Abstract:The Monument Valley site, a former uranium mining site located in the state of Arizona in the Southwest USA, has high concentrations of sulfate in groundwater. Stable isotope analysis of S and O for sulfate, in combination with geochemical and hydrogeological data, was used to characterize the sources and fate of sulfate. The results indicate the existence of two discrete sources of sulfate (in excess of baseline levels): sulfuric acid released during ore processing and sulfate generated via sulfide-mineral ox… Show more
“…The δ 34 S of sulfate in the groundwater contaminant plume is different from background due to the impact of sulfate generated from sulfuric acid and associated sulfate salts from mill operation, and reflects the proportional mixing of the two primary sources. The δ 34 S of sulfate for the sulfuric-acid source was determined to be +24.3‰ (Miao et al, 2013b). The value obtained for the baseline δ 34 S of sulfate in the test area of the plume (+16.1‰) prior to the test is consistent with the relative contributions of the two sources (74% from sulfuric acid and 26% from background).…”
Section: Resultsmentioning
confidence: 99%
“…Stable isotope analysis of S and O for sulfate, in combination with geochemical and hydrogeological data, was used recently to characterize the sources and background conditions for sulfate in groundwater at this site (Miao et al, 2013b). Regional baseline concentrations of sulfate in groundwater are low (~20–30 mg/L).…”
Section: Methodsmentioning
confidence: 99%
“…Rates of natural attenuation for nitrate and sulfate in the contaminant plume are slow and minimal, respectively, due to the generally oxidative conditions (Carroll et al, 2009; Miao et al, 2013b). Concentrations of organic carbon in groundwater and the sediment are low.…”
The impact of electron-donor addition on sulfur dynamics for a groundwater system with low levels of metal contaminants was evaluated with a pilot-scale biostimulation test conducted at a former uranium mining site. Geochemical and stable-isotope data collected before, during, and after the test were analyzed to evaluate the sustainability of sulfate reducing conditions induced by the test, the fate of hydrogen sulfide, and the impact on aqueous geochemical conditions. The results of site characterization activities conducted prior to the test indicated the absence of measurable bacterial sulfate reduction. The injection of an electron donor (ethanol) induced bacterial sulfate reduction, as confirmed by an exponential decrease of sulfate concentration in concert with changes in oxidation-reduction potential, redox species, alkalinity, production of hydrogen sulfide, and fractionation of δ34S-sulfate. High, stoichiometrically-equivalent hydrogen sulfide concentrations were not observed until several months after the start of the test. It is hypothesized that hydrogen sulfide produced from sulfate reduction was initially sequestered in the form of iron sulfides until the exhaustion of readily reducible iron oxides associated with the sediment. The fractionation of δ34S for sulfate was atypical, wherein the enrichment declined in the latter half of the experiment. It was conjectured that mixing effects associated with the release of sulfate from sulfate minerals associated with the sediments, along with possible sulfide re-oxidation contributed to this behavior. The results of this study illustrate the biogeochemical complexity that is associated with in-situ biostimulation processes involving bacterial sulfate reduction.
“…The δ 34 S of sulfate in the groundwater contaminant plume is different from background due to the impact of sulfate generated from sulfuric acid and associated sulfate salts from mill operation, and reflects the proportional mixing of the two primary sources. The δ 34 S of sulfate for the sulfuric-acid source was determined to be +24.3‰ (Miao et al, 2013b). The value obtained for the baseline δ 34 S of sulfate in the test area of the plume (+16.1‰) prior to the test is consistent with the relative contributions of the two sources (74% from sulfuric acid and 26% from background).…”
Section: Resultsmentioning
confidence: 99%
“…Stable isotope analysis of S and O for sulfate, in combination with geochemical and hydrogeological data, was used recently to characterize the sources and background conditions for sulfate in groundwater at this site (Miao et al, 2013b). Regional baseline concentrations of sulfate in groundwater are low (~20–30 mg/L).…”
Section: Methodsmentioning
confidence: 99%
“…Rates of natural attenuation for nitrate and sulfate in the contaminant plume are slow and minimal, respectively, due to the generally oxidative conditions (Carroll et al, 2009; Miao et al, 2013b). Concentrations of organic carbon in groundwater and the sediment are low.…”
The impact of electron-donor addition on sulfur dynamics for a groundwater system with low levels of metal contaminants was evaluated with a pilot-scale biostimulation test conducted at a former uranium mining site. Geochemical and stable-isotope data collected before, during, and after the test were analyzed to evaluate the sustainability of sulfate reducing conditions induced by the test, the fate of hydrogen sulfide, and the impact on aqueous geochemical conditions. The results of site characterization activities conducted prior to the test indicated the absence of measurable bacterial sulfate reduction. The injection of an electron donor (ethanol) induced bacterial sulfate reduction, as confirmed by an exponential decrease of sulfate concentration in concert with changes in oxidation-reduction potential, redox species, alkalinity, production of hydrogen sulfide, and fractionation of δ34S-sulfate. High, stoichiometrically-equivalent hydrogen sulfide concentrations were not observed until several months after the start of the test. It is hypothesized that hydrogen sulfide produced from sulfate reduction was initially sequestered in the form of iron sulfides until the exhaustion of readily reducible iron oxides associated with the sediment. The fractionation of δ34S for sulfate was atypical, wherein the enrichment declined in the latter half of the experiment. It was conjectured that mixing effects associated with the release of sulfate from sulfate minerals associated with the sediments, along with possible sulfide re-oxidation contributed to this behavior. The results of this study illustrate the biogeochemical complexity that is associated with in-situ biostimulation processes involving bacterial sulfate reduction.
“…Our irrigated plantings did not remove sulfate in the subpile soil, probably because redox conditions in the vadose zone did not favor sulfate reduction (Miao et al , ). However, the plantings did isolate sulfate in the subpile soil.…”
Section: Discussionmentioning
confidence: 99%
“…The goals of our research at Monument Valley were, first, to find ways to prevent further migration of contaminants from the subpile soil into groundwater; second, to prevent further spread of the groundwater plume; and third, to remove the contaminants. Previous studies characterized the movement of contaminants in the Monument Valley plume and evaluated options for remediation (Jordan et al , ; Carroll et al , ; Borden et al , ; Miao et al , , ). This study evaluated in situ bioremediation options (native plants and microbial processes) to isolate and remediate ammonium, nitrate, and sulfate remaining in the subpile soil.…”
We combined phytoremediation and soil microbial nitrification and denitrification cycles to reduce nitrate and ammonium levels at a former uranium mill site near Monument Valley, Arizona. Ammonia used in uranium extraction was present throughout the soil profile. Sulfate, applied as sulfuric acid to solubilize uranium, was also present in the soil. These contaminants were leaching from a denuded area where a tailings pile had been removed and were migrating away from the site in groundwater. We planted the source area with two deep-rooted native shrubs, Atriplex cansescens and Sarcobatus vermiculatus, and irrigated transplants for 11 years at 20% the rate of potential evapotranspiration to stimulate growth, then discontinued irrigation for 4 years. Over 15 years, total nitrogen levels dropped 82%, from 347 to 64 mg kg À1 . Analysis of δ 15 N supported our hypothesis that coupled microbial nitrification and denitrification processes were responsible for the loss of N. Soil sulfate levels changed little; however, evapotranspiration reduced sulfate leaching into the aquifer. For arid sites where traditional pump-and-treat methods are problematic, the Monument Valley data suggest that alternatives that incorporate native plants and rely on vadose zone biogeochemistry and hydrology could be a sustainable remediation for nitrogen contaminated soil.
Gypsum enriched aquifers (GEA) along with intensive agriculture regions (IAR) in semi-arid regions are responsible for very high amount of sulphate and nitrate in many groundwater systems of the world, respectively. However, in such regions, the problem of nitrate pollution and its associated health risk has been increasing and emerging as a global issue. But along with nitrate, sulphate contamination and its potential health risks are often neglected throughout the world in these regions. Therefore, considering sulphate along with nitrate as major threat to water quality in such regions, this study aimed to characterize hydrochemistry, factors controlling groundwater quality and assessment of risk to human health. To accomplish this objective, 116 groundwater samples were collected over pre-monsoon (PRM) and post-monsoon (POM) (2019) seasons in Bemetara district. As per Bureau of Indian standards (BIS) for drinking, SO 4 2− (28 and 19%) and NO 3 − (7 and 35%) exceeded the permissible limits in PRM and POM seasons respectively; thereby groundwater was not suitable for drinking. SO 4 2− and NO 3 − pollution sources were identi ed and mainly attributed to gypsum dissolution and agricultural activities as well as domestic sewage discharge, respectively. In addition, SO 4 2− and NO 3 − risk assessment results shows that total 20-46% of all samples surpassed the permissible limit (HQ = 1) risk to children and adult, over both seasons. To ensure drinking water security in this region, sustainable management of agricultural activities and treatment should be done to reduce the potential health risks due to SO 4 2− and NO 3 − .
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