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Time-dependent surface reactivity of Cd sorbed on calcite, hydroxylapatite and humic acid

Published online by Cambridge University Press:  05 July 2018

E. H. Bailey ,
J. F. W. Mosselmans  and
S. D. Young
E. H. Bailey*
Affiliation:
Environmental Science, School of Bioscience, The University of Nottingham, University Park, Nottingham NG7 2RD, UK
J. F. W. Mosselmans
Affiliation:
CCLRC Daresbury Laboratory, Daresbury, Warrington WA4 4AD, UK
S. D. Young
Affiliation:
Environmental Science, School of Bioscience, The University of Nottingham, University Park, Nottingham NG7 2RD, UK
*
*E-mail: [email protected]
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Abstract

Changes in the lability and local environment of Cd sorbed onto calcite, hydroxylapatite and humic acid have been investigated as a function of time (30 min–9 months) using a combination of X-ray adsorption spectroscopy (XAS) and isotopic dilution techniques with Cd concentrations between 1 and 1000 mmol kg –1. Enhanced X-ray absorption fine structure (EXAFS) shows that precipitation of Cd carbonate was initially observed on calcite. Ageing of a 10 mmol kg–1 sample showed replacement of Cd in the fourth shell with Ca, indicating diffusion between the two phases had occurred. This diffusion appeared to be ongoing for a 10 mmol kg–1 sample even after 9 months of reaction. Only 20% of the Cd in a sample with 10 mmol kg–1 Cd remained labile after 6 months of reaction, suggesting a high degree of incorporation into the solid phase, in agreement with the XAS results. The XAS results for hydroxylapatite indicated that Cd is not fixed in the mineral lattice and Cd lability in a sample loaded with 10 mmol kg–1 Cd was ∼55% after 6 months of reaction. This indicates that a relatively high proportion of the Cd sorbed to hydroxylapatite remained as kinetically active surface species. Little change was observed in the local environment of Cd adsorbed on flocculated Ca-humate samples as a function of time and ∼75% of the Cd remained radio-labile after 6 months of reaction regardless of initial Cd loading. High lability is expected because incorporation into a solid matrix or surface precipitation of a Cd phase is less likely than with the mineral phases.

Keywords

cadmiumXAShydroxylapatitecalcitehumic acid
Type
Research Article
Information
Mineralogical Magazine , Volume 69 , Issue 5 , October 2005 , pp. 563 - 575
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2005

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Footnotes

†

Present address: Diamond Source Ltd., Diamond House, Chilton, Didcot, Oxfordshire OX11 0DE, UK

References

Barrow, N.J. (1987) Reactions with Variable-Charge Soils. Martinus Nijhoff, The Netherlands.CrossRefGoogle Scholar
Binsted, N. (1998) EXCURV98. CCLRC Daresbury Laboratory Computer Program.Google Scholar
Borodin, V.L., Lyutin, V.I., Ilyukhin, V.V. and Belov, N.V. (1979) The isomorphous series calcite-otavite. Doklady Akademii Nauk SSSR, 245, 1099–1101.Google Scholar
Boyanov, M.I., Kelly, S.D., Kemner, K.M., Bunker, B.A., Fein, J.B. and Fowl, D.A. (2003) Adsorption of cadmium to Bacillus subtilis bacterial cell walls: A pH-dependent X-ray absorption fine structure spectroscopy study. Geochimica et Cosmochimica Acta, 67, 3299–3311.CrossRefGoogle Scholar
Collins, C.R., Ragnarsdottir, K.V. and Sherman, D.M. (1999) Effect of inorganic and organic ligands on the mechanism of cadmium sorption to goethite. Geochimica et Cosmochimica Acta, 63, 2989–3002.CrossRefGoogle Scholar
Davis, J.A., Fuller, C.C. and Cook, A.D. (1987) A model for trace metal sorption processes at the calcite surface: Adsorption of Cd2+ and subsequent solid solution formation. Geochimica et Cosmochimica Acta, 51, 1477–1490.CrossRefGoogle Scholar
Da Rocha, N.C.C., De Campos, R.C., Rossi, A.M., Moreira, E.L., Barbosa, A.D.O. and Moure, G.T. (2002) Cadmium uptake by hydroxyapatite synthe-sised in differenct conditions and submitted to thermal treatment. Environmental Science and Technology, 36, 1630–1635.CrossRefGoogle Scholar
Department of Environment, Food and Rural Affairs (DEFRA) and the Environment Agency (2002) Soil Guideline Values for Cadmium Contamination. Environment Agency, Bristol, UK.Google Scholar
Farquhar, M., Vaughan, D., Hughes, C., Charnock, J. and England, K (1997) Experimental studies of the interaction of aqueous metal cations with mineral substrates: Lead, cadmium and copper with perthitic feldspar, muscovite, and biotite. Geochimica et Cosmochimica Acta, 61, 3051–3064.CrossRefGoogle Scholar
Fedoroff, M., Jeanjean, J., Rouchaud, J.C., Mazerolles, L., Trocellier, P., Maireles-Torrws, P. and Jones, D.J. (1999) Sorption kinetics and diffusion of cadmium in calcium hydroxyapatites. Solid State Sciences, 1, 71–84.CrossRefGoogle Scholar
Fletcher, D.A., McMeeking, R.F. and Parkin, D. (1996) The United Kingdom Chemical Database Service. Journal of Chemical Information and Computer Sciences, 36, 746–749.CrossRefGoogle Scholar
Gooddy, D.C., Shand, P., Kinniburgh, D.G. and Van Riemsdijk, W.H. (1995) Field based partition coefficients for trace elements in soil solutions. European Journal of Soil Science, 46, 265—258.CrossRefGoogle Scholar
Hamon, R.E., McLaughlin, M.J., Naidu, R. and Correll, R. (1998) Long-term changes in cadmium bioavailability in soil. Environmental Science and Technology, 32, 3699–3703.CrossRefGoogle Scholar
Hirsch, D., Nir, S. and Banin, A. (1989) Prediction of cadmium complexation in solution and adsorption to montmorillonite. Soil Science Society of America Journal, 53, 716–721.CrossRefGoogle Scholar
Jeanjean, J., Fedoroff, M., Faverjon, F., Vincent, U. and Corset, J. (1995) Influence of pH on the sorption of cadmium ions on calcium hydroxyapatite. Journal of Materials Science, 30, 6156–6160.CrossRefGoogle Scholar
Lanfranco, A.M., Schofield, P.F., Murphy, P.J., Hodson, M.E., Mosselmans, J.F.W. and Valsami-Jones, E. (2003) Characterization and identification of mixed-metal phosphates in soils: the application of Raman spectroscopy. Mineralogical Magazine, 67, 1299–1316.CrossRefGoogle Scholar
Liu, A. and Gonzalez, R.D. (1999) Adsorption/ desorption in a system consisting of humic acid, heavy metals, and clay minerals. Journal of Colloid and Interface Science, 218, 225–232.CrossRefGoogle Scholar
Liu, C., Frenkel, A.I., Vairavamurthy, A. and Huang, P.M. (2001) Sorption of cadmium on humic acid: Mechanistic and kinetic studies with atomic force microscopy and X-ray absorption fine structure spectroscopy. Canadian Journal of Soil Science, 81, 337–348.CrossRefGoogle Scholar
Lorens, R.B. (1981) Sr, Cd, Mn, and Co distribution coefficients in calcite as a function of calcite precipitation rate. Geochimica et Cosmochimica Acta, 45, 553–561.CrossRefGoogle Scholar
Ministry for Agriculture, Fisheries and Food (MAFF) (1993) Code of Good Agricultural Practice for the Protection of Soil. MAFF Publications, London.Google Scholar
Marshall, S.J., Young, S.D. and Gregson, K. (1995) Humic-acid proton equilibria - a comparison of 2 models and assessment of titration error. European Journal of Soil Science, 46, 471–480.CrossRefGoogle Scholar
Martin-Garin, A., Van Cappellen, P. and Charlet, L. (2003) Aqueous cadmium uptake by calcite: A stirred flow-through reactor study. Geochimica et Cosmochimica Acta, 67, 2763–2774.CrossRefGoogle Scholar
McGrellis, S., Serafini, J.-N., Jeanjean, J., Pastol, J.-L. and Fedoroff, M. (2001) Influence of the sorption protocol on the uptake of cadmium ions in calcium hydroxyapatite. Separation and Purification Technology, 24, 129–138.CrossRefGoogle Scholar
Middelburg, J.J. and Comans, R.N.J. (1991) Sorption of cadmium on hydroxyapatite. Chemical Geology, 90, 45–53.CrossRefGoogle Scholar
Mustafa, G., Singh, B. and Kookana, R.S. (2004) Cadmium adsorption and desorption behaviour on goethite at low equilibrium concentrations: effects of pH and index cations. Chemosphere, 57, 1325–1333.CrossRefGoogle ScholarPubMed
Nakhone, L.N. and Young, S.D. (1993) The significance of (radio) labile cadmium pools in soil. Environmental Pollution, 82, 73–77.CrossRefGoogle ScholarPubMed
Parkman, R.H., Charnock, J.M., Bryan, N.D., Livens, F.R. and Vaughan, D.J. (1999) Reactions of copper and cadmium ions in aqueous solution with goethite, lepidocrocite, mackinawite, and pyrite. American Mineralogist, 84, 407–419.CrossRefGoogle Scholar
Randall, S.R., Sherman, D.M. and Ragnarsdottir, K.V. (1998) An extended X-ray absorption fine structure spectroscopy investigation of cadmium sorption on cryptomelane (KMn8O16). Chemical Geology, 151, 95–106.CrossRefGoogle Scholar
Randall, S.R., Sherman, D.M., Ragnarsdottir, K.V. and Collins, C.R. (1999) The mechanism of cadmium surface complexation on iron oxyhydroxide minerals. Geochimica et Cosmochimica Acta, 63, 2971–2987.CrossRefGoogle Scholar
Rieuwerts, J., Thornton, I., Farago, M. and Ashmore, M. (1998) Quantifying the influence of soil properties on the solubility of metals by predictive modelling of secondary data. Chemical Speciation and Bioavailability, 10, 83–94.CrossRefGoogle Scholar
Sery, A., Manceau, A. and Greaves, G.N. (1996) Chemical state of Cd in apatite phosphate ores as determined by EXAFS spectroscopy. American Mineralogist, 81, 864–873.CrossRefGoogle Scholar
Smith, S.R. (1994) Effect of soil-pH on availability to crops of metals in sewage sludge-treated soils. 2. Cadmium uptake by crops and implications for human dietary-intake. Environmental Pollution, 85, 321–327.CrossRefGoogle Scholar
Smolders, E., Brans, K., Foldi, A. and Merkx, R. (1999) Cadmium fixation in soils measured by isotopic dilution. Soil Science Society of America Journal, 63, 78–85.CrossRefGoogle Scholar
Stipp, S.L., Hochella, M.F., Parks, G.A. and Leckie, J.O. (1992) Cd2+ uptake by calcite, solid-state diffusion, and the formation of solid-solution: Interface processes observed with near-surface sensitive techniques (XPS, LEED, and AES). Geochimica et Cosmochimica Acta, 56, 1941–1954.CrossRefGoogle Scholar
Tipping, E. (1994) WHAM - A chemical equilibrium model and computer code for water, sediments and soils incorporating a discrete site/electrostatic model of ion-binding by humic substances. Computers and Geosciences, 20, 973–1023.CrossRefGoogle Scholar
Tipping, E. (1998) Humic ion-binding model VI: An improved description of the interactions of protons and metal ions with humic substances. Aquatic Chemistry, 4, 3–48.Google Scholar
Tye, A.M., Young, S.D., Crout, N.M.J., Zhang, H., Preston, S., Bailey, E.H., Davison, W., McGrath, S.P., Paton, G.I. and Kilham, K. (2002) Predicting arsenic solubility in contaminated soils using isotopic dilution techniques. Environmental Science and Technology, 36, 982–988.CrossRefGoogle ScholarPubMed
Tye, A.M., Young, S.D., Crout, N.M.J., Zhang, H., Preston, S., Barbosa-Jefferson, V.L., Davison, W., McGrath, S.P., Paton, G.I., Kilham, K. and Resende, L. (2003) Predicting the activity of Cd2+ and Zn2+ in soil pore water from the radio-labile metal fraction. Geochimica et Cosmochimica Acta, 67, 375—385.CrossRefGoogle Scholar
Wartchow, R. (1989) Datensammlung nach der “Learnt profile”-Methode(LP) fuer Calcit und Vergleich mit der “Background peak background”-Methode (BPB). Zeitschrift für Kristallographie, 186, 300–302.Google Scholar
Xu, Y., Schwartz, F.W. and Traina, S.J. (1994) Sorption of Zn2+ and Cd2+ on hydroxyapatite surfaces. Environmental Science and Technology, 28, 1472–1480.CrossRefGoogle ScholarPubMed
Yaron, B., Calvet, R. and Prost, R. (1996) Soil Pollution, Processes and Dynamics (chapter 6). Springer-Verlag, Berlin.CrossRefGoogle Scholar
Young, S.D., Tye, A., Carstensen, A., Resende, L. and Crout, N.J.M. (2000) Methods for determining labile cadmium and zinc in soil. European Journal of Soil Science, 51, 129–136.CrossRefGoogle Scholar
Young, S.D., Tye, A. and Crout, N.M.J. (2001) Rates of metal ion fixation in soils determined by isotopic dilution. Proceedings of the 6th International Conference on the Biogeochemistry of Trace Elements, Guelph, Canada, p. 106, ICOBTE.Google Scholar