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Model-Based Analysis of Arsenic Immobilization via Iron Mineral Transformation under Advective Flows.

ABSTRACT: Recent laboratory studies have demonstrated that coinjection of nitrate and Fe(II) (as ferrous sulfate) to As-bearing sediments can produce an Fe mineral assemblage containing magnetite capable of immobilizing advected As under a relatively wide range of aquifer conditions. This study combined laboratory findings with process-based numerical modeling approaches, to quantify the observed Fe mineral (trans)formation and concomitant As partitioning dynamics and to assess potential nitrate-Fe(II) remediation strategies for field implementation. The model development was guided by detailed solution and sediment data from our well-controlled column experiment. The modeling results demonstrated that the fate of As during the experiment was primarily driven by ferrihydrite formation and reductive transformation and that different site densities were identified for natural and neoformed ferrihydrite to explain the observations both before and after nitrate-Fe(II) injection. Our results also highlighted that when ferrihydrite was nearing depletion, As immobilization ultimately relied on the presence of magnetite. On the basis of the column model, field-scale predictive simulations were conducted to illustrate the feasibility of the nitrate-Fe(II) strategy for intercepting advected As from a plume. The predictive simulations, which suggested that long-term As immobilization was feasible, favored a scenario that maintains high dissolved Fe(II) concentration during injection periods and thereby converts ferrihydrite to magnetite.

SUBMITTER: Sun J

PROVIDER: S-EPMC6429028 | biostudies-literature | 2018 Aug

REPOSITORIES: biostudies-literature

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Model-Based Analysis of Arsenic Immobilization via Iron Mineral Transformation under Advective Flows.

Sun Jing J Prommer Henning H Siade Adam J AJ Chillrud Steven N SN Mailloux Brian J BJ Bostick Benjamin C BC

Environmental science & technology 20180808 16

Recent laboratory studies have demonstrated that coinjection of nitrate and Fe(II) (as ferrous sulfate) to As-bearing sediments can produce an Fe mineral assemblage containing magnetite capable of immobilizing advected As under a relatively wide range of aquifer conditions. This study combined laboratory findings with process-based numerical modeling approaches, to quantify the observed Fe mineral (trans)formation and concomitant As partitioning dynamics and to assess potential nitrate-Fe(II) re ...[more]

PMID: 30039966

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Project description:High levels of arsenic in groundwater and drinking water are a major health problem. Although the processes controlling the release of As are still not well known, the reductive dissolution of As-rich Fe oxyhydroxides has so far been a favorite hypothesis. Decoupling between arsenic and iron redox transformations has been experimentally demonstrated, but not quantitatively interpreted. Here, we report on incubation batch experiments run with As(V) sorbed on, or co-precipitated with, 2-line ferrihydrite. The biotic and abiotic processes of As release were investigated by using wet chemistry, X-ray diffraction, X-ray absorption and genomic techniques. The incubation experiments were carried out with a phosphate-rich growth medium and a community of Fe(III)-reducing bacteria under strict anoxic conditions for two months. During the first month, the release of Fe(II) in the aqueous phase amounted to only 3% to 10% of the total initial solid Fe concentration, whilst the total aqueous As remained almost constant after an initial exchange with phosphate ions. During the second month, the aqueous Fe(II) concentration remained constant, or even decreased, whereas the total quantity of As released to the solution accounted for 14% to 45% of the total initial solid As concentration. At the end of the incubation, the aqueous-phase arsenic was present predominately as As(III) whilst X-ray absorption spectroscopy indicated that more than 70% of the solid-phase arsenic was present as As(V). X-ray diffraction revealed vivianite Fe(II)3(PO4)2.8H2O in some of the experiments. A biogeochemical model was then developed to simulate these aqueous- and solid-phase results. The two main conclusions drawn from the model are that (1) As(V) is not reduced during the first incubation month with high Eh values, but rather re-adsorbed onto the ferrihydrite surface, and this state remains until arsenic reduction is energetically more favorable than iron reduction, and (2) the release of As during the second month is due to its reduction to the more weakly adsorbed As(III) which cannot compete against carbonate ions for sorption onto ferrihydrite. The model was also successfully applied to recent experimental results on the release of arsenic from Bengal delta sediments.

Project description:Nitrate can be reduced to other N inorganic species via denitrification and incorporated into organic matter by immobilization; however, the effect of biotic/abiotic and redox condition on immobilization and denitrification processes from a single system are not well documented. We hypothesize nitrate (NO3-) transformation pathways leading to the formation of dissolved- and solid-phase organic N are predominantly controlled by abiotic reactions, but the formation of soluble inorganic N species is controlled by redox condition. In this study, organic matter in the form of leaf compost (LC) was spiked with 15NO3- and incubated under oxic/anoxic and biotic/abiotic conditions at pH 6.5. We seek to understand how variations in environmental conditions impact NO3- transformation pathways through laboratory incubations. We find production of NH4+ is predominantly controlled by redox whereas NO3- conversion to dissolved organic nitrogen (DON) and immobilization in solid-phase N are predominantly controlled by abiotic processes. Twenty % of added 15N-NO3- was incorporated into DON under oxic conditions, with abiotic processes accounting for 85% of the overall incorporation. Nitrogen immobilization processes resulted in N concentrations of 4.1-6.6 μg N (g leaf compost)-1, with abiotic processes accounting for 100% and 66% of the overall (biotic+abiotic) N immobilization under anoxic and oxic conditions, respectively. 15N-NMR spectroscopy suggests 15NO3- was immobilized into amide/aminoquinones and nitro/oxime under anoxic conditions. A fraction of the NH4+ was produced abiotically under anoxic conditions (~10% of the total NH4+ production) although biotic organic N mineralization contributed to most of NH4+ production. Our results also indicate Fe(II) did not act as an electron source in biotic-oxic incubations; however, Fe(II) provided electrons for NO3- reduction in biotic-anoxic incubations although it was not the sole electron source. It is clear that, under the experimental conditions of this investigation, abiotic and redox processes play important roles in NO3- transformations. As climatic conditions change (e.g., frequency/intensity of rainfall), abiotic reactions that shift transformation pathways and N species concentrations from those controlled by biota might become more prevalent.

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Model-Based Analysis of Arsenic Immobilization via Iron Mineral Transformation under Advective Flows.

Publications

Model-Based Analysis of Arsenic Immobilization via Iron Mineral Transformation under Advective Flows.

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