Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Molecular speciation controls arsenic and lead bioaccessibility in fugitive dusts from sulfidic mine tailings

Journal Article · · Environmental Science: Processes & Impacts
DOI:https://doi.org/10.1039/d2em00182a· OSTI ID:2424905

Communities nearby mine wastes in arid and semi-arid regions are potentially exposed to high concentrations of toxic metal(loid)s from fugitive dusts deriving from impoundments. To assess the relation between potentially lofted particles and human health risk, we studied the relationship between pharmacokinetic bioaccessibility and metal(loid) molecular speciation for mine tailings dust particulate matter (PM), with elevated levels of arsenic and lead (up to 59 and 34 mmol kg-1, respectively), by coupling in vitro bioassay (IVBA) with X-ray absorption spectroscopy (XAS). Mine tailing efflorescent salts (PMES) and PM from the surface crust (0–1 cm, PMSC) and near surface (0–25 cm) were isolated to <10 μm and <150 μm effective spherical diameter (PM10 and PM150) and reacted with synthetic gastric and lung fluid for 30 s to 100 h to investigate toxic metal(loid) release kinetics. Bioaccessible (BAc) fractions of arsenic and lead were about 10 and 100 times greater in gastric than in lung fluid simulant, respectively, and 10–100% of the maximum gastric BAc from PM10 and PM150 occurred within 30 s, with parabolic dissolution of fine, highly-reactive particles followed by slower release from less soluble sources. Evaporite salts were almost completely solubilized in gastric-fluid simulants. Arsenate within jarosite and sorbed to ferrihydrite, and lead from anglesite, were identified by XAS as the principal contaminant sources in the near surface tailings. In the synthetic lung fluid, arsenic was released continuously to 100 h, suggesting that residence time in vivo must be considered for risk determination. Analysis of pre- and post-IVBA PM indicated the release of arsenic in lung fluid was principally from arsenic-substituted jarosite, whereas in synthetic gastric fluid arsenic complexed on ferrihydrite surfaces was preferentially released and subsequently repartitioned to jarosite-like coordination at extended exposures. Lead dissolved at 30 s was subsequently repartitioned back to the solid phase as pyromorphite in phosphate rich lung fluid. The bioaccessibility of lead in surface tailings PM was limited due to robust sequestration in plumbojarosite. Kinetic release of toxic elements in both synthetic biofluids indicated that a single IVBA interval may not adequately describe release dynamics.

Research Organization:
US Department of Energy (USDOE), Washington, DC (United States). Office of Science, Basic Energy Sciences (BES); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Aeronautics and Space Administration (NASA)
OSTI ID:
2424905
Journal Information:
Environmental Science: Processes & Impacts, Journal Name: Environmental Science: Processes & Impacts Journal Issue: 2 Vol. 25; ISSN 2050-7887
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (87)

Oxidative Weathering Decreases Bioaccessibility of Toxic Metal(loid)s in PM10 Emissions From Sulfide Mine Tailings journal April 2018
Carcinogenicity Assessment of Selected Nickel Compounds journal March 1997
Mouse models for human intestinal microbiota research: a critical evaluation journal November 2017
In vitro assessment of arsenic mobility in historical mine waste dust using simulated lung fluid journal May 2017
Metal and Metalloid Contaminants in Atmospheric Aerosols from Mining Operations journal March 2011
Investigation of arsenic species in tailings and windblown dust from a gold mining area journal September 2015
Mechanisms of lead neurotoxicity journal February 1991
Accumulation and metabolism of arsenic in mice after repeated oral administration of arsenate journal September 2003
Role of iron in controlling speciation and mobilization of arsenic in subsurface environment journal November 2002
A novel method for assessing dissolution of aerosol inhaler products journal April 2003
Analytical methods for assessing metal bioaccessibility in airborne particulate matter: A scoping review journal June 2015
Changes in lead and zinc lability during weathering-induced acidification of desert mine tailings: Coupling chemical and micro-scale analyses journal December 2009
Soil Cd, Cu, Pb and Zn contaminants around Mount Isa city, Queensland, Australia: Potential sources and risks to human health journal June 2010
Particle-size dependence on metal(loid) distributions in mine wastes: Implications for water contamination and human exposure journal April 2011
Direct characterization of airborne particles associated with arsenic-rich mine tailings: Particle size, mineralogy and texture journal September 2011
Effect of silicic acid on arsenate and arsenite retention mechanisms on 6-L ferrihydrite: A spectroscopic and batch adsorption approach journal November 2013
Toxic metal(loid) speciation during weathering of iron sulfide mine tailings under semi-arid climate journal November 2015
Arsenic speciation in synthetic jarosite journal February 2005
Modification of an existing in vitro method to predict relative bioavailable arsenic in soils journal August 2017
Tridentate arsenate complexation with ferric hydroxide and its effect on the kinetics of arsenate adsorption and desorption journal October 2017
Redox metabolism of ingested arsenic: Integrated activities of microbiome and host on toxicological outcomes journal February 2019
The dispersal and storage of sediment-associated metals in an arid river system: The Leichhardt River, Mount Isa, Queensland, Australia journal March 2008
Human health effects of air pollution journal January 2008
Bioaccessibility and health risk of arsenic, mercury and other metals in urban street dusts from a mega-city, Nanjing, China journal May 2011
Arsenic sequestration by sorption processes in high-iron sediments journal December 2007
Synthesis and phase transformations involving scorodite, ferric arsenate and arsenical ferrihydrite: Implications for arsenic mobility journal June 2008
Surficial weathering of iron sulfide mine tailings under semi-arid climate journal September 2014
Total X-ray scattering, EXAFS, and Mössbauer spectroscopy analyses of amorphous ferric arsenate and amorphous ferric phosphate journal September 2014
Arsenic speciation in multiple metal environments journal May 2008
Importance of the oral arsenic bioaccessibility factor for characterising the risk associated with soil ingestion in a mining-influenced zone journal February 2013
Arsenic bioaccessibility in gold mine tailings of Delita, Cuba journal November 2013
Laboratory dust generation and size-dependent characterization of metal and metalloid-contaminated mine tailings deposits journal September 2014
Low arsenic bioaccessibility by fixation in nanostructured iron (Hydr)oxides: Quantitative identification of As-bearing phases journal July 2018
A review on the importance of metals and metalloids in atmospheric dust and aerosol from mining operations journal September 2012
Environmental factors influencing the structural dynamics of soil microbial communities during assisted phytostabilization of acid-generating mine tailings: A mesocosm experiment journal December 2014
Ingestion and inhalation of metal(loid)s through preschool gardening: An exposure and risk assessment in legacy mining communities journal May 2020
Tissue dosimetry, metabolism and excretion of pentavalent and trivalent monomethylated arsenic in mice after oral administration journal October 2005
Tissue dosimetry, metabolism and excretion of pentavalent and trivalent dimethylated arsenic in mice after oral administration journal February 2008
How can biologically-based modeling of arsenic kinetics and dynamics inform the risk assessment process? — A workshop review journal November 2008
Chronic arsenic exposure enhances metastatic potential via NRF2-mediated upregulation of SOX9 journal September 2020
Plumbojarosite Remediation of Soil Affects Lead Speciation and Elemental Interactions in Soil and in Mice Tissues journal November 2021
Hygroscopic Properties and Respiratory System Deposition Behavior of Particulate Matter Emitted By Mining and Smelting Operations journal October 2016
Phytoremediation Reduces Dust Emissions from Metal(loid)-Contaminated Mine Tailings journal April 2018
In Vitro , in Vivo, and Spectroscopic Assessment of Lead Exposure Reduction via Ingestion and Inhalation Pathways Using Phosphate and Iron Amendments journal July 2019
Oral Bioavailability of As, Pb, and Cd in Contaminated Soils, Dust, and Foods based on Animal Bioassays: A Review journal August 2019
Comparison of Five In Vitro Digestion Models To Study the Bioaccessibility of Soil Contaminants journal August 2002
Lead Sorption onto Ferrihydrite. 2. Surface Complexation Modeling journal March 2003
Bioaccessibility of Arsenic(V) Bound to Ferrihydrite Using a Simulated Gastrointestinal System journal January 2006
Equilibrium Solubility and Dissolution Rate of the Lead Phosphate Chloropyromorphite journal December 2007
Changes in Zinc Speciation with Mine Tailings Acidification in a Semiarid Weathering Environment journal September 2011
Geochemical Weathering Increases Lead Bioaccessibility in Semi-Arid Mine Tailings journal May 2012
New Clues to the Local Atomic Structure of Short-Range Ordered Ferric Arsenate from Extended X-ray Absorption Fine Structure Spectroscopy journal March 2013
(Micro)spectroscopic Analyses of Particle Size Dependence on Arsenic Distribution and Speciation in Mine Wastes journal August 2013
Bioaccessibility of Arsenic in Mining-Impacted Circumneutral River Floodplain Soils journal October 2014
Validation of the Predictive Capabilities of the Sbrc-G in Vitro Assay for Estimating Arsenic Relative Bioavailability in Contaminated Soils journal October 2014
Correlation of in Vivo Relative Bioavailability to in Vitro Bioaccessibility for Arsenic in Household Dust from China and Its Implication for Human Exposure Assessment journal November 2014
Effects of Soil Composition and Mineralogy on the Bioaccessibility of Arsenic from Tailings and Soil in Gold Mine Districts of Nova Scotia journal April 2010
Estimation of Lead and Arsenic Bioavailability Using a Physiologically Based Extraction Test journal January 1996
Advances in Evaluating the Oral Bioavailability of Inorganics in Soil for Use in Human Health Risk Assessment journal November 1999
The gut microbiome is required for full protection against acute arsenic toxicity in mouse models journal December 2018
Development of an in vitro method to estimate lung bioaccessibility of metals from atmospheric particles journal January 2011
Climate change and the aridification of North America journal May 2020
Bioavailable soil Pb minimized by in situ transformation to plumbojarosite journal December 2020
Contaminant bioavailability in soils, sediments, and aquatic environments journal March 1999
Arsenic, lead, and cadmium bioaccessibility in contaminated soils: Measurements and validations journal August 2019
An In Vitro Procedure for Estimation of Lead Relative Bioavailability: With Validation journal March 2007
The bioaccessibility of lead from Welsh mine waste using a respiratory uptake test journal July 2007
In vivo and in vitro methods for evaluating soil arsenic bioavailability: relevant to human health risk assessment journal February 2018
Mouse Assay for Determination of Arsenic Bioavailability in Contaminated Soils journal July 2013
Updating the ICRP human respiratory tract model journal June 2007
Mobilisation and Bioavailability of Arsenic Around Mesothermal Gold Deposits in a Semiarid Environment, Otago, New Zealand journal January 2002
Analysis of wind-driven resuspension of metal mine sludge in a tailings pond journal March 2004
Arsenic species in weathering mine tailings and biogenic solids at the Lava Cap Mine Superfund Site, Nevada City, CA journal January 2011
Experimental determination of the oral bioavailability and bioaccessibility of lead particles journal November 2012
Arsenic Metabolism by Human Gut Microbiota upon in Vitro Digestion of Contaminated Soils journal July 2010
Relative Bioavailability and Bioaccessibility and Speciation of Arsenic in Contaminated Soils journal November 2011
Phytostabilization of Mine Tailings in Arid and Semiarid Environments—An Emerging Remediation Technology journal March 2008
Arsenic Exposure and Type 2 Diabetes: A Systematic Review of the Experimental and Epidemiologic Evidence journal May 2006
Bioaccessibility, release kinetics, and molecular speciation of arsenic and lead in geo-dusts from the Iron King Mine Federal Superfund site in Humboldt, Arizona journal February 2014
Characterization of Arsenate-For-Sulfate Substitution in Synthetic Jarosite Using X-Ray Diffraction and X-Ray Absorption Spectroscopy journal August 2003
Mine Wastes and Human Health journal December 2011
Quantitative arsenic speciation in mine tailings using X-ray absorption spectroscopy journal June 1998
XAFS determination of the chemical form of lead in smelter-contaminated soils and mine tailings; importance of adsorption processes journal March 1999
Uptake and release of arsenic and antimony in alunite-jarosite and beudantite group minerals journal May 2019
Solubility and cell Toxicity of Cadmium journal January 1979
Dissolution of Functional Materials and Rare Earth Oxides into Pseudo Alveolar Fluid journal January 2006
Barrier function of airway tract epithelium journal May 2013

Similar Records

Metal(loid) bioaccessibility and inhalation risk assessment: A comparison between an urban and an industrial area
Journal Article · Wed Aug 15 00:00:00 EDT 2018 · Environmental Research · OSTI ID:23107968

Identification of lead chemical form in mine waste materials by X-ray absorption spectroscopy
Journal Article · Wed Jun 23 00:00:00 EDT 2010 · AIP Conference Proceedings · OSTI ID:21431085

Geochemical Weathering Increases Lead Bioaccessibility in Semi-Arid Mine Tailings
Journal Article · Wed Sep 05 00:00:00 EDT 2012 · Environ. Sci. Technol. · OSTI ID:1047892