Geochemistry of Tungsten and Arsenic in Aquifer Systems: A Comparative Study of Groundwaters from West Bengal, India, and Nevada, USA

Mohajerin, T. Jade; Neal, A.; Telfeyan, Katherine; Sasihharan, Sankar M.; Ford, Sophie; Yang, Ningfang; Chevis, Darren A.; Grimm, Deborah A.; Datta, Saugata; White, Christopher D.; Johannesson, Karen H.

doi:10.1007/s11270-013-1792-x

Cited by 29 publications

(7 citation statements)

References 62 publications

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“…Tungsten, Mo, Fe, and Mn concentrations were quantified in surface and pore waters from the Terrebonne Bay study site using high resolution (magnetic sector) inductively coupled plasma mass spectrometry (HR-ICP-MS, Thermo Fisher Element II) following procedures described previously (Clausen et al, 2010;Johannesson et al, 2013;Mohajerin et al, 2014b;Yang et al, 2015). Here, all sample handling was conducted in a class 100 cleanroom, before introduction to the HR-ICP-MS for quantification.…”

Section: Trace Metal Analysismentioning

confidence: 99%

Tungsten–molybdenum fractionation in estuarine environments

Mohajerin

Helz

Johannesson

2016

Geochimica et Cosmochimica Acta

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Dissolved tungsten (W) and molybdenum (Mo) concentrations were measured in surface waters and sediment pore waters of Terrebonne Bay, a shallow estuary in the Mississippi River delta, to investigate the biogeochemical processes that fractionate these Group 6 elements relative to one another during transit from weathering to sedimentary environments. Although many of the chemical properties of W and Mo are similar, the two elements behave autonomously, and the fractionation mechanisms are only partly understood. In sulfidic pore waters, dissolved Mo is depleted relative to river water-seawater mixtures, whereas dissolved W is >10-fold enriched. Reductive dissolution of poorly crystalline phases like ferrihydrite, which is a preferential host of W relative to Mo in grain coatings on river-borne particles, can explain the dissolved W enrichment. Dissolved W becomes increasingly enriched as H 2 S(aq) rises above about 60 μM due to transformation of WO 4 2to thiotungstates as well as to additional reductive dissolution of phases that host W. In contrast, as rising sulfide transforms MoO 4 2to thiomolybdates in pore waters, dissolved Mo is suppressed, probably owing to equilibration with an Fe-Mo-S phase. This putative phase appears to control the aqueous ion product, Q = [Fe 2+ ][MoS 4 2-] 0.6 [H 2 S 0 ] 0.4 /[H + ] 0.8 , at a value of 10-7.78. Concentrations of dissolved W and Mo in pore waters bear no relation to concentrations in surface waters of the same salinity. In surface waters, dissolved Mo is nearly conserved in the estuarine mixing zone. Dissolved W appears also to be conserved except for several cases where W may have been enhanced by exchange with underlying, W-rich pore waters. With increasing salinity, the molar Mo/W ratio rises from about 10 to about 1000 in surface waters whereas it is mostly <10 in underlying pore waters and in highly sulfidic pore waters is mostly near 1. Differences in two chemical properties may account for this fractionation of Mo with respect to W; Mo VI is more susceptible to reduction than W VI , but the latter is more prone to adopting octahedral coordination. We propose that the first difference facilitates Mo but not W precipitation in sulfidic sediments, whereas the second explains tungsten's proportionately greater sequestration on river-borne particles and its subsequent release to sulfidic pore waters after the particles are deposited in the delta and become subject to reductive dissolution during diagenesis. Electronic Annex Click here to download Electronic Annex: Revised Electronic Annex_KHJ.docx *Revised Manuscript (marked MS Word) Click here to download Source or Other Companion File: Revised_GRH_KHJ.docx

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Section: Trace Metal Analysismentioning

confidence: 99%

Tungsten–molybdenum fractionation in estuarine environments

Mohajerin

Helz

Johannesson

2016

Geochimica et Cosmochimica Acta

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“…Tungsten (W) is both a naturally occurring element and an anthropogenic contaminant, that is increasingly released into the environment as a result of its use in a wide range of industrial products that require high heat resistance and mechanical toughness, such as light bulbs, bullets and many metal alloy (Koutsospyros et al, 2006). Recent reports of W contamination in groundwater and soil systems have raised concerns about its potential toxicity to plants, animals and humans (Kennedy et al, 2012;Tuna et al, 2012;Datta et al, 2017;Lindsay et al, 2017;Mohajerin et al, 2014a;2014b;Oburger et al, 2018), and because of its risk to natural systems, W has been listed as an emerging contaminant by the United States Environmental Protection Agency (EPA) (https://www.epa.gov/fedfac/technical-fact-sheet-tungsten). Despite its listed status however, the biogeochemical behavior and potential risks of W to human and environmental health are still poorly understood.…”

Section: Introductionmentioning

confidence: 99%

Natural organic matter decreases uptake of W(VI), and reduces W(VI) to W(V), during adsorption to ferrihydrite

et al. 2020

Chemical Geology

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Tungsten is both naturally occurring and an anthropogenically released contaminant metal in soils, sediments and water systems that typically exits as the soluble tungstate oxyanions, W(VI)O4 2− . Tungsten mobility and fate are strongly dependent on the adsorption of tungstate to mineral surfaces. However, environmental mineral surfaces are commonly coated with natural organic matter (NOM), and the role of this coating in the tungsten adsorption process, and thus in controlling tungsten reactivity and transport, is unclear. This study investigates W(VI) adsorption to ferrihydrite (Fh), a ubiquitous iron (hydr)oxide in soils and sediments, both in the absence and presence of humic acid (HA), a widely occurring type of NOM, using batch experiments coupled with spectroscopic and thermodynamic techniques. Kinetic results indicate that access to the adsorption sites for W(VI) on the organomineral surfaces is limited when Fh is coprecipitated with HA. Commensurate with this observation, batch experiments show that HA decreases W(VI) adsorption to Fh over a wide pH range (4-11), and this inhibitory effect is more pronounced at higher HA concentration. X-ray photoelectron spectroscopy (XPS) measurements demonstrate the formation of inner-sphere type W complexes on both the Fh and HA fraction of the Fh-HA binary composite. In particular, ~40% of the adsorbed W(VI) species is reduced to W(V) in the presence of HA. Attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR) results show the presence of poly tungstate species on Fh, particularly at lower pH and in the presence of HA. Isothermal titration calorimetry shows that W(VI) adsorption to Fh is an exothermic process both in the presence and absence of HA, and that process is accompanied by a positive entropy. The findings of this work suggest that NOM not only mobilizes tungstate but also reduces tungstate from W(VI) to W(V) at environmental iron (hydr)oxide-water interfaces, which is of significance for evaluating the migration and bioavailability of tungsten in both natural and contaminated environments.

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“…As far as we are aware, W in water has not been measured in previous studies in Bangladesh. Arsenic and W commonly co-occur in groundwater in parts of the United States, India and China (Gao et al, 2018; Mohajerin et al, 2014). For instance, a cluster between urinary As, W and U was found in the Strong Heart Study, a multi-center study in American Indian communities in the United States (Pang et al, 2016).…”

Section: Discussionmentioning

confidence: 99%

Urinary metals and metal mixtures in Bangladesh: Exploring environmental sources in the Health Effects of Arsenic Longitudinal Study (HEALS)

Sanchez

Slavkovich

LoIacono

et al. 2018

Environment International

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Introduction: Environmental exposure to toxic metals and metalloids is pervasive and occurs from multiple sources. The Health Effects of Arsenic Longitudinal Study (HEALS) is an ongoing prospective study predominantly focused on understanding health effects associated with arsenic exposure from drinking water. The goal of this project was to measure a suite of elements in urine to better understand potential exposure patterns and to identify common environmental sources of exposure among this semi-rural Bangladeshi population. Methods: In a random sample of 199 adult HEALS participants (50% female), the concentrations of 15 urinary elements (As, Ba, Cd, Co, Cs, Cu, Mn, Mo, Ni, Pb, Se, Sr, Tl, W, Zn) were assessed by Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) to assess commonalities with sociodemographic characteristics and potential sources of exposure. We used principal component analysis (PCA) with varimax normalized rotations, and hierarchical cluster analysis (CA), using Ward’s method with Euclidean distances, to evaluate these relationships. Results: PCA and CA showed similar patterns, suggesting 6 principal components (PC) and 5 clusters: 1)(PC: Sr-Ni-Cs/ CA: Sr-Ni-Co; 2) Pb-Tl/Pb-Tl-Se-Cs; 3) As-Mo-W/As-Mo-W; 4) Ba-Mn/Ba-Mn; 5) Cu-Zn/Cu-Zn-Cd; and 6) Cd. There was a strong significant association between the As-Mo-W PC/cluster and water arsenic levels (p<0.001) and between the Cd PC and betel nut use (p=0.003). The Sr-Ni-Cs PC was not related to any of the socio-demographic characteristics investigated, including smoking status and occupation. The first PC, Sr-Ni-Cs, explained 21% of the variability; the third PC, As-Mo-W, explained 12.5% of the variability; and the sixth PC, Cd, explained 10% of the variability. Day laborers appeared to have the highest exposure. Conclusions: Groundwater and betel nut use are likely important sources of metal and metalloid exposure in this population. These findings will guide future exposure assessment research in Bangladesh and future epidemiologic research investigating the degree to which metal mixtures play a role in disease development.

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Geochemistry of Tungsten and Arsenic in Aquifer Systems: A Comparative Study of Groundwaters from West Bengal, India, and Nevada, USA

Cited by 29 publications

References 62 publications

Tungsten–molybdenum fractionation in estuarine environments

Tungsten–molybdenum fractionation in estuarine environments

Natural organic matter decreases uptake of W(VI), and reduces W(VI) to W(V), during adsorption to ferrihydrite

Urinary metals and metal mixtures in Bangladesh: Exploring environmental sources in the Health Effects of Arsenic Longitudinal Study (HEALS)

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