Arsenic release and transport during oxidative dissolution of spatially-distributed sulfide minerals

Battistel, Maria; Stolze, Lucien; Muniruzzaman, Muhammad; Rolle, Massimo

doi:10.1016/j.jhazmat.2020.124651

Cited by 41 publications

(25 citation statements)

References 93 publications

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“…Pyrite reactivity may decrease after repeated ASR cycles or continuous injection due to depletion of a significant fraction of reactive pyrite , and/or surface passivation limiting the rate of oxidation. , Following oxidative dissolution of pyrite, ferrous iron quickly oxidizes to form poorly crystalline Fe (oxyhydr)oxides (e.g., ferrihydrite), which have a strong sorption affinity for oxyanions including those of As, Mo, and V. Dissolved contaminant concentrations generally remain low in the presence of stable surface complexes. For example, during ASR injection, when oxygen is continuously provided and oxic conditions maintain the stability of Fe (oxyhydr)oxides, dissolved As concentrations remain low. ,, Similarly, in well-aerated infiltration systems, As is most likely initially bound to Fe (oxyhydr)oxides, and mobilization depends on the stability of surface complexes.…”

Section: Mechanisms Of Contaminant Mobilizationmentioning

confidence: 99%

Mobilization of Arsenic and Other Naturally Occurring Contaminants during Managed Aquifer Recharge: A Critical Review

Fakhreddine

Prommer

Scanlon

et al. 2021

Environ. Sci. Technol.

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Population growth and climate variability highlight the need to enhance freshwater security and diversify water supplies. Subsurface storage of water in depleted aquifers is increasingly used globally to alleviate disparities in water supply and demand often caused by climate extremes including floods and droughts. Managed aquifer recharge (MAR) stores excess water supplies during wet periods via infiltration into shallow underlying aquifers or direct injection into deep aquifers for recovery during dry seasons. Additionally, MAR can be designed to improve recharge water quality, particularly in the case of soil aquifer treatment and riverbank filtration. While there are many potential benefits to MAR, introduction of recharge water can alter the native geochemical and hydrological conditions in the receiving aquifer, potentially mobilizing toxic, naturally occurring (geogenic) contaminants from sediments into groundwater where they pose a much larger threat to human and ecosystem health. On the basis of the present literature, arsenic poses the most widespread challenge at MAR sites due to its ubiquity in subsurface sediments and toxicity at trace concentrations. Other geogenic contaminants of concern include fluoride, molybdenum, manganese, and iron. Water quality degradation threatens the viability of some MAR projects with several sites abandoning operations due to arsenic or other contaminant mobilization. Here, we provide a critical review of studies that have uncovered the geochemical and hydrological mechanisms controlling mobilization of arsenic and other geogenic contaminants at MAR sites worldwide, including both infiltration and injection sites. These mechanisms were evaluated based on site-specific characteristics, including hydrological setting, native aquifer geochemistry, and operational site parameters (e.g., source of recharge water and recharge/recovery cycling). Observed mechanisms of geogenic contaminant mobilization during MAR via injection include shifting redox conditions and, to a lesser extent, pH-promoted desorption, mineral solubility, and competitive ligand exchange. The relative importance of these mechanisms depends on various site-specific, operational parameters, including pretreatment of injection water and duration of injection, storage, and recovery phases. This critical review synthesizes findings across case studies in various geochemical, hydrological, and operational settings to better understand controls on arsenic and other geogenic contaminant mobilization and inform the planning and design of future MAR projects to protect groundwater quality. This critical review concludes with an evaluation of proposed management strategies for geogenic contaminants and identification of knowledge gaps regarding fate and transport of geogenic contaminants during MAR.

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Section: Mechanisms Of Contaminant Mobilizationmentioning

confidence: 99%

Mobilization of Arsenic and Other Naturally Occurring Contaminants during Managed Aquifer Recharge: A Critical Review

Fakhreddine

Prommer

Scanlon

et al. 2021

Environ. Sci. Technol.

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“…An increasing use of surrogate models in the field of groundwater contamination and remediation would help lowering the technical barriers in the simulation and increase the trust in technologies that are currently considered very difficult to predict due to the complex interplay between several physical and biogeochemical processes. In fact, complexity is a key feature of subsurface systems where inherently coupled flow, mass transfer processes, chemical and biological reactions control the fate of contaminants (Battistel et al., 2021; Fakhreddine et al., 2016; Guo et al., 2020; Li, 2019; Prommer et al., 2019; Rathi et al., 2017; Steefel et al., 2015; Stolze et al., 2019a, 2019b) and the efficiency of in situ remediation technologies (Ni et al., 2015; Piscopo et al., 2013; Sookhak Lari et al., 2019; Sprocati et al., 2020).…”

Section: Discussionmentioning

confidence: 99%

Integrating Process‐Based Reactive Transport Modeling and Machine Learning for Electrokinetic Remediation of Contaminated Groundwater

Sprocati

Rolle

2021

Water Resources Research

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Advanced reactive transport models of fluid flow and solute transport in subsurface porous media are instrumental for the assessment of contaminant environmental fate and for the design of in situ remediation interventions. However, the increasing complexity of process‐based reactive transport simulators often leads to long runtimes, which poses severe restrictions for tasks that require numerous model evaluations. To overcome this limitation, we demonstrate how machine learning surrogate models, trained on the outputs of a limited number of process‐based reactive transport simulations, can predict the evolution of complex subsurface systems. We focus on electrokinetic enhanced bioremediation of chlorinated solvents in low‐permeability porous media, which is an in situ remediation technology entailing a suite of complex and coupled physical, chemical, and biological processes. A process‐based, multicomponent reactive transport model, capable of describing the key mechanisms of electrokinetic flow and transport, is setup in a two‐dimensional domain. The model accounts for electromigration and electroosmosis, the electrostatic interactions between charged species, the chemistry of the pore water solution, the microbially mediated degradation of the organic compounds, and the dynamics of different degraders. We develop a response surface surrogate framework using an artificial neural network as approximation function and we show that the surrogate model has the capability and the flexibility to capture the complex dynamics of electrokinetic remediation in subsurface porous media and allows computationally efficient model exploration, sensitivity analysis, and uncertainty quantification.

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“…On the one hand, during the oxidative dissolution of As-containing sulfide minerals driven by microbial Fe/S oxidation in acidic environments such as acid mine drainage (AMD) sites, a series of iron/sulfur-containing intermediates and secondary products are formed, e.g., orpiment (As 2 S 3 ), jarosite (M[Fe 3 (OH) 6 (SO 4 ) 2 ], M = K + , Na + , NH 4 + , or H 3 O + ), scorodite (FeAsO 4 ⋅2H 2 O), and schwertmannite [Fe 8 O 8 (OH) 8–2x (SO 4 ) x (where 1 ≤ x ≤ 1.75)], leading to changes in As speciation and occurrence forms due to As adsorption to or coprecipitation with the Fe/S secondary products ( Zhang et al, 2019 ; Tabelin et al, 2020 ; Battistel et al, 2021 ). On the other hand, several acidophilic bacteria and archaea in acidic environments as well as neutrophilic Fe(III)- and sulfate-reducing bacteria (IRB and SRB, e.g., Shewanella and Desulfovibrio , respectively) in pH-neutral and mildly alkaline environments can lead to the reductive dissolution of Fe(III) minerals with the formation of Fe/S secondary products, such as mackinawite (FeS) and siderite (FeCO 3 ), with a release of As species and the reduction of As(V) to As(III) ( Drahota et al, 2013 ; Wang et al, 2016 ; Hedrich and Schippers, 2021 ).…”

Section: Introductionmentioning

confidence: 99%

Correlation Between Fe/S/As Speciation Transformation and Depth Distribution of Acidithiobacillus ferrooxidans and Acidiphilium acidophilum in Simulated Acidic Water Column

et al. 2022

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It is well known that speciation transformations of As(III) vs. As(V) in acid mine drainage (AMD) are mainly driven by microbially mediated redox reactions of Fe and S. However, these processes are rarely investigated. In this study, columns containing mine water were inoculated with two typical acidophilic Fe/S-oxidizing/reducing bacteria [the chemoautotrophic Acidithiobacillus (At.) ferrooxidans and the heterotrophic Acidiphilium (Aph.) acidophilum], and three typical energy substrates (Fe2+, S0, and glucose) and two concentrations of As(III) (2.0 and 4.5 mM) were added. The correlation between Fe/S/As speciation transformation and bacterial depth distribution at three different depths, i.e., 15, 55, and 105 cm from the top of the columns, was comparatively investigated. The results show that the cell growth at the top and in the middle of the columns was much more significantly inhibited by the additions of As(III) than at the bottom, where the cell growth was promoted even on days 24–44. At. ferrooxidans dominated over Aph. acidophilum in most samples collected from the three depths, but the elevated proportions of Aph. acidophilum were observed in the top and bottom column samples when 4.5 mM As(III) was added. Fe2+ bio-oxidation and Fe3+ reduction coupled to As(III) oxidation occurred for all three column depths. At the column top surfaces, jarosites were formed, and the addition of As(III) could lead to the formation of the amorphous FeAsO4⋅2H2O. Furthermore, the higher As(III) concentration could inhibit Fe2+ bio-oxidation and the formation of FeAsO4⋅2H2O and jarosites. S oxidation coupled to Fe3+ reduction occurred at the bottom of the columns, with the formations of FeAsO4⋅2H2O precipitate and S intermediates. The formed FeAsO4⋅2H2O and jarosites at the top and bottom of the columns could adsorb to and coprecipitate with As(III) and As(V), resulting in the transfer of As from solution to solid phases, thus further affecting As speciation transformation. The distribution difference of Fe/S energy substrates could apparently affect Fe/S/As speciation transformation and bacterial depth distribution between the top and bottom of the water columns. These findings are valuable for elucidating As fate and toxicity mediated by microbially driven Fe/S redox in AMD environments.

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Arsenic release and transport during oxidative dissolution of spatially-distributed sulfide minerals

Cited by 41 publications

References 93 publications

Mobilization of Arsenic and Other Naturally Occurring Contaminants during Managed Aquifer Recharge: A Critical Review

Mobilization of Arsenic and Other Naturally Occurring Contaminants during Managed Aquifer Recharge: A Critical Review

Integrating Process‐Based Reactive Transport Modeling and Machine Learning for Electrokinetic Remediation of Contaminated Groundwater

Correlation Between Fe/S/As Speciation Transformation and Depth Distribution of Acidithiobacillus ferrooxidans and Acidiphilium acidophilum in Simulated Acidic Water Column

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