Carbon and methane cycling in arsenic-contaminated aquifers

Stopelli, Emiliano; Duyen, Vu Thi; Prommer, Henning; Głodowska, Martyna; Kappler, Andreas; Schneider, M.; Eiche, Elisabeth; Lightfoot, Alexandra; Schubert, Carsten J.; Trang, P. K.; Viet, Pham Hung; Kipfer, Rolf; Winkel, Lenny H. E.; Berg, Michael; members, AdvectAs team

doi:10.1016/j.watres.2021.117300

Cited by 29 publications

(28 citation statements)

References 55 publications

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“…Only low abundances of genes related to methane oxidation ( mmoXYBC , average FPKM from 0.11 to 1.23) and undetectable genes underpinning methanogenic processes ( mcrABC ) were found in our datasets, potentially due to the significant downregulation of the key enzymes regulating methanogenesis by ammonium . Moreover, genes related to methane oxidation did not have observable Spearman correlations with those associated with Fe(III) reduction genes, although methane oxidation coupled As-bearing Fe(III) reduction was reported as one of the key As-mobilizing pathways in other high-As groundwaters. ,, Collectively, our data suggest that methane oxidation may have limited contributions to Fe(III) reduction in the study area.…”

Section: Resultsmentioning

confidence: 69%

“…92 Moreover, genes related to methane oxidation did not have observable Spearman correlations with those associated with Fe(III) reduction genes, although methane oxidation coupled As-bearing Fe(III) reduction was reported as one of the key As-mobilizing pathways in other high-As groundwaters. 17,18,93 Collectively, our data suggest that methane oxidation may have limited contributions to Fe(III) reduction in the study area.…”

Section: ■ Materials and Methodsmentioning

confidence: 70%

“…High-arsenic (As) groundwater (As > 10 μg/L, WHO guideline) is placing millions of people across the world under the risk of severe health problems, including skin, lung, bladder, liver, and kidney cancers. , Interactions between indigenous aquifer microbial communities and associated hydro-geochemical processes are key to understanding As behavior in natural groundwater systems . The microbially mediated reductive dissolution of As-bearing Fe(III) oxides (the dominant As sink in aquifer sediments) is the most commonly accepted mechanism of groundwater As enrichment. ,− Multiple electron donors can support the microbial reduction of Fe(III) oxides, including organic matter, elemental sulfur (S 0 ), , ammonium, and methane, which have all been reported in high-As aquifers. ,− Given the coexistence of these potential electron donors for microbial Fe(III) oxide reduction in natural groundwater systems, groundwater As enrichment is tightly interconnected with the biogeochemical transformations of C, N, S, and Fe. ,, …”

Section: Introductionmentioning

confidence: 99%

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Genome-Resolved Metagenomic Analysis of Groundwater: Insights into Arsenic Mobilization in Biogeochemical Interaction Networks

Xiu

Nixon

et al. 2022

Environ. Sci. Technol.

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Section: Resultsmentioning

confidence: 69%

Section: ■ Materials and Methodsmentioning

confidence: 70%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Genome-Resolved Metagenomic Analysis of Groundwater: Insights into Arsenic Mobilization in Biogeochemical Interaction Networks

Xiu

Nixon

et al. 2022

Environ. Sci. Technol.

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“…The concentration of dissolved Fe 2+ is also high (10 to 20 mg/L) indicating strongly reducing conditions (van Geen et al, 2013). Furthermore, the Holocene aquifer is characterized by nearly flammable CH4 concentrations (>50 mg/L) (Postma et al, 2017;Stopelli et al, 2021). Afterward, all samples were stored at 4°C anoxically in the dark until further use.…”

Section: Study Site and Sediment Sample Collectionmentioning

confidence: 99%

Nitrate leaching and its implication for Fe and As mobility in a Southeast Asian aquifer

Głodowska

Smith

et al. 2022

Preprint

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The drinking water quality of millions of people in South and Southeast Asia is at risk due to arsenic (As) contamination of groundwater and insufficient access to water treatment facilities. Intensive use of nitrogen (N) fertilizer increases the possibility of nitrate (NO3-) leaching into aquifers, yet very little is known about how the N cycle will interact with and affect the iron (Fe) and As mobility in aquifers. We hypothesized that input of NO3- into highly methanogenic aquifers can stimulate nitrate-dependent anaerobic methane oxidation (N-DAMO) and subsequently help to remove NO3- and decrease CH4 emission. We, therefore, investigated the effects of N input into aquifers and its effect on Fe and As mobility, by running a set of microcosm experiments using aquifer sediment from Van Phuc, Vietnam supplemented with 15NO3- and 13CH4. Additionally, we assessed the effect of N-DAMO by inoculating the sediment with two different N-DAMO enrichment cultures (N-DAMO(O) and N-DAMO(V)). We found that native microbial communities and both N-DAMO enrichments could efficiently consume nearly 5 mM NO3- in 5 days. In an uninoculated setup, NO3- was preferentially used over Fe(III) as an electron acceptor and consequently inhibited Fe(III) reduction and As mobilization. The addition of N-DAMO(O) and N-DAMO(V) enrichment cultures led to substantial Fe(III) reduction followed by the release of Fe2+ (0.190 mM and 0.350 mM, respectively) and buildup of sedimentary Fe(II) (11.20 mM and 10.91 mM, respectively) at the end of the experiment (day 64). Only in the N-DAMO(O) inoculated setup, As was mobilized (27.1 ug/L), while in the setup inoculated with N-DAMO(V) a significant amount of Mn (24.15 mg/L) was released to the water. Methane oxidation and 13CO2 formation were observed only in the inoculated setups, suggesting that the native microbial community did not have sufficient potential for N-DAMO. An increase of NH4+ implied that dissimilatory nitrate reduction to ammonium (DNRA) took place in both inoculated setups. The archaeal community in all treatments was dominated by Ca. Methanoperedens while the bacterial community consisted largely of various denitrifiers. Overall, our results suggest that input of N fertilizers to the aquifer decreases As mobility and that CH4 cannot serve as an electron donor for the native NO3- reducing community.

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“…Arsenic is serious contaminant affecting many aquifers around the world that can be influenced by aquifer-aquitard exchange. Such exchange is increasingly being challenged as a contributing factor toward As mobilization in contaminated aquifers, with several studies either confirming or anticipating a significant input or exchange of solutes at the aquitard-aquifer interface (McMahon & Chapelle, 1991;McMahon, 2001;Mihajlov et al, 2020;Stopelli et al, 2020Stopelli et al, , 2021. This exchange further offers to be a contributing explanation toward the particularly high and heterogeneous As concentrations often observed in affected aquifers (e.g., Smedley & Kinniburgh, 2002;Van Geen et al, 2006;Wallis et al, 2020).…”

mentioning

confidence: 99%

Noble gases in aquitard provide insight into underlying subsurface stratigraphy and free gas formation

Lightfoot

Stopelli

Berg

et al. 2022

Vadose Zone Journal

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Biogeochemical gas production resulting in free gas phase formation can severely affect groundwater and solute transport in aquifers. Such gas-water interactions are important in aquifers affected by geogenic As, which are commonly associated with biogeochemical CH 4 production. Additionally, the influence of aquitards on As concentrations in contaminated aquifers has recently been challenged. These observations prompted the analysis through a heterogeneous aquitard overlying a high CH 4 −gas-producing zone of an As-contaminated aquifer. A sediment core taken through the aquitard was analyzed for noble gases to assess how the aquitard physically contributes to the underlying gas production. Results reveal that the aquitard pore space is unsaturated in two separate layers resulting in hanging pore water constrained by an air-like gas phase. This interlayering of unsaturated and saturated zones identifies the aquitard's stratigraphy as key in determining hydrostatic pressure-a main control of free gas formation (i.e., CH 4 ) in the underlying aquifer. The partly unsaturated conditions reduce the hydrostatic pressure by 30% compared with fully saturated conditions. To our knowledge, this is the first study applying noble gases to examine the influence of an aquitards physical state on gas production in an underlying aquifer. Further, such partly unsaturated sediment layers of low conductivity might provide preferential pathways for periodic water flow, fostering aquitard-aquifer solute transport. Groundwater samples additionally collected throughout the study site confirm more widespread degassing than previously reported. Up to 90% of the expected atmospheric noble gas concentrations is lost from groundwater immediately below the investigated sediment core. INTRODUCTIONNoble gases are increasingly being applied as reliable geochemical tracers in aquatic sediments to investigate the dynamics of fluids and gases in the sediment pore space.

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Carbon and methane cycling in arsenic-contaminated aquifers

Cited by 29 publications

References 55 publications

Genome-Resolved Metagenomic Analysis of Groundwater: Insights into Arsenic Mobilization in Biogeochemical Interaction Networks

Genome-Resolved Metagenomic Analysis of Groundwater: Insights into Arsenic Mobilization in Biogeochemical Interaction Networks

Nitrate leaching and its implication for Fe and As mobility in a Southeast Asian aquifer

Noble gases in aquitard provide insight into underlying subsurface stratigraphy and free gas formation

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