A method to determine silver partitioning and lability in soils
Lara Settimio A C , Mike J. McLaughlin A B , Jason K. Kirby B and Kate A. Langdon BA Waite Research Institute, School of Agriculture, Food and Wine, University of Adelaide, Adelaide, Waite Road, SA 5064, Australia.
B CSIRO Land and Water, Contaminant Chemistry and Ecotoxicology program, Minerals Down Under Flagship, Waite Campus, Waite Road, Adelaide, SA 5064, Australia.
C Corresponding author. Email: lara.settimo@adelaide.edu.au
Environmental Chemistry 11(1) 63-71 https://doi.org/10.1071/EN13163
Submitted: 28 August 2013 Accepted: 3 December 2013 Published: 21 February 2014
Environmental context. Soils contaminated with silver can have detrimental environmental effects because of silver’s toxicity to a range of soil-dwelling organisms. The total concentration of silver in soil, however, is often not a good indicator of potential toxicity as it does not account for variations in bioavailability. We report a method for soil analysis that measures the amount of silver available for uptake by soil-dwelling organisms, and hence could provide data that better reflect potential toxicity.
Abstract. There is increasing potential for pollution of soils by silver because of an increased use of this metal in consumer and industrial products. Silver may undergo reactions with soil components that mitigate its availability and potential toxicity, so that the total concentration of this metal in soil is not a useful indicator of potential risk. We developed an isotopic dilution method to simultaneously measure the partitioning (Kd-value) and lability (E-value) of Ag in soils, using the 110mAg isotope. An equilibration solution containing 10 mM Ca(NO3)2 was used along with a cation exchange resin to correct for possible interferences from non-isotopically exchangeable Ag associated with soil colloids in suspension (Er-value). The quantification limits for Kd and Er will depend on the amounts of radioisotope spiked and daily detection limits of inductively coupled plasma-mass spectrometry instrumentation but are typically >4000 L kg–1 and <0.92 mg kg–1. Measurement of Kd values for Ag in a range of soils indicated strong partitioning to the solid phase is positively associated with soil cation-exchange capacity or total organic carbon and pH. The concentrations of labile Ag in soils geogenically enriched in Ag were not detectable indicating occlusion of the Ag within poorly soluble solid phases. Measurement of labile Ag in soils spiked with a soluble Ag salt and aged for 2 weeks indicated rapid conversion of soluble Ag into non-isotopically exchangeable forms, either irreversibly adsorbed or precipitated in the soil. These results indicate that measurement of labile Ag will be important to estimate toxicity risks to soil organisms or to predict bioaccumulation through the food chain.
Additional keywords: E-value, isotope dilution, Kd, partition coefficient.
References
[1] R. Eisler, Silver hazards to fish, wildlife, and invertebrates: a synoptic review, in Contaminant Hazard Reviews 1997, pp. 2–5 (US Department of the Interior: Washington, DC).[2] I. C. Smith, B. L. Carson, Volume 2: Silver, in Trace Metals in the Environment 1977, p. 204 (Ann Arbor Science Publishers: Ann Arbor, MI).
[3] Silver Uses 2011 (The Silver Institute). Available at http://www.silverinstitute.org/silver_uses.php [Verified 29 May 2011].
[4] J. R. Morones, J. L. Elechiguerra, A. Camacho, K. Holt, J. B. Kouri, J. T. Ramírez, M. J. Yacaman, The bactericidal effect of silver nanoparticles. Nanotechnology 2005, 16, 2346.
| The bactericidal effect of silver nanoparticles.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXht1CiurjJ&md5=4c2b48daa4c25552131adb6c4d84b36eCAS | 20818017PubMed |
[5] T. Benn, B. Cavanagh, K. Hristovski, J. D. Posner, P. Westerhoff, The release of nanosilver from consumer products used in the home. J. Environ. Qual. 2010, 39, 1875.
| The release of nanosilver from consumer products used in the home.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXhsVKlu7zO&md5=665579b3e77d38985564355f31a44340CAS | 21284285PubMed |
[6] C. L. Doolette, M. J. McLaughlin, J. K. Kirby, D. J. Batstone, H. H. Harris, H. Q. Ge, G. Cornelis, Transformation of PVP coated silver nanoparticles in a simulated wastewater treatment process and the effect on microbial communities. Chem. Cent. J. 2013, 7, 46.
| Transformation of PVP coated silver nanoparticles in a simulated wastewater treatment process and the effect on microbial communities.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3sXpvVKlsrs%3D&md5=f3a87cce8f06c4d2557451407b16abaeCAS | 23497481PubMed |
[7] M. J. Eckelman, T. E. Graedel, Silver emissions and their environmental impacts: a multilevel assessment. Environ. Sci. Technol. 2007, 41, 6283.
| Silver emissions and their environmental impacts: a multilevel assessment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2sXot1ahsr0%3D&md5=9f7da99683e892561f9ba63c9181397cCAS | 17937316PubMed |
[8] J. Johnson, J. Jirikowic, M. Bertram, D. Van Beers, R. B. Gordon, K. Henderson, R. J. Klee, T. Lanzano, R. Lifset, L. Oetjen, T. E. Graedel, Contemporary anthropogenic silver cycle: a multilevel analysis. Environ. Sci. Technol. 2005, 39, 4655.
| Contemporary anthropogenic silver cycle: a multilevel analysis.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXjvFKjsrc%3D&md5=1646ddb9d6bd62d7795d6d7fcbef8c78CAS | 16047806PubMed |
[9] H. G. Petering, C. J. McClain, Silver, in Metals and Their Compounds in the Environment: Occurrence, Analysis and Biological Relevance (Ed. E. Merian) 1991, pp. 1191–1202 (VCH: Weinham, Germany).
[10] B. Elvers, S. Hawkins, W. Russey, G. Schulz, Silver, silver compounds and silver alloys, in Ullmann’s Encyclopedia of Industrial Chemistry (Ed. H. Renner) 1993, pp. 1–77 (VCH: Weinham, Germany).
[11] I. W. Oliver, M. J. McLaughlin, G. Merrington, Temporal trends of total and potentially available element concentrations in sewage biosolids: a comparison of biosolid surveys conducted 18 years apart. Sci. Total Environ. 2005, 337, 139.
| Temporal trends of total and potentially available element concentrations in sewage biosolids: a comparison of biosolid surveys conducted 18 years apart.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXktFOr&md5=1839f0d8dd79ce49796c30259b50d165CAS | 15626385PubMed |
[12] H. T. Ratte, Bioaccumulation and toxicity of silver compounds: a review. Environ. Toxicol. Chem. 1999, 18, 89.
| Bioaccumulation and toxicity of silver compounds: a review.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXkt1Or&md5=3d5a7fbb056a3de8b9b7c5de7810058cCAS |
[13] J. Y. Roh, S. J. Sim, J. Yi, K. Park, K. H. Chung, D. Y. Ryu, J. Choi, Ecotoxicity of silver nanoparticles on the soil nematode Caenorhabditis elegans using functional ecotoxicogenomics. Environ. Sci. Technol. 2009, 43, 3933.
| Ecotoxicity of silver nanoparticles on the soil nematode Caenorhabditis elegans using functional ecotoxicogenomics.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXkvVSktLs%3D&md5=e233e9535dcd28e8b0395413a44ea842CAS | 19544910PubMed |
[14] F. P. C. Blamey, P. M. Kopittke, J. B. Wehr, T. B. Kinraide, N. W. Menzies, Rhizotoxic effects of silver in cowpea seedlings. Environ. Toxicol. Chem. 2010, 29, 2072.
| Rhizotoxic effects of silver in cowpea seedlings.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3cXht12jsL3L&md5=457626e3547e42a05ba115f8104115ffCAS |
[15] I. N. Throbäck, M. Johansson, M. Rosenquist, M. Pell, M. Hansson, S. Hallin, Silver (Ag+) reduces denitrification and induces enrichment of novel Nir-k genotypes in soil. FEMS Microbiol. Lett. 2007, 270, 189.
| Silver (Ag+) reduces denitrification and induces enrichment of novel Nir-k genotypes in soil.Crossref | GoogleScholarGoogle Scholar | 17250758PubMed |
[16] T. Murata, M. Kanao-Koshikawa, T. Takamatsu, Effects of Pb, Cu, Sb, In and Ag contamination on the proliferation of soil bacterial colonies, soil dehydrogenase activity, and phospholipid fatty acid profiles of soil microbial communities. Water Air Soil Pollut. 2005, 164, 103.
| Effects of Pb, Cu, Sb, In and Ag contamination on the proliferation of soil bacterial colonies, soil dehydrogenase activity, and phospholipid fatty acid profiles of soil microbial communities.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXmvFOksrw%3D&md5=d7d646269d79a35ac23110624dfb16b7CAS |
[17] S. Sauvé, W. Hendershot, H. E. Allen, Solid-solution partitioning of metals in contaminated soils: dependence on pH, total metal burden, and organic matter. Environ. Sci. Technol. 2000, 34, 1125.
| Solid-solution partitioning of metals in contaminated soils: dependence on pH, total metal burden, and organic matter.Crossref | GoogleScholarGoogle Scholar |
[18] G. Cornelis, J. K. Kirby, D. Beak, D. Chittleborough, M. J. McLaughlin, A method for determination of retention of silver and cerium oxide manufactured nanoparticles in soils. Environ. Chem. 2010, 7, 298.
| A method for determination of retention of silver and cerium oxide manufactured nanoparticles in soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC3MXhtFOnsrw%3D&md5=d2dca43d470834db8ab85d37c7384b3bCAS |
[19] J. D. Allison, T. L. Allison, Partition coefficients for metals in surface water, soil and waste. EPA/600/R-05/074 2005, (US Environmental Protection Agency: Washington, DC).
[20] L. J. Evans, S. J. Barabash, Molybdenum, silver, thallium and vanadium, in Trace Elements in Soils (Ed. P. S. Hooda) 2010, pp. 516–49 (Blackwell Publishing Ltd: Wiltshire).
[21] K. Lock, C. R. Janssen, Influence of aging on metal availability in soils, in Reviews of Environmental Contamination and Toxicology, Vol 178 (Ed. G. W. Ware) 2003, pp. 1–21 (Springer: New York).
[22] S. D. Young, H. Zhang, A. M. Tye, A. Maxted, C. Thums, I. Thornton, Characterizing the availability of metals in contaminated soils. I. The solid phase: sequential extraction and isotopic dilution. Soil Use Manage. 2005, 21, 450.
| Characterizing the availability of metals in contaminated soils. I. The solid phase: sequential extraction and isotopic dilution.Crossref | GoogleScholarGoogle Scholar |
[23] H. Zhang, S. D. Young, Characterizing the availability of metals in contaminated soils. II. The soil solution. Soil Use Manage. 2005, 21, 459.
| Characterizing the availability of metals in contaminated soils. II. The soil solution.Crossref | GoogleScholarGoogle Scholar |
[24] A. L. Nolan, Y. B. Ma, E. Lombi, M. J. McLaughlin, Measurement of labile Cu in soil using stable isotope dilution and isotope ratio analysis by ICP-MS. Anal. Bioanal. Chem. 2004, 380, 789.
| Measurement of labile Cu in soil using stable isotope dilution and isotope ratio analysis by ICP-MS.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2cXhtVarsr3I&md5=dbdc43c60a159352ff975f5ed9bbab50CAS | 15517206PubMed |
[25] L. A. Wendling, Y. B. Ma, J. K. Kirby, M. J. McLaughlin, A predictive model of the effects of aging on cobalt fate and behavior in soil. Environ. Sci. Technol. 2009, 43, 135.
| A predictive model of the effects of aging on cobalt fate and behavior in soil.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1cXhtl2ltb7E&md5=3d8593a6392aa3a570676c7564413f80CAS | 19209596PubMed |
[26] J. K. Kirby, M. J. McLaughlin, Y. B. Ma, B. Ajiboye, Aging effects on molybdate lability in soils. Chemosphere 2012, 89, 876.
| Aging effects on molybdate lability in soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC38XoslGqsrk%3D&md5=d4b1e8f94fae5f95915cb44a2c561e4cCAS | 22704209PubMed |
[27] S. D. Young, N. M. J. Crout, J. Hutchinson, A. Tye, S. Tandy, L. Nakhone, Techniques for measuring attenuation: isotopic dilution methods, in In Natural Attenuation of Trace Element Availability in Soils 2005, pp. 19–37 (Society of Environmental Toxicology and Chemistry (SETAC): Pensacola, FL).
[28] R. E. Hamon, D. R. Parker, E. Lombi, Advances in isotopic dilution techniques in trace element research: a review of methodologies, benefits and limitations. Adv. Agron. 2008, 99, 289.
| Advances in isotopic dilution techniques in trace element research: a review of methodologies, benefits and limitations.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD1MXhslWjsr0%3D&md5=aeb25b675e7d479d5105ea0135ef7a99CAS |
[29] R. E. Hamon, I. Bertrand, M. J. McLaughlin, Use and abuse of isotopic exchange data in soil chemistry. Aust. J. Soil Res. 2002, 40, 1371.
| Use and abuse of isotopic exchange data in soil chemistry.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXlvFeisA%3D%3D&md5=a2335fd5c2d0289139864b888b130ceaCAS |
[30] R. E. Hamon, E. Lombi, P. Fortunati, A. L. Nolan, M. J. McLaughlin, Coupling speciation and isotope dilution techniques to study arsenic mobilization in the environment. Environ. Sci. Technol. 2004, 38, 1794.
| Coupling speciation and isotope dilution techniques to study arsenic mobilization in the environment.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2cXht1Wis7s%3D&md5=b9c61ce59f7859c73ee88c02dccdd7c0CAS | 15074691PubMed |
[31] L. A. Wendling, J. K. Kirby, M. J. McLaughlin, A novel technique to determine cobalt exchangeability in soils using isotope dilution. Environ. Sci. Technol. 2008, 42, 140.
| A novel technique to determine cobalt exchangeability in soils using isotope dilution.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2sXhtlaktbrI&md5=7f617c14f6d3e7fdb7edd64bf4e06647CAS | 18350888PubMed |
[32] E. Lombi, R. E. Hamon, S. P. McGrath, M. J. McLaughlin, Lability of Cd, Cu, and Zn in polluted soils treated with lime, beringite, and red mud and identification of a non-labile colloidal fraction of metals using isotopic techniques. Environ. Sci. Technol. 2003, 37, 979.
| Lability of Cd, Cu, and Zn in polluted soils treated with lime, beringite, and red mud and identification of a non-labile colloidal fraction of metals using isotopic techniques.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXosVWgtg%3D%3D&md5=28c89196f94c22ce8d328a07efb8c1a5CAS | 12666929PubMed |
[33] G. W. Gee, J. W. Bauder, Particle size analysis, in Methods of soil analysis. Part 1. Physical and mineralogical methods 1986, pp. 383–411 (American Society of Agronomy Inc. and Soil Science Society of America Inc.: Madison, WI).
[34] G. E. Rayment, F. R. Higginson, Australian Laboratory Handbook of Soil and Water Chemical Methods 1992 (Inkata Press: Melbourne).
[35] T. J. Marshall, J. W. Holmes, C. W. Rose, Soil Physics 1979 (Cambridge University Press: Cambridge, UK).
[36] L. R. Rodríguez Barquero, J. M. Los Arcos, Study of the stability problems of 110mAg samples in several commercial liquid scintillators. Appl. Radiat. Isot. 2000, 52, 679.
| Study of the stability problems of 110mAg samples in several commercial liquid scintillators.Crossref | GoogleScholarGoogle Scholar |
[37] E. Smolders, K. Brans, A. Foldi, R. Merckx, Cadmium fixation in soils measured by isotopic dilution. Soil Sci. Soc. Am. J. 1999, 63, 78.
| Cadmium fixation in soils measured by isotopic dilution.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXitFGgsb8%3D&md5=28a1fbf366eb37c5b3dab4e2fe8aa7e3CAS |
[38] S. D. Young, A. Tye, A. Carstensen, L. Resende, N. Crout, Methods for determining labile cadmium and zinc in soil. Eur. J. Soil Sci. 2000, 51, 129.
| Methods for determining labile cadmium and zinc in soil.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3cXisVKmsb0%3D&md5=0bbe8f1e0e696f858eee8491f18bb3bfCAS |
[39] J. Gustafsson, Visual Minteq, Version: 3.0 2010 (KTH Royal Institute of Technology: Stockholm, Sweden). Available at http://www2.lwr.kth.se/English/OurSoftware/vminteq/ [Verified 7 February 2014].
[40] G. Cornelis, C. Doolette, M. Thomas, M. J. McLaughlin, J. K. Kirby, D. G. Beak, D. Chittleboroug, Retention and dissolution of engineered silver nanoparticles in natural soils. Soil Sci. Soc. Am. J. 2012, 76, 891.
| Retention and dissolution of engineered silver nanoparticles in natural soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BC38XosFejur0%3D&md5=fc4482ad314a7eac6744f5f27411d0c6CAS |
[41] D. S. Smith, R. A. Bell, J. R. Kramer, Metal speciation in natural waters with emphasis on reduced sulfur groups as strong metal binding sites. Comp. Biochem. Physiol. C: Pharmacol. Toxicol 2002, 133, 65.
| Metal speciation in natural waters with emphasis on reduced sulfur groups as strong metal binding sites.Crossref | GoogleScholarGoogle Scholar |
[42] J. R. Kramer, R. A. Bell, D. S. Smith, Determination of sulfide ligands and association with natural organic matter. Appl. Geochem. 2007, 22, 1606.
| Determination of sulfide ligands and association with natural organic matter.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2sXpt1yls74%3D&md5=2147babe9913b78475b919dc9e1bbddaCAS |
[43] N. W. H. Adams, J. R. Kramer, Silver speciation in wastewater effluent, surface waters, and pore waters. Environ. Toxicol. Chem. 1999, 18, 2667.
| Silver speciation in wastewater effluent, surface waters, and pore waters.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaK1MXns1GlsL8%3D&md5=6499af5799b870255728a065b248c84aCAS |
[44] F. N. Ponnamperuma, E. M. Tianco, T. A. Loy, Ionic strengths of the solutions of flooded soils and other natural aqueous solutions from specific conductance. Soil Sci. 1966, 102, 408.
| Ionic strengths of the solutions of flooded soils and other natural aqueous solutions from specific conductance.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaF2sXhtVCgtLk%3D&md5=5eeb3fc33795a7715203c55a0576d2c7CAS |
[45] S. Larsen, A. E. Widdowson, Chemical composition of soil solution. J. Sci. Food Agric. 1968, 19, 693.
| Chemical composition of soil solution.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaF1MXls1Onsw%3D%3D&md5=c8b61050fbcc5785a76b901d6c437a05CAS |
[46] G. P. Gillman, L. C. Bell, Soil solution studies on weathered soils from tropical north Queensland. Aust. J. Soil Res. 1978, 16, 67.
| Soil solution studies on weathered soils from tropical north Queensland.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaE1cXksFyqsb0%3D&md5=c79eca00a855eddb90ee2b143aaf206aCAS |
[47] P. de Caritat, C. Reimann, Comparing results from two continental geochemical surveys to world soil composition and deriving Predicted Empirical Global Soil (PEGS2) reference values. Earth Planet. Sci. Lett. 2012, 319–320, 269.
| Comparing results from two continental geochemical surveys to world soil composition and deriving Predicted Empirical Global Soil (PEGS2) reference values.Crossref | GoogleScholarGoogle Scholar |
[48] K. C. Jones, B. E. Davies, P. J. Peterson, Silver in Welsh soils – physical and chemical distribution studies. Geoderma 1986, 37, 157.
| Silver in Welsh soils – physical and chemical distribution studies.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DyaL28XhslWqs78%3D&md5=c3225c4f13806802dabf95a5ddc6e3d9CAS |
[49] G. Szabó, J. Guczi, J. Valyon, R. A. Bulman, Investigations of the sorption characteristics of radiosilver on some natural and artificial soil particles. Sci. Total Environ. 1995, 172, 65.
| Investigations of the sorption characteristics of radiosilver on some natural and artificial soil particles.Crossref | GoogleScholarGoogle Scholar |
[50] A. R. Jacobson, M. B. McBride, P. Baveye, T. S. Steenhuis, Environmental factors determining the trace-level sorption of silver and thallium to soils. Sci. Total Environ. 2005, 345, 191.
| Environmental factors determining the trace-level sorption of silver and thallium to soils.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD2MXks1Klurk%3D&md5=5ed5dd6d3dad249c5036fb2788b1699dCAS | 15919539PubMed |
[51] P. Ciffroy, J. M. Garnier, L. Benyahya, Kinetic partitioning of Co, Mn, Cs, Fe, Ag, Zn and Cd in fresh waters (Loire) mixed with brackish waters (Loire estuary): experimental and modelling approaches. Mar. Pollut. Bull. 2003, 46, 626.
| Kinetic partitioning of Co, Mn, Cs, Fe, Ag, Zn and Cd in fresh waters (Loire) mixed with brackish waters (Loire estuary): experimental and modelling approaches.Crossref | GoogleScholarGoogle Scholar | 1:CAS:528:DC%2BD3sXjsVaqtLc%3D&md5=0daa90c5e46a73d20d297628edcd940cCAS | 12735960PubMed |