Arsenic in groundwater of the Red River floodplain, Vietnam: Controlling geochemical processes and reactive transport modeling

Arsenic contamination of groundwater continues to threaten the health of millions of people in southeast Asia. The oxidation of organic carbon, coupled to the reductive dissolution of arsenic-bearing iron oxides, is thought to control the release of sediment-bound arsenic into groundwater. However, the cause of the high spatial variability in groundwater arsenic concentrations—which can range from 5 to 500 μg l−1 within distances of a few kilometres—has been uncertain. Here, we combine measurements of sediment age, organic-matter reactivity and water chemistry at four locations along a cross-section of the arsenic-contaminated Red River floodplain in Vietnam to determine the origin of variations in groundwater arsenic concentrations. The burial age of the aquifer sediments, determined using optical stimulated luminescence, ranged from 460 years near the course of the present-day river to 5,900 years at the margin of the floodplain. The groundwater arsenic content and the reactivity of sedimentary organic carbon, determined using radiotracer measurements of the rate of methanogenesis, declined with sediment age. The sedimentary pools of both iron and arsenic also declined with the burial age of the sediments. We suggest that the age of aquifer sediments is a key determinant of groundwater arsenic concentrations. Arsenic contamination of groundwater threatens the health of millions of people in southeast Asia. Measurements in an arsenic-contaminated aquifer in Vietnam point to sediment age as a key determinant of groundwater arsenic concentrations.

Groundwater arsenic concentrations in Vietnam controlled by sediment age

The diverse microbial populations that inhabit pristine aquifers are known to catalyze critical in situ biogeochemical reactions, yet little is known about how the structure and diversity of this subsurface community correlates with and impacts upon groundwater chemistry. Herein we examine 8,786 bacterial and 8,166 archaeal 16S rRNA gene sequences from an array of monitoring wells in the Mahomet aquifer of east-central Illinois. Using multivariate statistical analyses we provide a comparative analysis of the relationship between groundwater chemistry and the microbial communities attached to aquifer sediment along with those suspended in groundwater. Statistical analyses of 16S rRNA gene sequences showed a clear distinction between attached and suspended communities; with iron-reducing bacteria far more abundant in attached samples than suspended, while archaeal clones related to groups associated with anaerobic methane oxidation and deep subsurface gold mines (ANME-2D and SAGMEG-1, respectively) distinguished the suspended community from the attached. Within the attached bacterial community, cloned sequences most closely related to the sulfate-reducing Desulfobacter and Desulfobulbus genera represented 20% of the bacterial community in wells where the concentration of sulfate in groundwater was high (> 0.2 mM), compared to only 3% in wells with less sulfate. Sequences related to the genus Geobacter, a genus containing ferric-iron reducers, were of nearly equal abundance (15%) to the sulfate reducers under high sulfate conditions, however their relative abundance increased to 34% when sulfate concentrations were   0.2 mM sulfate. In the suspended fraction of wells where the concentration of sulfate was between 0.03 and 0.2 mM, the archaeal community was dominated by sequences most closely related to the ANME-2D, a group of archaea known for anaerobically oxidizing methane. Based on available energy (∆GA) estimations, results varied little for both sulfate reduction and methanogenesis throughout all wells studied, but could favor anaerobic oxidation of methane (AOM) in wells containing minimal sulfate and dihydrogen, suggesting AOM coupled with H2-oxidizing organisms such as sulfate or iron reducers could be an important pathway occurring in the Mahomet aquifer. Overall, the results show several distinct factors control the composition of microbial communities in the Mahomet aquifer. Bacteria that respire insoluble substrates such as iron oxides, i.e. Geobacter, comprise a greater abundance of the attached community than the suspended regardless of groundwater chemistry. Differences in community structure driven by the concentration of sulfate point to a clear link between the availability of substrate and the abundance of certain functional groups, particularly iron reducers, sulfate reducers, methanogens, and methanotrophs. Integrating both geochemical and microbiological observations suggest that the relationships between these functional groups could be driven in part by mutualism, especially between ferric-iron and sulfate reducers.

https://link.springer.com/content/pdf/10.1186%2F1471-2180-13-146.pdf

Functional microbial diversity explains groundwater chemistry in a pristine aquifer

In a methanogenic crude oil contaminated aquifer near Bemidji, Minnesota, the decrease in dissolved CH(4) concentrations along the groundwater flow path, along with the positive shift in δ(13) C(CH) (4) and negative shift in δ(13) C(DIC) , is indicative of microbially mediated CH(4) oxidation. Calculations of electron acceptor transport across the water table, through diffusion, recharge, and the entrapment and release of gas bubbles, suggest that these processes can account for at most 15% of the observed total reduced carbon oxidation, including CH(4) . In the anaerobic plume, the characteristic Fe(III)-reducing genus Geobacter was the most abundant of the microbial groups tested, and depletion of labile sediment iron is observed over time, confirming that reduced carbon oxidation coupled to iron reduction is an important process. Electron mass balance calculations suggest that organic carbon sources in the aquifer, BTEX and non-volatile dissolved organic carbon, are insufficient to account for the loss in sediment Fe(III), implying that CH(4) oxidation may also be related to Fe(III) reduction. The results support a hypothesis of Fe(III)-mediated CH(4) oxidation in the contaminated aquifer.

Evidence for iron-mediated anaerobic methane oxidation in a crude oil-contaminated aquifer.

A model for the evolution in water chemistry of an arsenic contaminated aquifer over the last 6000 years, Red River floodplain, Vietnam

Geochemistry at the sulfate reduction–methanogenesis transition zone in an anoxic aquifer—A partial equilibrium interpretation using 2D reactive transport modeling

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Geochemistry at the sulfate reduction–methanogenesis transition zone in an anoxic aquifer—A partial equilibrium interpretation using 2D reactive transport modeling