Abstract
In its soluble ionic forms, lead (Pb) is a toxic element occurring in waters and soils mainly as the result of human activities. The bioavailability of lead ions can be decreased by complexation with various materials in order to decrease their toxicity. Pb chemical immobilization using phosphate addition is a widely accepted technique to immobilize Pb from aqueous solution and contaminated soils. The application of different P amendments cause Pb in soils to shift from forms with high availability to the most strongly bound Pb fractions. The increase of Pb in the residual or insoluble fraction results from formation of pyromorphite Pb5(PO4)3X where X = F, Cl, Br, OH, the most stable environmental Pb compounds under a wide range of pH and Eh natural conditions. Accidental pyromorphite ingestion does not yield bioavailable lead, because pyromorphite is insoluble in the intestinal tract. Numerous natural and synthetic phosphates materials have been used to immobilize Pb: apatite and hydroxyapatite, biological apatite, rock phosphate, soluble phosphate fertilizers such as monoammonium phosphate, diammonium phosphate, phosphoric acid, biosolids rich in P, phosphatic clay and mixtures. The identification of pyromorphite in phosphate amended soils has been carried out by different non destructive techniques such as X-ray diffraction, scanning electron microscopy coupled with energy dispersive X-ray spectroscopy, X-ray absorption fine structure, transmission electron microscopy and electron microprobe analysis. The effectiveness of in situ Pb immobilization has also been evaluated by selective sequential extraction, by the toxicity leaching procedure and by a physiologically based extraction procedure simulating metal ingestion and gastrointestinal bioavailability to humans. Efficient Pb immobilization using P amendments requires increasing the solubility of the phosphate phase and of the Pb species phase by inducing acid conditions. Although phosphorus addition seems to be highly effective, excess P in soil and its potential effect on eutrophication of surface water, and the possibility of As enhanced leaching remains a concern. The use of mixed treatments may be a useful strategy to improve their effectiveness in reducing lead phyto- and bioavailability.
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References
Admassu W, Breese T (1999) Feasibility of using natural fishbone apatite as a substitute for hydroxyapatite in remediating aqueous heavy metals. J Hazard Mater 69:187–196
Adriano D (2001) Trace elements in terrestrial environments: biogeochemistry, bioavailability and risks of metals, 2nd edn. Springer, New York
Alloway BJ, Ayres DC (1997) Chemical principles of environmental pollution. Blackie Academic and Professional, London
Arnich N, Lanhers MC, Laurensot F, Podor R, Montiel A, Burnel D (2003) In vitro and in vivo studies of lead immobilization by synthetic hydroxyapatite. Environ Pollut 124:139–149
Basta N, Gradwohl R, Snethen K, Schroder J (2001) Chemical immobilization of lead, zinc and cadmium in smelter contaminated soils using biosolids and rock phosphate. J Environ Qual 30:1222–1230
Berti W, Cunningham S (1997) In-place inactivation of Pb in Pb-contaminated soils. Environ Sci Technol 31:1359–1364
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 104:225–233
Bolan N, Adriano D, Naidu R (2003) Role of phosphorus in (im)mobilization and baiovailability of heavy metals in the soil–plant system. Rev Environ Contam Toxicol 177:1–44
Bradl H (2004) Adsorption of heavy metal ions on soils and soils constituents. J Colloid Interface Sci 277:1–18
Brown S, Chaney R, Hallfrisch J, Xue Q (2003) Effect of biosolids processing on lead bioavailability in an urban soil. J Environ Qual 32:100–108
Brown S, Chaney R, Hallfrisch J, Ryan J, Berti W (2004) In situ soil treatments to reduce the phyto- and bioavailability of lead, zinc and cadmium. J Environ Qual 33:522–531
Brown S, Christensen B, Lombi E, McLaughlin M, McGrath S, Colpaert J, Vangronsveld J (2005) An inter-laboratory study to test the ability of amendments to reduce the availability of Cd, Pb, and Zn in situ. Environ Pollut 138:34–45
Cao RX, Ma LQ, Singh S, Chen M, Harris W, Kizza P (2001) Field demonstration of metal immobilization in contaminated soils using phosphate amendments. Florida Institute of Phosphate Research, Gainesville
Cao RX, Ma LQ, Chen M, Singh S, Harris W (2002) Impacts of phosphate amendments on lead biogeochemistry at a contaminated site. Environ Sci Technol 36:5296–5304
Cao RX, Ma LQ, Chen M, Singh S, Harris W (2003) Phosphate-induced metal immobilization in a contaminated site. Environ Pollut 122:19–28
Cao RX, Ma LQ, Rhue D, Appel C (2004) Mechanisms of lead, copper and zinc retention by phosphate rock. Environ Pollut 131:435–444
Chen X, Wright J, Conca J, Peurrung L (1997a) Effects of pH on heavy metal sorption on mineral apatite. Environ Sci Technol 31:624–631
Chen X, Wright J, Conca J, Perurrung L (1997b) Evaluation of heavy metal remediation using mineral apatite. Water Air Soil Pollut 98:57–78
Chen M, Ma LQ, Singh S, Cao R, Melamed R (2003) Field demonstration of in situ immobilization of soil Pb using P amendments. Adv Environ Res 8:93–102
Chen S, Zhu Y, Ma Y (2006) The effect of grain size of rock phosphate amendment on metal immobilization in contaminated soils. J Hazard Mater 134:74–79
Chen S, Xu M, Ma Y, Yang J (2007) Evaluation of different phosphate amendments on availability of metals in contaminated soil. Ecotoxicol Environ Saf 67:278–285
Cheng S, Hseu Z (2002) In-situ immobilization of cadmium and lead by different amendments in two contaminated soils. Water Air Soil Pollut 140:73–84
Chrysochoou M, Dermatas D, Grubb D (2007) Phosphate application to firing range soils for Pb immobilization: the unclear role of phosphate. J Hazard Mater 144:1–14
Cotter-Howells J, Caporn S (1996) Remediation of contaminated land by formation of heavy metal phosphates. Appl Geochem 11:335–342
Cotter-Howells J, Cahmpness P, Charnock J, Pattrick R (1994) Identification of pyromorphite in mine-waste contaminated soils by ATEM and EXAFS. Eur J Soil Sci 45:393–402
Crannell B, Eighmy T, Krzanowski J, Eudsden J, Shaw E, Francis C (2000) Heavy metal stabilization in municipal solid waste combustion bottom ash using soluble phosphate. Waste Manage 20:135–148
Davis BE (1995) Lead. In: Alloway BJ (eds) Heavy metals in soil. Blackie Academic and Professional, Glasgow, pp 208–223
Deydier E, Guillet R, Cren S, Pereas V, Mouchet F, Gauthier L (2007) Evaluation of meat and bone meal combustion residue as lead immobilizing material for in situ remediation of polluted aqueous solutions and soils: “chemical and ecotoxicological studies”. J Hazard Mater 146:227–236
Eighmy T, Crannell B, Butler L, Cartledge F, Emery E, Oblas D, et al (1997) Heavy metal stabilization in municipal solid waste combustion dry scrubber residue using soluble phosphate. Environ Sci Technol 31:3330–3338
Eighmy T, Crannell B, Krzanowski J, Butler L, Cartledge F, Emery E, et al (1998) Characterization and phosphate stabilization of dusts from the vitrification of MSW combustion residues. Waste Manage 34:4614–4619
Essington M, Foss J, Roh Y (2004) The soil mineralogy of lead at Horace’s Villa. Soil Sci Soc Am J 68:979–993
Farfel M, Orlovaa A, Chaneyb R, Leesc P, Rohded C, Ashleye P (2005) Biosolids compost amendment for reducing soil lead hazards: a pilot study of Orgro® amendment and grass seeding in urban yards. Sci Total Environ 340:81–95
Garrido F, Illera V, Campbell C, Garcia-González M (2006) Regulating the mobility of Cd, Cu and Pb in an acid soil with amendments of phosphogypsum, sugar foam and phosphoric rock. Eur J Soil Sci 57:95–105
Heredia O, Fernández-Cirelli A (2007) Environmental risks of increasing phosphorus addition in relation to soil sorption capacity. Geoderma 137:426–431
Hettiarachchi G, Pierzynski G (2004) Soil lead bioavailability and in situ remediation of lead-contaminated soils: a review. Environ Prog 23:78–93
Hettiarachchi G, Pierzynski G, Ransom M (2000) In situ stabilization of soil lead using phosphorus and manganese oxide. Environ Sci Technol 34:4614–4619
Hettiarachchi G, Pierzynski G, Ransom M (2001) In situ stabilization of soil lead using phosphorus. J Environ Qual 30:1214–1221
Hodson M, Valsami-Jones E, Cotter-Howells J, Dubbin W, Kemp A, Thornton I, Warren A (2001) Effect of bone meal (calcium phosphate) amendments on metal release from contaminated soils-a leaching column study. Environ Pollut 112:233–243
Knox A, Kaplan D, Adriano D, Hinton T, Wilson M (2003) Apatite and phillipsite as sequestering agents for metals and radionuclides. J Environ Qual 32:515–525
Laperche V, Traina S (1998) Immobilization of Pb by hydroxyapatite. In: Jenne E (ed) Adsorption of metals by geomedia. Academic, London, pp 255–276
Laperche V, Traina S, Gaddam P, Logan T (1996) Chemical and mineralogical characterizations of Pb in a contaminated soil: reactions with synthetic apatite. Environ Sci Technol 30:3321–3326
Laperche V, Logan T, Gaddam P, Traina S (1997) Effect of apatite amendments on plant uptake of lead from contaminated soil. Environ Sci Technol 31:2745–2753
Li Y, Chaney R, Siebielec G, Kerschner B (2000) Response of four turf grass cultivars to limestone and biosolids-compost amendment of a zinc and cadmium contaminated soil at Palmerton, PA. J Environ Qual 29:1440–1447
Lin C, Lian J, Fang H (2005) Soil lead immobilization using phosphate rock. Water Air Soil Pollut 161:113–123
Lindsay WL (1979) Chemical equilibria in soils. Wiley, New York
Liu R, Zhao D (2007) Reducing leachability and bioaccessibility of lead in soils using a new class of stabilized iron phosphate nanoparticles. Water Res 41:2491–2502
Lower S, Maurice P, Traina SJ (1998) Simultaneous dissolution of hydroxylapatite and precipitation of hydroxypyromorphite: direct evidence of homogeneous nucleation. Geochim Cosmochim Acta 62:1773–1780
Ma LQ, Rao G (1999) Aqueous Pb reduction in Pb-contaminated soils by phosphate rocks. Water Air Soil Pollut 110:1–16
Ma QY, Traina SJ, Logan TJ (1993) In situ lead immobilization by apatite. Environ Sci Technol 27:1803–1810
Ma QY, Logan TJ, Traina SJ, Ryan J (1994a) Effects of NO −3 , Cl−, F−, SO 2−4 and CO 2−3 on Pb2+ immobilization by hydroxyapatite. Environ Sci Technol 28:408–418
Ma QY, Traina SJ, Logan TJ, Ryan J (1994b) Effects of aqueous Al, Cd, Cu, Fe (II), Ni and Zn on Pb immobilization by hydroxyapatite. Environ Sci Technol 28:1219–1228
Ma QY, Logan TJ, Traina SJ (1995) Lead immobilization from aqueous solutions and contaminated soils using phosphate rocks. Environ Sci Technol 29:1118–1126
Manecki M, Maurice P, Traina SJ (2000) Uptake of aqueous Pb by Cl−, F− and OH− apatite: mineralogical evidence for nucleation mechanisms. Am Mineral 85:932–942
Mavropoulos E, Rossi A, Costa A, Perez C, Moreira J, Saldanha M (2002) Studies on the mechanisms of lead immobilization by hydroxyapatite. Environ Sci Technol 36:1625–1629
Mavropoulos E, Rocha N, Morieira J, Rossi A, Soares G (2004) Characterization of phase evolution during lead immobilization by synthetic hydroxyapatite. Mater Charact 53:71–78
McGowen SL, Basta NT, Brown GO (2001) Use of diammonium phosphate to reduce heavy metal solubility and transport in smelter-contaminated soil. J Environ Qual 30:493–500
Melamed R, Cao X, Chen M, Ma LQ (2003) Field assessment of lead immobilization in a contaminated soil after phosphate application. Sci Total Environ 305:117–127
Mouflih M, Aklil A, Jahroud N, Gourai M, Sebti S (2006) Removal of lead from aqueous solutions by natural phosphate. Hydrometallurgy 81:219–225
Nriagu JO (1984) Formation and stability of base metal phosphates in soils and sediments. In: Nriagu JO, Moore P (eds) Phosphate minerals. Springer, London, pp 318–329
Peryea F, Kammereck R (1997) Phosphate-enhanced movement of arsenic out of lead-arsenate-contaminated topsoil and through uncontaminated subsoil. Water Air Soil Poll 93:243–254
Porter S, Scheckel K, Impellitteri C, Ryan J (2004) Toxic metals in the environment: thermodynamic considerations for possible immobilization strategies for Pb, Cd, As and Hg. Crit Rev Environ Sci Technol 34:495–604
Ruby M, Davis A, Nicholson A (1994) In situ formation of lead phosphates in soils as a method to immobilize lead. Environ Sci Technol 28:646–653
Ruby M, Davis A, Schoof R, Eberle S, Sellstone C (1996) Estimation of bioavailability using a physiologically based extraction test. Environ Sci Technol 30:420–430
Ryan K, Zhang P, Hesterberg D, Chou J, Sayers D (2001) Formation of chloropyromorphite in a lead-contaminated soil amended with hydroxyapatite. Environ Sci Technol 35:3798–3803
Sauvé S, Martínez C, McBride M, Hendershot W (2000) Adsorption of free lead (Pb2+) by pedogenic oxides, ferrihydrite and leaf compost. Soil Sci Soc Am J 64:595–599
Scheckel K, Ryan J (2002) Effects of aging and pH on dissolution kinetics and stability of chloropyromorphite. Environ Sci Technol 36:2198–2204
Scheckel K, Ryan J (2004) Spectroscopic speciation and quantification of lead in soils. J Environ Qual 33:1288–1295
Scheckel K, Impellitteri C, Ryan J, McEvoy T (2003) Assessment of a sequential extraction procedure for perturbed lead-contaminated samples with and without phosphorus amendments. Environ Sci Technol 37:1892–1898
Scheckel K, Ryan J, Allen D, Lescano N (2005) Determining speciation of Pb in phosphate-amended soils: method limitations. Sci Total Environ 350:261–272
Scheinost A, Abend S, Pandya K, Sparks D (2001) Kinetic controls on Cu and Pb sorption by ferrihydrite. Environ Sci Technol 35:1090–1096
Schwab A, Lewis K, Banks M (2006) Lead stabilization by phosphate amendments in soil impacted by paint residue. J Environ Sci Health A Tox Hazard Subst Environ Eng 41:359–368
Seaman J, Arey J, Bertsch P (2001) Immobilization of Ni and other metals in contaminated sediments by hydroxyapatite addition. J Environ Qual 30:460–469
Shashkova I, Rat’Ko A, Kitikova N (1999) Removal of heavy metal ions from aqueous solutions by alkaline-earth metal phosphates. Colloids Surf A Physicochem Eng Asp 160:207–215
Singh S, Ma LQ, Harris W (2001) Heavy metal interactions with phosphatic clay: sorption and desorption behaviour. J Environ Qual 30:1961–1968
Sneddon I, Orueetxebarria M, Hodson M, Schofield P, Valsami-Jones E (2006) Use of bone meal amendments to immobilize Pb, Zn and Cd in soil: a leaching column study. Environ Pollut 144:816–825
Srinivasan M, Ferraris C, White T (2006) Cadmium and lead ion capture with three dimensionally ordered macroporous hydroxyapatite. Environ Sci Technol 40:7054–7059
Strawn D, Hickey P, Knudesen A, Baker L (2007) Geochemistry of lead contaminated wetland soils amended with phosphorus. Environ Geol 52:109–122
Sugiyama S, Ichii T, Fujisawa M, Kawashiro K, Tomida T, Shigemoto N, Hayashi H (2003) Heavy metal immobilization in aqueous solution using calcium phosphate and calcium hydrogen phosphates. J Colloid Interface Sci 259:408–410
Suzuki Y, Kyoichi I, Miyake M (1981) Synthetic hydroxyapatites employed as inorganic cation-exchangers. J Chem Soc Faraday Trans 77:1059–1062
Takeuchi Y, Arai H (1990) Removal of coexisting Pb2+, Cu2+ and Cd2+ ions from water by addition of hydroxyapatite powder. J Chem Eng Jpn 23:75–80
Tang X, Zhu Y, Chen S, Tang L, Chen X (2004) Assessment of the effectiveness of different phosphorus fertilizers to remediate Pb contaminated soil using in vitro test. Environ Int 30:531–537
Traina S., Laperche V. (1999) Contaminant bioavailability in soils, sediments and aquatic environments. Proc Natl Acad Sci USA 96:3365–3371
U.S. Environmental Protection Agency (USEPA) (1996) Soil screening guidance, user’s guidance, EPA 540/R−96/018. Office of Solid and Emergency Response, Washington, DC
U.S. Environmental Protection Agency (USEPA) Region 10 (2001) Consensus plan for soil and sediment studies: Coeur d´ Alene river soils and sediments bioavailability studies (URS DCN: 4162500.06161.05a.EPA:16.2), pp 1–16
Vangronsveld J, Cunningham SD (1998) Introduction to the concepts. In: Vangronsveld J, Cunningham SD (eds) Metal contaminated soils: in situ inactivation and phytorestoration. Springer, Berlin, pp 1–15
Wilson C, Brigmon R, Knox A, Seaman J, Smith G (2006) Effects of microbial and phosphate amendments on the bioavailability of lead (Pb) in shooting range soil. Bull Environ Contam Toxicol 76:392–399
Xu Y, Schwartz F (1994) Lead immobilization by hydroxyapatite in aqueous solution. J Contam Hydrol 15:187–206
Xu Y, Schwartz F, Traina S (1994) Sorption of Zn2+ and Cd2+ on hydroxyapatite surfaces. Environ Sci Technol 28:1472–1480
Yang J, Mosby D (2006) Field assessment of treatment efficacy by three methods of phosphoric acid application in lead-contaminated urban soil. Sci Total Environ 366:136–142
Yang J, Mosby D, Casteel S, Blanchar R (2001) Lead immobilization using phosphoric acid in a smelter-contaminated urban soil. Environ Sci Technol 35:3553–3559
Yoon J, Cao X, Ma LQ (2007) Application methods affect phosphorus-induced lead immobilization from a contaminated soil. J Environ Qual 36:373–378
Zhang P, Ryan J (1999a) Formation of chloropyromorphite from galena (PbS) in the presence of hydroxyapatite. Environ Sci Technol 33:618–624
Zhang P, Ryan J (1999b) Transformation of Pb (II) from cerrusite to chloropyromorphite in the presence of hydroxyapatite under varying conditions of pH. Environ Sci Technol 32:625–630
Zhang P, Ryan J, Bryndzia L (1997) Pyromorphite formation from goethite adsorbed lead. Environ Sci Technol 31:2673–2678
Zhang P, Ryan J, Yang J (1998) In vitro soil Pb solubility in the presence of hydroxyapatite. Environ Sci Technol 32:2763–2768
Zhu W, Chen S, Yang J (2004) Effects of soil amendments on lead uptake by two vegetable crops from a lead-contaminated soil from Anhui, China. Environ Int 30:351–356
Zwonitzer J, Pierzynski G, Hettiarachchi G (2003) Phosphorus source and rate effects on lead, cadmium and zinc bioavailability in a metal contaminated soil. Water Air Soil Pollut 143:193–209
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Miretzky, P., Fernandez-Cirelli, A. Phosphates for Pb immobilization in soils: a review. Environ Chem Lett 6, 121–133 (2008). https://doi.org/10.1007/s10311-007-0133-y
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DOI: https://doi.org/10.1007/s10311-007-0133-y