and heavy metal mobility in iron oxide-amended contaminated soils as evaluated by short- and long-term leaching tests. Environ Pollut 131:495–504CrossRefGoogle Scholar
  13. Helfferich F (1962) Ion exchange. McGraw-Hill, New YorkGoogle Scholar
  14. Helgesen H, Larsen EH (1998) Bioavailability and speciation of arsenic in carrots grown in contaminated soil. Analyst 123:791–796CrossRefGoogle Scholar
  15. Hobson JP (1969) Physical adsorption isotherms extending from ultrahigh vacuum to vapor pressure. J Phys Chem 73:2720–2727CrossRefGoogle Scholar
  16. IARC (2004) IARC monographs on arsenic in drinking water. IARC (International Agency for Research on Cancer), LyonsGoogle Scholar
  17. Juhasz AL, Weber J, Smith E, Naidu R, Rees M, Rofe A, Kuchel T, Sansom L (2009) Assessment of four commonly employed in vitro arsenic bioaccessibility assays for predicting in vivo relative arsenic bioavailability in contaminated soils. Environ Sci Technol 43:9487–9494CrossRefGoogle Scholar
  18. Krishna BS, Murty DSR, Jai Prakash BS (2001) Surfactant-modified clay as adsorbent for chromate. Appl Clay Sci 20:65–71CrossRefGoogle Scholar
  19. Li Z, Willms CA, Kniola K (2003) Removal of anionic contaminants using surfactant-modified palygorskite and sepiolite. Clays Clay Miner 51:445–451CrossRefGoogle Scholar
  20. Mahramanlioglu M, Kizilcikli I, Bicer IO (2002) Adsorption of fluoride from aqueous solution by acid treated spent bleaching earth. J Fluorine Chem 115:41–47CrossRefGoogle Scholar
  21. Malekian R, Abedi-Koupai J, Eslamian SS (2011) Influences of clinoptilolite and surfactant-modified clinoptilolite zeolite on nitrate leaching and plant growth. J Hazard Mater 185:970–976CrossRefGoogle Scholar
  22. Miretzky P, Cirelli AF (2010) Remediation of arsenic-contaminated soils by iron amendments: a review. Crit Rev Environ Sci Technol 40:93–115CrossRefGoogle Scholar
  23. Mohan D, Pittman JCU (2007) Arsenic removal from water/wastewater using adsorbents—a critical review. J Hazard Mater 142:1–53CrossRefGoogle Scholar
  24. Moon DH, Dermatas D, Menounou N (2004) Arsenic immobilization by calcium-arsenic precipitates in lime treated soils. Sci Total Environ 330:171–185CrossRefGoogle Scholar
  25. Nagar R, Sarkar D, Makris K, Datta R, Sylvia V (2009) Bioavailability and bioaccessibility of arsenic in a soil amended with drinking-water treatment residuals. Arch Environ Contam Toxicol 57:755–766CrossRefGoogle Scholar
  26. Naidu R, Bhattacharya P (2009) Arsenic in the environment—risks and management strategies. Environ Geochem Health 31:1–8CrossRefGoogle Scholar
  27. Naidu R, Smith E, Owens G, Bhattacharya P, Nadebaum P (2006) Managing arsenic in the Asia-Pacific region: an overview. In: Naidu R, Smith E, Owens G, Bhattacharya P, Nadebaum P (eds) Managing arsenic in the environment from soil to human health. CSIRO, Adelaide, pp 641–645Google Scholar
  28. Naidu R, Smith E, Imamul Huq S, Owens G (2009) Sorption and bioavailability of arsenic in selected Bangladesh soils. Environ Geochem Health 31:61–68CrossRefGoogle Scholar
  29. Onyango MS, Kojima Y, Aoyi O, Bernardo EC, Matsuda H (2004) Adsorption equilibrium modeling and solution chemistry dependence of fluoride removal from water by trivalent-cation-exchanged zeolite F-9. J Colloid Interface Sci 279:341–350CrossRefGoogle Scholar
  30. Özcan AS, Erdem B, Özcan A (2005) Adsorption of Acid Blue 193 from aqueous solutions onto BTMA-bentonite. Colloids Surfaces A 266:73–81CrossRefGoogle Scholar
  31. Rahman M, Chen Z, Naidu R (2009a) Extraction of arsenic species in soils using microwave-assisted extraction detected by ion chromatography coupled to inductively coupled plasma mass spectrometry. Environ Geochem Health 31:93–102CrossRefGoogle Scholar
  32. Rahman M, Naidu R, Bhattacharya P (2009b) Arsenic contamination in groundwater in the Southeast Asia region. Environ Geochem Health 31:9–21CrossRefGoogle Scholar
  33. Rahman M, Ng J, Naidu R (2009c) Chronic exposure of arsenic via drinking water and its adverse health impacts on humans. Environ Geochem Health 31:189–200CrossRefGoogle Scholar
  34. Rayment GE, Higginson FR (1992) Australian laboratory handbook of soil and water chemical methods. Inkata, MelbourneGoogle Scholar
  35. Ruby MV, Davis A, Link TE, Schoof R, Chaney RL, Freeman GB, Bergstrom P (1993) Development of an in vitro screening test to evaluate the in vivo bioaccessibility of ingested mine-waste lead. Environ Sci Technol 27:2870–2877CrossRefGoogle Scholar
  36. Ruby MV, Davis A, Schoof R, Eberle S, Sellstone CM (1996) Estimation of lead and arsenic bioavailability using a physiologically based extraction test. Environ Sci Technol 30:422–430CrossRefGoogle Scholar
  37. Sarkar D, Makris KC, Vandanapu V, Datta R (2007) Arsenic immobilization in soils amended with drinking-water treatment residuals. Environ Pollut 146:414–419CrossRefGoogle Scholar
  38. Sarkar B, Megharaj M, Xi Y, Krishnamurti GSR, Naidu R (2010a) Sorption of quaternary ammonium compounds in soils: implications to the soil microbial activities. J Hazard Mater 184:448–456CrossRefGoogle Scholar
  39. Sarkar B, Xi Y, Megharaj M, Krishnamurti GSR, Naidu R (2010b) Synthesis and characterisation of novel organopalygorskites for removal of p-nitrophenol from aqueous solution: isothermal studies. J Colloid Interface Sci 350:295–304CrossRefGoogle Scholar
  40. Sarkar B, Xi Y, Megharaj M, Krishnamurti GSR, Rajarathnam D, Naidu R (2010c) Remediation of hexavalent chromium through adsorption by bentonite based Arquad® 2HT-75 organoclays. J Hazard Mater 183:87–97CrossRefGoogle Scholar
  41. Sarkar B, Megharaj M, Xi Y, Naidu R (2011a) Structural characterisation of Arquad® 2HT-75 organobentonites: surface charge characteristics and environmental application. J Hazard Mater 195:155–161CrossRefGoogle Scholar
  42. Sarkar B, Xi Y, Megharaj M, Naidu R (2011b) Orange II adsorption on palygorskites modified with alkyl trimethylammonium and dialkyl dimethylammonium bromide—an isothermal and kinetic study. Appl Clay Sci 51:370–374CrossRefGoogle Scholar
  43. Sarkar B, Megharaj M, Xi Y, Naidu R (2012a) Surface charge characteristics of organo-palygorskites and adsorption of p-nitrophenol in flow-through reactor system. Chem Eng J 185–186:35–43Google Scholar
  44. Sarkar B, Xi Y, Megharaj M, Krishnamurti GSR, Bowman M, Rose H, Naidu R (2012b) Bio-reactive organoclay: a new technology for environmental remediation. Crit Rev Environ Sci Technol 42(5):435–488CrossRefGoogle Scholar
  45. Smith E, Naidu R, Alston AM (1998) Arsenic in the soil environment: a review. In: Donald LS (ed) Adv Agron 64:149–195Google Scholar
  46. Tamaki S, Frankenberger WT Jr (1992) Environmental biochemistry of arsenic. Rev Environ Contam Toxicol 124:79–110CrossRefGoogle Scholar
  47. WHO (2001) Arsenic in Drinking Water, WHO Fact Sheet No. 210. Avaialble from: http://www.who.int/mediacentre/factsheets/fs210/en/
  48. Xi Y, Ding Z, He H, Frost RL (2004) Structure of organoclays—an X-ray diffraction and thermogravimetric analysis study. J Colloid Interface Sci 277:116–120CrossRefGoogle Scholar
  49. Xi Y, Frost RL, He H (2007) Modification of the surfaces of Wyoming montmorillonite by the cationic surfactants alkyl trimethyl, dialkyl dimethyl, and trialkyl methyl ammonium bromides. J Colloid Interface Sci 305:150–158CrossRefGoogle Scholar
  50. Zhang M, Wang Y, Zhao D, Pan G (2010) Immobilization of arsenic in soils by stabilized nanoscale zero-valent iron, iron sulfide (FeS), and magnetite (Fe3O4) particles. Chin Sci Bull 55:365–372CrossRefGoogle Scholar
  51. Zhu J, He H, Guo J, Yang D, Xie X (2003) Arrangement models of alkylammonium cations in the interlayer of HDTMA+ pillared montmorillonites. Chin Sci Bull 48:368–372Google Scholar

Copyright information

© Springer-Verlag 2012

Authors and Affiliations

  • Binoy Sarkar
    • 1
    • 2
  • Ravi Naidu
    • 1
    • 2
    Email author
  • Mohammad Mahmudur Rahman
    • 1
    • 2
  • Mallavarapu Megharaj
    • 1
    • 2
  • Yunfei Xi
    • 1
    • 2
  1. 1.CERAR-Centre for Environmental Risk Assessment and Remediation, Building XUniversity of South AustraliaMawson LakesAustralia
  2. 2.CRC CARE-Cooperative Research Centre for Contamination Assessment and Remediation of the Environment, Building XUniversity of South AustraliaMawson LakesAustralia

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