In Situ Fixation of Metal(loid)s in Contaminated Soils: A Comparison of Conventional, Opportunistic, and Engineered Soil Amendments

Mele, Elena; Donner, Erica; Juhasz, Albert L.; Brunetti, Gianluca; Smith, Euan; Betts, Aaron R.; Castaldi, Paola; Deiana, Salvatore; Scheckel, Kirk G.; Lombi, Enzo

doi:10.1021/acs.est.5b01356

In Situ Fixation of Metal(loid)s in Contaminated Soils: A Comparison of Conventional, Opportunistic, and Engineered Soil Amendments

Journal Article · Mon Oct 12 00:00:00 EDT 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.5b01356· OSTI ID:1228097

Mele, Elena ^[1]; Donner, Erica ^[2]; Juhasz, Albert L. ^[2]; Brunetti, Gianluca ^[2]; Smith, Euan ^[2]; Betts, Aaron R. ^[3]; Castaldi, Paola ^[1]; Deiana, Salvatore ^[1]; Scheckel, Kirk G. ^[4]; Lombi, Enzo ^[5]

Univ. of Sassari (Italy)
Univ. of South Australia, South Australia (Australia); Cooperative Research Centre for Contamination Assessment and Remediation of the Environment (CRC CARE), South Australia (Australia)
United States Environmental Protection Agency, Cincinnati, OH (United States); Oak Ridge Inst. for Science and Education (ORISE), Oak Ridge, TN (United States)
United States Environmental Protection Agency, Cincinnati, OH (United States)
Univ. of South Australia, South Australia (Australia)

This study aimed to assess and compare the in vitro and in vivo bioaccessibility/bioavailability of As and Pb in a mining contaminated soil (As, 2267 mg kg^–1; Pb, 1126 mg kg^–1), after the addition of conventional (phosphoric acid), opportunistic [water treatment residues (WTRs)], and engineered [nano- and microscale zero valent iron (ZVI)] amendments. Phosphoric acid was the only amendment that could significantly decrease Pb bioaccessibility with respect to untreated soil (41 and 47% in the gastric phase and 2.1 and 8.1% in the intestinal phases, respectively), giving treatment effect ratios (TERs, the bioaccessibility in the amended soil divided by the bioaccessibility in the untreated soil) of 0.25 and 0.87 in the gastric and intestinal phase, respectively. The in vivo bioavailability of Pb decreased in the phosphate treatment relative to the untreated soil (6 and 24%, respectively), and also in the Fe WTR 2% (12%) and nZVI-2 (13%) treatments. The ZVI amendments caused a decrease in As bioaccessibility, with the greatest decrease in the nZVI2-treated soil (TERs of 0.59 and 0.64 in the gastric and intestinal phases, respectively). Furthermore, arsenic X-ray absorption near-edge spectroscopy analysis indicated that most of the As in the untreated soil was present as As(V) associated with Fe mineral phases, whereas in the treated soil, the proportion of arsenosiderite increased. Arsenite was present only as a minor species (3–5%) in the treated soils, with the exception of an nZVI treatment [~14% of As(III)], suggesting a partial reduction of As(V) to As(III) caused by nZVI oxidation.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Australian Government’s Cooperative Research Centres Programme; Australian Research Council (ARC); USDOE

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1228097

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 22 Vol. 49; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

References (51)

Short-term changes in water chemistry in the Baccu Locci stream (Sardinia, Italy) affected by past mining Frau, Franco; Cidu, Rosa; Ardau, Carla Applied Geochemistry, Vol. 27, Issue 9 https://doi.org/10.1016/j.apgeochem.2012.02.019	journal	September 2012
In vitro and in vivo studies of lead immobilization by synthetic hydroxyapatite Arnich, Nathalie; Lanhers, Marie-Claire; Laurensot, Franck Environmental Pollution, Vol. 124, Issue 1 https://doi.org/10.1016/s0269-7491(02)00416-5	journal	July 2003
Arsenic Mobilization by Citrate and Malate from a Red Mud-Treated Contaminated Soil Castaldi, Paola; Silvetti, Margherita; Mele, Elena Journal of Environmental Quality, Vol. 42, Issue 3 https://doi.org/10.2134/jeq2012.0425	journal	May 2013
Estimating dissolved organic carbon in natural waters by UV absorbance (254 nm) Brandstetter, Anton; Sletten, Ronald S.; Mentler, Axel Zeitschrift für Pflanzenernährung und Bodenkunde, Vol. 159, Issue 6 https://doi.org/10.1002/jpln.1996.3581590612	journal	December 1996
Heavy Metal Toxicity and the Environment Tchounwou, Paul B.; Yedjou, Clement G.; Patlolla, Anita K. Experientia Supplementum https://doi.org/10.1007/978-3-7643-8340-4_6	book	January 2012
Effect of Bile Type on the Bioaccessibility of Soil Contaminants in an In Vitro Digestion Model Oomen, A. G.; Rompelberg, C. J. M.; Kamp, E. Van de Archives of Environmental Contamination and Toxicology, Vol. 46, Issue 2 https://doi.org/10.1007/s00244-003-2138-2	journal	February 2004
Arsenic Bioaccessibility in a Soil Amended with Drinking-Water Treatment Residuals in the Presence of Phosphorus Fertilizer Sarkar, D.; Quazi, S.; Makris, K. C. Archives of Environmental Contamination and Toxicology, Vol. 53, Issue 3 https://doi.org/10.1007/s00244-006-0170-8	journal	July 2007
Bioavailability and Bioaccessibility of Arsenic in a Soil Amended with Drinking-Water Treatment Residuals Nagar, Rachana; Sarkar, Dibyendu; Makris, Konstantinos C. Archives of Environmental Contamination and Toxicology, Vol. 57, Issue 4 https://doi.org/10.1007/s00244-009-9318-7	journal	April 2009
Decrease of Pb bioavailability in solis by addition of phosphate ions Manecki, Maciej; Bogucka, Anna; Bajda, Tomasz Environmental Chemistry Letters, Vol. 3, Issue 4 https://doi.org/10.1007/s10311-005-0030-1	journal	January 2006
Lead phosphate formation in soils Cotter-Howells, Janet Environmental Pollution, Vol. 93, Issue 1 https://doi.org/10.1016/0269-7491(96)00020-6	journal	January 1996
Characterization of humified compounds by extraction and fractionation on solid polyvinylpyrrolidone Ciavatta, C.; Govi, M.; Antisari, L. Vittori Journal of Chromatography A, Vol. 509, Issue 1 https://doi.org/10.1016/S0021-9673(01)93248-0	journal	June 1990
Extraction of arsenic in a synthetic arsenic-contaminated soil using phosphate Alam, M. G. M.; Tokunaga, S.; Maekawa, T. Chemosphere, Vol. 43, Issue 8 https://doi.org/10.1016/S0045-6535(00)00205-8	journal	June 2001
Minerals controlling arsenic and lead solubility in an abandoned gold mine tailings Roussel, Christophe; Néel, Catherine; Bril, Hubert Science of The Total Environment, Vol. 263, Issue 1-3 https://doi.org/10.1016/S0048-9697(00)00707-5	journal	December 2000
In situ fixation of metals in soils using bauxite residue: chemical assessment Lombi, Enzo; Zhao, Fang-Jie; Zhang, Gangya Environmental Pollution, Vol. 118, Issue 3 https://doi.org/10.1016/S0269-7491(01)00294-9	journal	August 2002
In vitro and in vivo studies of lead immobilization by synthetic hydroxyapatite Arnich, Nathalie; Lanhers, Marie-Claire; Laurensot, Franck Environmental Pollution, Vol. 124, Issue 1 https://doi.org/10.1016/S0269-7491(02)00416-5	journal	July 2003
Speciation of metal(loid)s in environmental samples by X-ray absorption spectroscopy: A critical review Gräfe, Markus; Donner, Erica; Collins, Richard N. Analytica Chimica Acta, Vol. 822 https://doi.org/10.1016/j.aca.2014.02.044	journal	April 2014
Arsenic mobilization and iron transformations during sulfidization of As(V)-bearing jarosite Johnston, Scott G.; Burton, Edward D.; Keene, Annabelle F. Chemical Geology, Vol. 334 https://doi.org/10.1016/j.chemgeo.2012.09.045	journal	December 2012
In vitro assessment of arsenic bioaccessibility in contaminated (anthropogenic and geogenic) soils Juhasz, Albert L.; Smith, Euan; Weber, John Chemosphere, Vol. 69, Issue 1 https://doi.org/10.1016/j.chemosphere.2007.04.046	journal	August 2007
Characterization of zero-valent iron nanoparticles Sun, Yuan-Pang; Li, Xiao-qin; Cao, Jiasheng Advances in Colloid and Interface Science, Vol. 120, Issue 1-3 https://doi.org/10.1016/j.cis.2006.03.001	journal	June 2006
Assessment of zerovalent iron for stabilization of chromium, copper, and arsenic in soil Kumpiene, Jurate; Ore, Solvita; Renella, Giancarlo Environmental Pollution, Vol. 144, Issue 1 https://doi.org/10.1016/j.envpol.2006.01.010	journal	November 2006
Surficial weathering of iron sulfide mine tailings under semi-arid climate Hayes, Sarah M.; Root, Robert A.; Perdrial, Nicolas Geochimica et Cosmochimica Acta, Vol. 141 https://doi.org/10.1016/j.gca.2014.05.030	journal	September 2014
Leachability, bioaccessibility and plant availability of trace elements in contaminated soils treated with industrial by-products and subjected to oxidative/reductive conditions Silvetti, Margherita; Castaldi, Paola; Holm, Peter E. Geoderma, Vol. 214-215 https://doi.org/10.1016/j.geoderma.2013.09.010	journal	February 2014
Reduction of As(V) to As(III) by commercial ZVI or As(0) with acid-treated ZVI Sun, Fenglong; Osseo-Asare, Kwadwo A.; Chen, Yongsheng Journal of Hazardous Materials, Vol. 196 https://doi.org/10.1016/j.jhazmat.2011.09.029	journal	November 2011
Influence of saliva, gastric and intestinal phases on the prediction of As relative bioavailability using the Unified Bioaccessibility Research Group of Europe Method (UBM) Juhasz, Albert L.; Weber, John; Smith, Euan Journal of Hazardous Materials, Vol. 197 https://doi.org/10.1016/j.jhazmat.2011.09.068	journal	December 2011
Reduction and adsorption of Pb2+ in aqueous solution by nano-zero-valent iron—A SEM, TEM and XPS study Xi, Yunfei; Mallavarapu, Megharaj; Naidu, Ravendra Materials Research Bulletin, Vol. 45, Issue 10 https://doi.org/10.1016/j.materresbull.2010.06.046	journal	October 2010
Influence of in vitro assay pH and extractant composition on As bioaccessibility in contaminated soils Smith, Euan; Scheckel, Kirk; Miller, Bradley W. Science of The Total Environment, Vol. 473-474 https://doi.org/10.1016/j.scitotenv.2013.12.030	journal	March 2014
Reducing leachability and bioaccessibility of lead in soils using a new class of stabilized iron phosphate nanoparticles Liu, Ruiqiang; Zhao, Dongye Water Research, Vol. 41, Issue 12 https://doi.org/10.1016/j.watres.2007.03.026	journal	June 2007
Adsorption, Sequestration, and Bioaccessibility of As(V) in Soils Yang, Jae-Kyu; Barnett, Mark O.; Jardine, Philip M. Environmental Science & Technology, Vol. 36, Issue 21 https://doi.org/10.1021/es011507s	journal	November 2002
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 Lombi, Enzo; Hamon, Rebecca E.; McGrath, Steve P. Environmental Science & Technology, Vol. 37, Issue 5 https://doi.org/10.1021/es026083w	journal	March 2003
In Vivo–in Vitro and XANES Spectroscopy Assessments of Lead Bioavailability in Contaminated Periurban Soils Smith, Euan; Kempson, Ivan M.; Juhasz, Albert L. Environmental Science & Technology, Vol. 45, Issue 14 https://doi.org/10.1021/es200653k	journal	July 2011
Kinetics of Zero Valent Iron Nanoparticle Oxidation in Oxygenated Water Greenlee, Lauren F.; Torrey, Jessica D.; Amaro, Robert L. Environmental Science & Technology, Vol. 46, Issue 23 https://doi.org/10.1021/es303037k	journal	November 2012
Evaluation of SBRC-Gastric and SBRC-Intestinal Methods for the Prediction of In Vivo Relative Lead Bioavailability in Contaminated Soils Juhasz, Albert L.; Weber, John; Smith, Euan Environmental Science & Technology, Vol. 43, Issue 12 https://doi.org/10.1021/es803238u	journal	June 2009
Estimation of Lead and Arsenic Bioavailability Using a Physiologically Based Extraction Test Ruby, Michael V.; Davis, Andy; Schoof, Rosalind Environmental Science & Technology, Vol. 30, Issue 2 https://doi.org/10.1021/es950057z	journal	January 1996
An In Vitro Gastrointestinal Method To Estimate Bioavailable Arsenic in Contaminated Soils and Solid Media Rodriguez, Robin R.; Basta, Nicholas T.; Casteel, Stan W. Environmental Science & Technology, Vol. 33, Issue 4 https://doi.org/10.1021/es980631h	journal	February 1999
Advances in Evaluating the Oral Bioavailability of Inorganics in Soil for Use in Human Health Risk Assessment Ruby, M. V.; Schoof, R.; Brattin, W. Environmental Science & Technology, Vol. 33, Issue 21 https://doi.org/10.1021/es990479z	journal	November 1999
Simultaneous Oxidation and Reduction of Arsenic by Zero-Valent Iron Nanoparticles: Understanding the Significance of the Core−Shell Structure Ramos, Mauricio A. V.; Yan, Weile; Li, Xiao-qin The Journal of Physical Chemistry C, Vol. 113, Issue 33 https://doi.org/10.1021/jp9051837	journal	July 2009
Selected bioavailability assays to test the efficacy of amendment-induced immobilization of lead in soils Geebelen, W.; Adriano, D. C.; van der Lelie, D. Plant and Soil, Vol. 249, Issue 1, p. 217-228 https://doi.org/10.1023/A:1022534524063	journal	February 2003
The New MRCAT (Sector 10) Bending Magnet Beamline at the Advanced Photon Source Kropf, A. J.; Katsoudas, J.; Chattopadhyay, S. SRI 2009, 10TH INTERNATIONAL CONFERENCE ON RADIATION INSTRUMENTATION, AIP Conference Proceedings https://doi.org/10.1063/1.3463194	conference	January 2010
A radio-isotopic dilution technique for functional characterisation of the associations between inorganic contaminants and water-dispersible naturally occurring soil colloids Tavakkoli, Ehsan; Donner, Erica; Juhasz, Albert Environmental Chemistry, Vol. 10, Issue 4 https://doi.org/10.1071/EN13020	journal	January 2013
Heavy metal distribution, bioaccessibility, and phytoavailability in long-term contaminated soils from Lake Macquarie, Australia Kim, Kwon-Rae; Owens, Gary; Naidu, Ravi Soil Research, Vol. 47, Issue 2 https://doi.org/10.1071/SR08054	journal	January 2009
The Influence of Liquid to Soil Ratios on Arsenic and Lead Bioaccessibility in Reference and Field Soil Smith, B. A.; Kirk, J. L.; Stephenson, G. L. Human and Ecological Risk Assessment: An International Journal, Vol. 16, Issue 1 https://doi.org/10.1080/10807030903459163	journal	February 2010
Amending Soils With Phosphate As Means To Mitigate Soil Lead Hazard: A Critical Review Of The State Of The Science Scheckel, Kirk G.; Diamond, Gary L.; Burgess, Michele F. Journal of Toxicology and Environmental Health, Part B, Vol. 16, Issue 6 https://doi.org/10.1080/10937404.2013.825216	journal	August 2013
Arsenic(Iii) and Arsenic(V) Adsorption on Three California Soils Manning, Bruce A.; Goldberg, Sabine Soil Science, Vol. 162, Issue 12 https://doi.org/10.1097/00010694-199712000-00004	journal	January 1997
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Chemical Immobilization of Lead, Zinc, and Cadmium in Smelter-Contaminated Soils Using Biosolids and Rock Phosphate Basta, N. T.; Gradwohl, R.; Snethen, K. L. Journal of Environmental Quality, Vol. 30, Issue 4 https://doi.org/10.2134/jeq2001.3041222x	journal	January 2001
Treatment of Contaminated Soil with Phosphorus and Manganese Oxide Reduces Lead Absorption by Sprague–Dawley Rats Hettiarachchi, Ganga M.; Pierzynski, Gary M.; Oehme, Fredrick W. Journal of Environment Quality, Vol. 32, Issue 4 https://doi.org/10.2134/jeq2003.1335	journal	January 2003
Phosphorus Retention Mechanisms of a Water Treatment Residual Ippolito, J. A.; Barbarick, K. A.; Heil, D. M. Journal of Environmental Quality, Vol. 32, Issue 5 https://doi.org/10.2134/jeq2003.1857	journal	September 2003
Assessment of the Use of Industrial By-Products to Remediate a Copper- and Arsenic-Contaminated Soil Lombi, Enzo; Hamon, Rebecca E.; Wieshammer, Gerlinde Journal of Environment Quality, Vol. 33, Issue 3 https://doi.org/10.2134/jeq2004.0902	journal	January 2004
Validation of the In Vitro Gastrointestinal (IVG) Method to Estimate Relative Bioavailable Lead in Contaminated Soils Schroder, J. L.; Basta, N. T.; Casteel, S. W. Journal of Environmental Quality, Vol. 33, Issue 2 https://doi.org/10.2134/jeq2004.5130	journal	March 2004
Drinking Water Treatment Residuals: A Review of Recent Uses Ippolito, J. A.; Barbarick, K. A.; Elliott, H. A. Journal of Environmental Quality, Vol. 40, Issue 1 https://doi.org/10.2134/jeq2010.0242	journal	January 2011
Competitive Sorption of Arsenate and Phosphate on Different Clay Minerals and Soils Violante, Antonio; Pigna, Massimo Soil Science Society of America Journal, Vol. 66, Issue 6 https://doi.org/10.2136/sssaj2002.1788	journal	January 2002

Cited By (2)

Evaluation of the stability of a nanoremediation strategy using barley plants Gil-Díaz, M.; González, A.; Alonso, J. Journal of Environmental Management, Vol. 165 https://doi.org/10.1016/j.jenvman.2015.09.032	journal	January 2016
Nanoremediation of As and metals polluted soils by means of graphene oxide nanoparticles Baragaño, Diego; Forján, Rubén; Welte, Lorena Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-58852-4	journal	February 2020

Similar Records

Predictive Capabilities of in Vitro Assays for Estimating Pb Relative Bioavailability in Phosphate Amended Soils

Journal Article · Tue Nov 08 19:00:00 EST 2016 · Environmental Science and Technology · OSTI ID:1340718

Comparison of the Bioavailability of Waste Laden Soils Using ''In Vivo'' ''In Vitro'' Analytical Methodology and Bioaccessibility of Radionuclides for Refinement of Exposure/Dose Estimates

Technical Report · Wed Sep 15 00:00:00 EDT 1999 · OSTI ID:14331

Lead Speciation and In Vitro Bioaccessibility of Compost-Amended Urban Garden Soils

Journal Article · Sat Dec 31 23:00:00 EST 2016 · Journal of Environmental Quality · OSTI ID:1411777

Related Subjects

54 ENVIRONMENTAL SCIENCES
bioaccessibility
minerals
phosphates
redox reactions
soils

In Situ Fixation of Metal(loid)s in Contaminated Soils: A Comparison of Conventional, Opportunistic, and Engineered Soil Amendments

Citation Formats

References (51)

Cited By (2)

Similar Records

Related Subjects