Abstract
This study combined the original unsaturated-column-percolation test with X-ray diffraction (XRD) analysis to understand how lead is transformed into lead-insoluble phase and immobilized by hydroxyapatite during lead migration in the water-unsaturated soil of different lead mobilities. The amounts of lead migrated from the soils without hydroxyapatite ranged from 4 to 46%, depending on the lead mobilities of soils. On the other hand, those of soils with hydroxyapatite were greatly suppressed by > 95% as compared with those without hydroxyapatite. The XRD analysis showed that the amounts of lead transformed into pyromorphite were compatible with those of lead migrated from the soil irrespective of the different lead mobilities. To the best of our knowledge, this study provides the first experimental evidence that lead migration can induce lead to transform into pyromorphite in the water-unsaturated soil. In addition, this study quantitatively demonstrates that the amount of lead migrated is almost equal to that of lead formed into pyromorphite. Thus, it was found that even if soluble lead remains after the application of immobilization material, it would be immobilized by the material during the lead migration as long as adequate material is applied to the soil.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Álvarez-Ayuso E, Otones V, Murciego A, García-Sánchez A (2013) Evaluation of different amendments to stabilize antimony in mining polluted soils. Chemosphere 90(8):2233–2239. https://doi.org/10.1016/j.chemosphere.2012.09.086
Baldock JA, Skjemstad JO (2000) Role of the soil matrix and minerals in protecting natural organic materials against biological attack. Org Geochem 31(7-8):697–710. https://doi.org/10.1016/S0146-6380(00)00049-8
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(2):225–233. https://doi.org/10.1016/S0269-7491(98)00184-5
Bolan N, Kunhikrishnan A, Thangarajan R, Kumpiene J, Park J, Makino T, Kirkham MB, Scheckel K (2014) Remediation of heavy metal(loid)s contaminated soils—to mobilize or to immobilize? J Hazard Mater 266:141–166. https://doi.org/10.1016/j.jhazmat.2013.12.018
Cao X, Ma LQ, Chen M, Hardison DW, Harris WG (2003) Lead transformation and distribution in the soils of shooting ranges in Florida, USA. Sci Total Environ 307(1-3):179–189. https://doi.org/10.1016/S0048-9697(02)00543-0
Cao X, Ma LQ, Rhue DR, Appel CS (2004) Mechanisms of lead, copper, and zinc retention by phosphate rock. Environ Pollut 131(3):435–444. https://doi.org/10.1016/j.envpol.2004.03.003
Chen M, Ma LQ, Singh SP, Cao RX, Melamed R (2003) Field demonstration of in situ immobilization of soil Pb using P amendments. Adv Environ Res 8(1):93–102. https://doi.org/10.1016/S1093-0191(02)00145-4
Chen SB, Zhu YG, Ma YB (2006) The effect of grain size of rock phosphate amendment on metal immobilization in contaminated soils. J Hazard Mater B 134(1-3):74–79. https://doi.org/10.1016/j.jhazmat.2005.10.027
Chrysochoou M, Dermatas D, Grubb DG (2007) Phosphate application to firing range soils for Pb immobilization: the unclear role of phosphate. J Hazard Mater 144(1-2):1–14. https://doi.org/10.1016/j.jhazmat.2007.02.008
Dermatas D, Cao X, Tsaneva V, Shen G, Grubb DG (2006) Fate and behavior of metal(loid) contaminants in an organic matter-rich shooting range soil: implications for remediation. Water Air Soil Pollut: Focus 6(1-2):143–155. https://doi.org/10.1007/s11267-005-9003-4
Eren E, Gumus H (2011) Characterization of the structural properties and Pb (II) adsorption behavior of iron oxide coated sepiolite. Desalination 273(2-3):276–284. https://doi.org/10.1016/j.desal.2011.01.004
Furuta S, Katsuki H, Komarneni S (1998) Porous hydroxyapatite monoliths from gypsum waste. J Mater Chem 8(12):2803–2806. https://doi.org/10.1039/a806659k
Gangloff S, Stille P, Pierret MC, Weber T, Chabaux F (2014) Characterization and evolution of dissolved organic matter in acidic forest soil and its impact on the mobility of major and trace elements (case of the Strengbach watershed). Geochim Cosmochim Acta 130:21–41. https://doi.org/10.1016/j.gca.2013.12.033
Guo G, Zhou Q, Ma LQ (2006) Availability and assessment of fixing additives for the in situ remediation of heavy metal contaminated soils: a review. Environ Monit Assess 116(1-3):513–528. https://doi.org/10.1007/s10661-006-7668-4
He M, Shi H, Zhao X, Yu Y, Qu B (2013) Immobilization of Pb and Cd in contaminated soil using nano-crystallite hydroxyapatite. Procedia Environ Sci 18:657–665. https://doi.org/10.1016/j.proenv.2013.04.090
Heier LS, Meland S, Ljønes M, Salbu B, Strømseng AE (2010) Short-term temporal variations in speciation of Pb, Cu, Zn and Sb in a shooting range runoff stream. Sci Total Environ 408(11):2409–2417. https://doi.org/10.1016/j.scitotenv.2010.02.019
Katoh M, Murase J, Kimura M (2004) Sites and processes of nutrient accumulation in the subsoil through water percolation from the plow layer in a submerged paddy soil microcosm. Soil Sci Plant Nutr 50(5):731–738. https://doi.org/10.1080/00380768.2004.10408529
Katoh M, Murase J, Sugimoto A, Kimura M (2005) Effect of rice straw amendment on dissolved organic and inorganic carbon and cationic nutrients in percolating water from a flooded paddy soil: a microcosm experiment using 13C-enriched rice straw. Org Geochem 36(5):803–811. https://doi.org/10.1016/j.orggeochem.2004.12.006
Katoh M, Tsuda K, Sato T (2014) Formation of lead insoluble phases with water condition in contaminated soil. In: Abdulmalek B, Samuel YTS, Bruce B (eds) 7th International Congress on Environmental Geotechnics. Engineers Australia, Barton, pp 1581–1587
Katoh M, Tsuda K, Matsumoto N, Sato T (2016) Formation of pyromorphite and lead mobilization in contaminated soils amended with hydroxyapatite in the presence of iron oxyhydroxide and water percolation. Water Air Soil Pollut 227(12):470. https://doi.org/10.1007/s11270-016-3172-9
Knox AS, Kaplan DI, Paller MH (2006) Phosphate sources and their suitability for remediation of contaminated soils. Sci Total Environ 357(1-3):271–279. https://doi.org/10.1016/j.scitotenv.2005.07.014
Komárek M, Vaněk A, Ettler V (2013) Chemical stabilization of metals and arsenic in contaminated soils using oxides—a review. Environ Pollut 172:9–22. https://doi.org/10.1016/j.envpol.2012.07.045
Kumpiene J, Lagerkvist A, Maurice C (2008) Stabilization of As, Cr, Cu, Pb and Zn in soil using amendments—a review. Waste Manag 28(1):215–225. https://doi.org/10.1016/j.wasman.2006.12.012
Mahar A, Wang P, Li R, Zhang Z (2015) Immobilization of lead and cadmium in contaminated soil using amendments: a review. Pedosphere 25(4):555–568. https://doi.org/10.1016/S1002-0160(15)30036-9
Maie N, Watanabe A, Kimura M (1998) Origin and properties of humus in the subsoil of irrigated rice paddies III. Changes in binding type of humus in submerged plow layer soil. Soil Sci Plant Nutr 44(3):331–345. https://doi.org/10.1080/00380768.1998.10414455
Martin WA, Lee LS, Schwab P (2013) Antimony migration trends from a small arms firing range compared to lead, copper, and zinc. Sci Total Environ 463-464:222–228. https://doi.org/10.1016/j.scitotenv.2013.05.086
Martinez RE, Sharma P, Kappler A (2010) Surface binding site analysis of Ca2+-homoionized clay-humic acid complexes. J Colloid Interface Sci 352(2):526–534. https://doi.org/10.1016/j.jcis.2010.08.082
Mavropouls E, Rossi AM, Costa AM, Perez CAC, Moreira JC, Saldanha M (2002) Studies on the mechanisms of lead immobilization by hydroxyapatite. Environ Sci Technol 36(7):1625–1629. https://doi.org/10.1021/es0155938
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(1-3):117–127. https://doi.org/10.1016/S0048-9697(02)00469-2
MOE of Japan (2016) Results of the survey on the enforcement status of the soil contamination countermeasures act and soil contamination investigations and countermeasures in FY 2014 (in Japanese), Ministry Environment Government of Japan, Environmental Management Bureau
Mulligan CN, Yong RN, Gibbs BF (2001) An evaluation of technologies for the heavy metal remediation of dredged sediments. J Hazard Mater 85(1-2):145–163. https://doi.org/10.1016/S0304-3894(01)00226-6
Ogawa S, Katoh M, Sato T (2014) Contribution of hydroxyapatite and ferrihydrite in combined applications for the removal of lead and antimony from aqueous solutions. Water Air Soil Pollut 225(7):2023–2034. https://doi.org/10.1007/s11270-014-2023-9
Ogawa S, Katoh M, Sato T (2015) Simultaneous lead and antimony immobilization in shooting range soil by combined application of hydroxyapatite and ferrihydrite. Environ Technol 36(20):2647–2656. https://doi.org/10.1080/09593330.2015.1042071
Orsetti S, Quiroga MM, Andrade EM (2006) Binding of Pb(II) in the system humic acid/goethite at acidic pH. Chemosphere 65(11):2313–2321. https://doi.org/10.1016/j.chemosphere.2006.05.009
Richmond WR, Loan M, Morton J, Parkinson GM (2004) Arsenic removal from aqueous solution via ferrihydrite crystallization control. Environ Sci Technol 38(8):2368–2372. https://doi.org/10.1021/es0353154
Sanderson P, Naidu R, Bolan N (2016) The effect of environmental conditions and soil physicochemistry on phosphate stabilization of Pb in shooting range soils. J Environ Manag 170:123–130. https://doi.org/10.1016/j.jenvman.2016.01.017
Scheckel KG, Ryan JA (2002) Effects of aging and pH on dissolution kinetics and stability of chloropyromorphite. Environ Sci Technol 36(10):2198–2204. https://doi.org/10.1021/es015803g
Scheckel KG, Ryan JA (2004) Spectroscopic speciation and quantification of lead in phosphate-amended soils. J Environ Qual 33(4):1288–1295. https://doi.org/10.2134/jeq2004.1288
Scheckel KG, Ryan JA, Allen D, Lescano NV (2005) Determining speciation of Pb in phosphate-amended soils: method limitations. Sci Total Environ 350(1-3):261–272. https://doi.org/10.1016/j.scitotenv.2005.01.020
Shen P, Huang C, Ganguly C, Gaboriault-Whitcomb S, Rabideau AJ, Van Benschoten JE (2001) Comparison of soluble and immobilized acetate for removing Pb from contaminated soil. J Hazard Mater 87(1-3):59–72. https://doi.org/10.1016/S0304-3894(01)00204-7
Spuller C, Weigand H, Marb C (2007) Trace metal stabilization in a shooting range soil: mobility and phytotoxicity. J Hazard Mater 141(2):378–387. https://doi.org/10.1016/j.jhazmat.2006.05.082
Suzuki T, Hatsushika T, Hayakawa Y (1981) Synthetic hydroxyapatite employed as inorganic cation exchangers. J Chem Soc Faraday Trans I 77(5):1059–1062. https://doi.org/10.1039/f19817701059
Suzuki T, Nakamura A, Niinae M, Nakata H, Fujii H, Tasaka Y (2013) Lead immobilization in artificially contaminated kaolinite using magnesium oxide-based materials: immobilization mechanisms and long-term evaluation. Chem Eng J 232:80–387
USEPA (1996) Recent developments for in situ treatment of metals contaminated soils. U.S. Environmental Protection Agency, Office of Solid Waste and Emergency Response
Wenzel WW, Kirchbaumer N, Prohaska T, Stingeder G, Lombi E, Adriano DC (2001) Arsenic fractionation in soils using an improved sequential extraction procedure. Anal Chim Acta 436(2):309–323. https://doi.org/10.1016/S0003-2670(01)00924-2
Xie ZM, Chen J, Naidu R (2013) Not all phosphate fertilizers immobilize lead in soils. Water Air Soil Pollut 224(12):1712. https://doi.org/10.1007/s11270-013-1712-0
Yin X, Gao B, Ma LQ, Saha UK, Sun H, Wang G (2010) Colloid-facilitated Pb transport in two shooting-range soils in Florida. J Hazard Mater 177(1-3):620–625. https://doi.org/10.1016/j.jhazmat.2009.12.077
Acknowledgements
The ICP-AES and CN analyzer used for chemical analysis in this study were made available by the Division of Instrumental Analysis at Gifu University. The authors are grateful to Prof. Y. Ohya, Prof. F. Li, and Prof. T. Yamada (Gifu University) for permitting the use of the XRD and TOC analyzer.
Funding
This study was supported by the Japan Society for the Promotion of Science (JSPS) KAKENHI (grant number 25740036).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Responsible editor: Zhihong Xu
Electronic supplementary material
ESM 1
(DOCX 46 kb)
Rights and permissions
About this article
Cite this article
Ogawa, S., Sato, T. & Katoh, M. Formation of a lead-insoluble phase, pyromorphite, by hydroxyapatite during lead migration through the water-unsaturated soils of different lead mobilities. Environ Sci Pollut Res 25, 7662–7671 (2018). https://doi.org/10.1007/s11356-017-1093-9
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-017-1093-9