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Fluoride sorption and desorption on soils located in the surroundings of an aluminium smelter in Galicia (NW Spain)

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Abstract

Aluminium smelters are major sources of F emission to the environment. We studied, in laboratory experiments, the sorption and desorption of fluoride on organic and mineral horizons of soils located within 2 km from one of these factories, situated in the northern coast of Galicia (NW Spain). The soils, developed from granite, are acid (pH H2O 3.9–5.5), rich in organic matter (4–16 % C in the A horizon) and most A horizons have high Al saturation in the exchange complex. All samples showed a notable F sorption, between 1,066 and 1,589 mg kg−1, after adding 200 mg F L−1, which accounts for 53–80 % of F added. The sorption was slightly higher in the A horizons than in the respective organic horizons (differences of up to 194 mg kg−1). The fluoride sorption upon addition of 200 mg F L−1 correlated significantly (p < 0.05) with soil pH in water (r = −0.77), iron extracted by acid ammonium oxalate (r = 0.68), aluminium plus iron extracted by acid ammonium oxalate (r = 0.63), exchange aluminium (r = 0.52) and clay percentage in soil (r = 0.76). The F sorption fitted to both Langmuir and Freundlich models. Desorbed F accounted for only 12–22 % of sorbed fluoride and correlated (p < 0.05) negatively with non-crystalline (extracted by acid ammonium oxalate) Fe (r = −0.51) and clay content (r = −0.74) and positively with organic matter (r = 0.69) and with the effective cation exchange capacity of the soil (r = 0.50).

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References

  • Álvarez E, Romar A, Fernández-Marcos ML (2013) Fluorine immission to soil and its influence on aluminium dynamics in the vicinity of an aluminium smelter in Galicia (NW Spain). J Soils Sediment 131:72–81

    Article  Google Scholar 

  • Ando M, Tadano M, Asanuma S, Tamura K, Matsushima S, Watanabe T, Kondo T, Sakurai S, Ji R, Liang C, Cao S (1998) Health effects of indoor fluoride pollution from coal burning in China. Environ Health Perspect 106:239–244

    Article  Google Scholar 

  • Arnesen AKM (1997) Availability of fluoride to plants grown in contaminated soils. Plant Soil 191:13–25

    Article  Google Scholar 

  • Arnesen AKM, Krogstad T (1998) Sorption and desorption of fluoride in soil polluted from the aluminium smelter at Årdal in Western Norway. Water Air Soil Pollut 103:357–373

    Article  Google Scholar 

  • Arnesen AKM, Abrahamsen G, Sandvik G, Krogstad T (1995) Aluminium-smelters and fluoride pollution of soil and soil solution in Norway. Sci Total Environ 163:39–53

    Article  Google Scholar 

  • Bar-Yosef B, Afik I, Rosenberg R (1988) Fluoride sorption by montmorillonite and kaolinite. Soil Sci 145:194–200

    Article  Google Scholar 

  • Bhatnagar A, Kumar E, Sillanpää M (2011) Fluoride removal from water by adsorption—a review. Chem Eng J 171:811–840

    Article  Google Scholar 

  • Bower CA, Hatcher JT (1967) Adsorption of fluoride by soils and minerals. Soil Sci 103:151–154

    Article  Google Scholar 

  • Chang CC, Huang YH, Chen HT (2010) Adsorption thermodynamic and kinetic studies of fluoride aqueous solution treated with waste iron oxide. Sep Sci Technol 45:370–379

    Article  Google Scholar 

  • Cronin SJ, Manoharan V, Hedley MJ, Loganathan P (2000) Fluoride: review of its fate, bioavailability and risks of fluorosis in grazed-Pasture systems in New Zealand. N Z J Agric Res 43:295–321

    Article  Google Scholar 

  • Cronin SJ, Neall VE, Lecointre JA, Hedley MJ, Loganathan P (2003) Environmental hazards of fluoride in volcanic ash: a case study from Ruapehu volcano. N Z J Volcanol Geotherm Res 121:271–291

    Article  Google Scholar 

  • D’Alessandro W, Bellomo S, Parello F (2012) Fluorine adsorption by volcanic soils at Mt. Etna, Italy. Appl Geochem 27:1179–1188

    Article  Google Scholar 

  • Dang D, Ding W, Cheng A, Liu S, Zhang X (2011) Isotherm equation study of F adsorbed from water solution by Fe-2(SO4)(3)-modified granular activated alumina. Chin J Chem Eng 19:581–585

    Article  Google Scholar 

  • Farrah H, Slavek J, Pickering WF (1987) Fluoride interactions with hydrous aluminum-oxides and alumina. Aust J Soil Res 25:55–69

    Article  Google Scholar 

  • Fluhler H, Polomski J, Blaser P (1982) Retention and movement of fluoride in soils. J Environ Qual 11:461–468

    Article  Google Scholar 

  • Gago C, Fernández-Marcos ML, Alvarez E (2002) Aqueous aluminium species in forest soils affected by fluoride emissions from an aluminium smelter in NW Spain. Fluoride 35:110–121

    Google Scholar 

  • Gago C, Romar A, Fernández-Marcos ML, Álvarez E (2012) Fluorine sorption by soils developed from various parent materials in Galicia (NW Spain). J Colloid Interf Sci 374:232–236

    Article  Google Scholar 

  • Gong WX, Qu JH, Liu RP, Lan HC (2012) Adsorption of fluoride onto different types of aluminas. Chem Eng J 189:126–133

    Article  Google Scholar 

  • Haidouti C, Chronopoulou A, Chronopoulos J (1993) Effects of fluoride emissions from industry on the fluoride concentration of soils and vegetation. Biochem Syst Ecol 21:195–208

    Article  Google Scholar 

  • Harrington LF, Cooper EM, Vasudevan D (2003) Fluoride sorption and associated aluminum release in variable charge soils. J Colloid Interface Sci 267:302–313

    Article  Google Scholar 

  • Höflich BLW, Weinbruch S, Theissmann R, Gorzawski H, Ebert M, Ortner HM, Skogstad A, Ellingsen DG, Drabløs PA, Thomassen Y (2005) Characterization of individual aerosol particles in workroom air of aluminium smelter potrooms. J Environ Monit 7:419–424

    Article  Google Scholar 

  • Huang PM, Jackson ML (1965) Mechanism of reaction of neutral fluoride solution with layer silicates and oxides of soils. Soil Sci Soc Am Proc 29:661–665

    Article  Google Scholar 

  • Huang YH, Shih YJ, Chang CC (2011) Adsorption of fluoride by waste iron oxide: the effects of solution pH, major coexisting anions, and adsorbent calcination temperature. J Hazard Mater 186:1355–1359

    Article  Google Scholar 

  • Hufschmid J, Beveridge I, Coulson G, Gould J (2011) Bone fluoride concentrations of eastern grey kangaroos (Macropus giganteus) resident near an aluminium smelter in south-eastern Australia. Ecotoxicology 20:1378–1387

    Article  Google Scholar 

  • IUSS Working Group WRB (2006) Word reference base for soil resources 2006. Word Soil Resources Reports No. 103 FAO, Rome

  • Jimenez-Becerril J, Solache-Rios M, Garcia-Sosa I (2012) Fluoride removal from aqueous solutions by boehmite. Water Air Soil Pollut 223:1073–1078

    Article  Google Scholar 

  • Kau PMH, Smith DW, Binning P (1997) Fluoride retention by kaolin clay. J Contam Hydrol 28:267–288

    Article  Google Scholar 

  • Kau PMH, Smith DW, Binning P (1998) Experimental sorption of fluoride by kaolinite and bentonite. Geoderma 84:89–108

    Article  Google Scholar 

  • Kaufhold S, Dohrmann R, Abidin Z, Henmi T, Matsue N, Eichinger L, Kaufhold A, Jahn R (2010) Allophane compared with other sorbent minerals for the removal of fluoride from water with particular focus on a mineable Ecuadorian allophane. Appl Clay Sci 50:25–33

    Article  Google Scholar 

  • Khare N, Hesterberg D, Martin JD (2005) XANES investigation of phosphate sorption in single and binary systems of iron and aluminum oxide minerals. Environ Sci Technol 39:2152–2160

    Article  Google Scholar 

  • Kooner ZS, Jardine PM, Feldman S (1995) Competitive surface complexation reactions of sulfate and natural organic carbon on soil. J Environ Qual 24:656–662

    Article  Google Scholar 

  • Kumar P, Rani M (2011) Impact of fluoride on flora in and around Hindalco Industries Ltd., Renukoot (India). J Appl Environ Biol Sci 1:81–83

    Google Scholar 

  • L’vov BV, Polzik LK, Weinbruch S, Ellingsen DG, Thomassen Y (2005) Theoretical aspects of fluoride air contaminant formation in aluminium smelter potrooms. J Environ Monit 7:425–430

    Article  Google Scholar 

  • Larsen S, Widdowson AE (1971) Soil fluorine. J Soil Sci 22:210–221

    Article  Google Scholar 

  • Loganathan P, Gray CW, Hedley MJ, Roberts AHC (2006) Total and soluble fluorine concentrations in relation to properties of soils in New Zealand. Eur J Soil Sci 57:411–421

    Article  Google Scholar 

  • Loganathan P, Vigneswaran S, Kandasamy J, Naidu R (2013) Defluoridation of drinking water using adsorption processes. J Hazard Mater 248:1–19

    Article  Google Scholar 

  • Maiti A, Basu JK, De S (2011) Chemical treated laterite as promising fluoride adsorbent for aqueous system and kinetic modeling. Desalination 265:28–36

    Article  Google Scholar 

  • Monterroso C, Fernández-Marcos ML, Alvarez E (1996) Factors influencing phosphorus adsorption in mine soils in Galicia, Spain. Sci Total Environ 180:137–145

    Article  Google Scholar 

  • Omueti JAI, Jones RL (1977) Fluoride adsorption by Illinois soils. J Soil Sci 28:564–572

    Article  Google Scholar 

  • Peek DC, Volk VV (1985) Fluoride sorption and desorption in soils. Soil Sci Soc Am J 49:583–586

    Article  Google Scholar 

  • Romar A, Gago C, Fernandez-Marcos ML, Álvarez E (2009) Influence of fluoride addition on the composition of solutions in equilibrium with acid soils. Pedosphere 19:60–70

    Article  Google Scholar 

  • Simard RE, Lafrance P (1996) Fluoride sorption and desorption indices in Quebec soils. Commun Soil Sci Plan 27:853–866

    Article  Google Scholar 

  • Skopp J (2009) Derivation of the Freundlich adsorption isotherm from kinetics. J Chem Educ 86:1341–1343

    Article  Google Scholar 

  • Sujana MG, Soma G, Vasumathi N, Anand S (2009) Studies on fluoride adsorption capacities of amorphous Fe/Al mixed hydroxides from aqueous solutions. J Fluor Chem 130:749–754

    Article  Google Scholar 

  • Tang Y, Guan X, Wang J, Gao N, McPhail MR, Chusuei CC (2009) Fluoride adsorption onto granular ferric hydroxide: effects of ionic strength, pH, surface loading, and major co-existing anions. J Hazard Mater 171:774–779

    Article  Google Scholar 

  • Thonstad J, Fellner P, Haarberg GM, Hives J, Kvande H, Sterten A (2001) Aluminium electrolysis. Aluminium-Verlag, Düsseldorf

    Google Scholar 

  • Totsche KU, Wilcke W, Orber M, Zech W (2000) Evaluation of fluoride-induced metal mobilization in soil columns. J Environ Qual 29:454–459

    Article  Google Scholar 

  • Valdivieso AL, Bahena JLR, Song S, Urbina RH (2006) Temperature effect on the zeta potential and fluoride adsorption at the α-Al2O3/aqueous solution interface. J Colloid Interface Sci 298:1–5

    Article  Google Scholar 

  • Vikas C, Kushwaha R, Ahmad W, Prasannakumar V, Reghunath R (2013) Genesis and geochemistry of high fluoride bearing groundwater from a semi-arid terrain of NW India. Environ Earth Sci 68:289–305

    Article  Google Scholar 

  • Vike E (2005) Uptake, deposition and wash off of fluoride and aluminium in plant foliage in the vicinity of an aluminium smelter in Norway. Water Air Soil Pollut 160:145–159

    Article  Google Scholar 

  • Vike E, Habjørg A (1995) Variation in fluoride content and leaf injury on plants associated with three aluminium smelters in Norway. Sci Total Environ 163:25–35

    Article  Google Scholar 

  • Vikøren T, Stuve G (1996) Fluoride exposure in cervids inhabiting areas adjacent to aluminum smelters in Norway. II. Fluorosis. J Wildl Dis 32:181–189

    Article  Google Scholar 

  • Wang YX, Reardon EJ (2001) Activation and regeneration of a soil sorbent for defluoridation of drinking water. Appl Geochem 16:531–539

    Article  Google Scholar 

  • Wei S, Xiang W (2012) Surface properties and adsorption characteristics for fluoride of kaolinite, ferrihydrite and kaolinite–ferrihydrite association. J Food Agric Environ 10:923–929

    Google Scholar 

  • Wenzel WW, Blum WEH (1992) Fluorine speciation and mobility in F-contaminated soils. Soil Sci 153:357–364

    Article  Google Scholar 

  • Young SM, Pitawala A, Ishiga H (2011) Factors controlling fluoride contents of groundwater in north-central and northwestern Sri Lanka. Environ Earth Sci 63:1333–1342

    Article  Google Scholar 

  • Zhu MX, Xie M, Jiang X (2006) Interaction of fluoride with hydroxyaluminum–montmorillonite complexes and implications for fluoride-contaminated acidic soils. Appl Geochem 21:675–683

    Article  Google Scholar 

  • Zhu MX, Ding KY, Jiang X, Wang HH (2007) Investigation on co-sorption and desorption of fluoride and phosphate in a red soil of China. Water Air Soil Pollut 183:455–465

    Article  Google Scholar 

Download references

Acknowledgments

The research was supported by the Government of Spain.

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Gago, C., Romar, A., Fernández-Marcos, M.L. et al. Fluoride sorption and desorption on soils located in the surroundings of an aluminium smelter in Galicia (NW Spain). Environ Earth Sci 72, 4105–4114 (2014). https://doi.org/10.1007/s12665-014-3304-8

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