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Results for “Frontiers in Environmental Chemistry”

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USGS2023

Using mercury stable isotope fractionation to identify the contribution of historical mercury mining sources present in downstream water, sediment and fish

Ecosystems downstream of mercury (Hg) contaminated sites can be impacted by both localized releases as well as Hg deposited to the watershed from atmospheric transport. Identifying the source of Hg in water, sediment, and fish downstream of contaminated sites is important for determining the effectiveness of source-control remediation actions. This study uses measurements of Hg stable isotopes in soil, sediment, water, and fish to differentiate between Hg from an abandoned Hg mine from non-mine-related sources. The study site is located within the Willamette River watershed (Oregon, United States), which includes free-flowing river segments and a reservoir downstream of the mine. The concentrations of total-Hg (THg) in the reservoir fish were 4-fold higher than those further downstream (>90 km) from the mine site in free-flowing sections of the river. Mercury stable isotope fractionation analysis showed that the mine tailings (δ 202 Hg: −0.36‰ ± 0.03‰) had a distinctive isotopic composition compared to background soils (δ 202 Hg: −2.30‰ ± 0.25‰). Similar differences in isotopic composition were observed between stream water that flowed through the tailings (particulate bound δ 202 Hg: −0.58‰; dissolved: −0.91‰) versus a background stream (particle-bound δ 202 Hg: −2.36‰; dissolved: −2.09‰). Within the reservoir sediment, the Hg isotopic composition indicated that the proportion of the Hg related to mine-release increased with THg concentrations. However, in the fish samples the opposite trend was observed—the degree of mine-related Hg was lower in fish with the higher THg concentrations. While sediment concentrations clearly show the influence of the mine, the relationship in fish is more complicated due to differences in methylmercury (MeHg) formation and the foraging behavior of different fish species. The fish tissue δ 13 C and Δ 199 Hg values indicate that there is a higher influence of mine-sourced Hg in fish feeding in a more sediment-based food web and less so in planktonic and littoral-based food webs. Identifying the relative proportion of Hg from local contaminated site can help inform remediation decisions, especially when the relationship between total Hg concentrations and sources do not show similar covariation between abiotic and biotic media.

Oregon↗

USGS2019

Groundwater and surface-water resources near Red Fleet Reservoir, Uintah County, Utah

Red Fleet Reservoir in Uintah County, Utah, is an approximately 26,000 acre-foot (acre-ft) on-channel reservoir in the Big Brush Creek drainage on the south slopes of the Uinta Mountains. It is operated primarily for irrigation needs while providing a supplemental drinking-water supply to the Vernal, Utah area. Red Fleet Reservoir, which was operated by the Bureau of Reclamation and the Uintah Water Conservancy District through 2015, began storing water in May 1980. The reservoir is on southward dipping Mesozoic lithologies ranging from Jurassic to Cretaceous in age. The Nugget and Frontier Sandstone aquifers are the targeted units in this investigation, which is to characterize groundwater conditions that exist in each sandstone aquifer and how they interact with Red Fleet Reservoir. Groundwater levels were measured in six wells and one spring in the Nugget Sandstone and the Frontier Sandstone aquifers. Water levels in the Nugget Sandstone aquifer were 35–70 feet above the maximum stage of Red Fleet Reservoir on the west and east banks. Water levels in the Frontier Sandstone aquifer were 15–30 feet below the observed stage of Red Fleet Reservoir on the west bank during the study period. A water budget was calculated for Red Fleet Reservoir between May 1980 and December 2015. During this period, 1,050,000 acre-ft of water from Big Brush Creek discharged into the reservoir, while 993,000 acre-ft of water was released downstream of Red Fleet Dam. Total evaporation from May 1980 through December 2015 was about 52,000 acre-ft, while total precipitation over the same period was about 12,000 acre-ft. From May 1980 through December 2015, the total pumped volume of water from the Tyzack Pump Station, at the base of Red Fleet Dam, was about 42,000 acre-ft. Total groundwater discharge to Red Fleet Reservoir from 1980 through 2015 was about 40,000 acre-ft. Water was sampled from four wells and from the inflow arm of Red Fleet Reservoir, and analyzed for major-ion chemistry, select trace metals, nutrients, and environmental tracers. Water sampled from the Nugget Sandstone aquifer yielded good-quality water with dissolved-solids concentrations of less than 200 milligram per liter, and no trace elements above the Environmental Protection Agency drinking-water standards. Water sampled from the Frontier Sandstone aquifer yielded poor-quality water with dissolved-solids concentrations of about 2,150 milligrams per liter with trace elements approaching drinking-water standards for arsenic. Dissolved noble gases used to identify recharge elevations and temperatures for groundwater indicate that water in the Nugget Sandstone aquifer likely recharged at a high altitude and low temperature, and not locally because of interaction with Red Fleet Reservoir. The Frontier Sandstone aquifer is likely recharged at low elevation and at temperatures similar to those observed at Red Fleet Reservoir.

Utah↗

USGS2016

Environmental drivers of differences in microbial community structure in crude oil reservoirs across a methanogenic gradient

Stimulating in situ microbial communities in oil reservoirs to produce natural gas is a potentially viable strategy for recovering additional fossil fuel resources following traditional recovery operations. Little is known about what geochemical parameters drive microbial population dynamics in biodegraded, methanogenic oil reservoirs. We investigated if microbial community structure was significantly impacted by the extent of crude oil biodegradation, extent of biogenic methane production, and formation water chemistry. Twenty-two oil production wells from north central Louisiana, USA, were sampled for analysis of microbial community structure and fluid geochemistry. Archaea were the dominant microbial community in the majority of the wells sampled. Methanogens, including hydrogenotrophic and methylotrophic organisms, were numerically dominant in every well, accounting for, on average, over 98% of the total Archaea present. The dominant Bacteria groups were Pseudomonas, Acinetobacter , Enterobacteriaceae, and Clostridiales, which have also been identified in other microbially-altered oil reservoirs. Comparing microbial community structure to fluid (gas, water, and oil) geochemistry revealed that the relative extent of biodegradation, salinity, and spatial location were the major drivers of microbial diversity. Archaeal relative abundance was independent of the extent of methanogenesis, but closely correlated to the extent of crude oil biodegradation; therefore, microbial community structure is likely not a good sole predictor of methanogenic activity, but may predict the extent of crude oil biodegradation. However, when the shallow, highly biodegraded, low salinity wells were excluded from the statistical analysis, no environmental parameters could explain the differences in microbial community structure. This suggests that the microbial community structure of the 5 shallow, up-dip wells was different than the 17 deeper, down-dip wells. Also, the 17 down-dip wells had statistically similar microbial communities despite significant changes in environmental parameters between oil fields. Together, this implies that no single microbial population is a reliable indicator of a reservoir's ability to degrade crude oil to methane, and that geochemistry may be a more important indicator for selecting a reservoir suitable for microbial enhancement of natural gas generation.

Louisiana↗

USGS2021

Integrating high-resolution coastal acidification monitoring data across seven United States estuaries

Beginning in 2015, the United States Environmental Protection Agency’s (EPA’s) National Estuary Program (NEP) started a collaboration with partners in seven estuaries along the East Coast (Barnegat Bay; Casco Bay), West Coast (Santa Monica Bay; San Francisco Bay; Tillamook Bay), and the Gulf of Mexico (GOM) Coast (Tampa Bay; Mission-Aransas Estuary) of the United States to expand the use of autonomous monitoring of partial pressure of carbon dioxide ( p CO 2 ) and pH. Analysis of high-frequency (hourly to sub-hourly) coastal acidification data including p CO 2 , pH, temperature, salinity, and dissolved oxygen (DO) indicate that the sensors effectively captured key parameter measurements under challenging environmental conditions, allowing for an initial characterization of daily to seasonal trends in carbonate chemistry across a range of estuarine settings. Multi-year monitoring showed that across all water bodies temperature and p CO 2 covaried, suggesting that p CO 2 variability was governed, in part, by seasonal temperature changes with average p CO 2 being lower in cooler, winter months and higher in warmer, summer months. Furthermore, the timing of seasonal shifts towards increasing (or decreasing) p CO 2 varied by location and appears to be related to regional climate conditions. Specifically, p CO 2 increases began earlier in the year in warmer water, lower latitude water bodies in the GOM (Tampa Bay; Mission-Aransas Estuary) as compared with cooler water, higher latitude water bodies in the northeast (Barnegat Bay; Casco Bay), and upwelling-influenced West Coast water bodies (Tillamook Bay; Santa Monica Bay; San Francisco Bay). Results suggest that both thermal and non-thermal influences are important drivers of p CO 2 in Tampa Bay and Mission-Aransas Estuary. Conversely, non-thermal processes, most notably the biogeochemical structure of coastal upwelling, appear to be largely responsible for the observed p CO 2 values in West Coast water bodies. The co-occurrence of high salinity, high p CO 2 , low DO, and low temperature water in Santa Monica Bay and San Francisco Bay characterize the coastal upwelling paradigm that is also evident in Tillamook Bay when upwelling dominates freshwater runoff and local processes. These data demonstrate that high-quality carbonate chemistry observations can be recorded from estuarine environments using autonomous sensors originally designed for open-ocean settings.

California, Florida, Maine, New Jersey, Oregon, Te↗

USGS2019

Soil aggregates as a source of dissolved organic carbon to streams: An experimental study on the effect of solution chemistry on water extractable carbon

Over the past two decades, headwater streams of the northern hemisphere have shown increased amounts of dissolved organic carbon (DOC), coinciding with decreased acid deposition. The exact nature of the mechanistic link between precipitation composition and stream water DOC is still widely debated in the literature. We hypothesize that soil aggregates are the main source of stream water DOC and that DOC release is greater in organic rich, riparian soils vs. hillslope soils. To test these hypotheses, we collected soils from two main landscape positions (hillslope and riparian zones) from the acid-impacted Sleepers River Research Watershed in northeastern Vermont. We performed aqueous soil extracts with solutions of different ionic strength (IS) and composition to simulate changes in soil solution. We monitored dynamic changes in soil particle size, aggregate architecture and composition, leachate DOC concentrations, dissolved organic matter (DOM) characteristics by fluorescence spectroscopy and trends in bioavailability. In low IS solutions, extractable DOC concentrations were significantly higher, particle size (by laser diffraction) was significantly smaller and organic material was separated from mineral particles in scanning electron microscope observations. Furthermore, higher DOC concentrations were found in Na + compared to Ca 2+ solutions of the same IS. These effects are attributed to aggregate dispersion due to expanding diffuse double layers in decreased IS solutions and to decreased bridging by divalent cations. Landscape position impacted quality but not quantity of released DOC. Overall, these results indicate that soil aggregates might be one important link between Critical Zone inputs (i.e., precipitation) and exports in streams.

Vermont↗

USGS2023

Land development and road salt usage drive long-term changes in major-ion chemistry of streamwater in six exurban and suburban watersheds, southeastern Pennsylvania, 1999-2019

In urbanized areas, the “freshwater salinization syndrome” (FSS), which pertains to long-term increases in concentrations of major ions and metals in fresh surface waters, has been attributed to road salt application. In addition to FSS, the water composition changes as an influx of sodium (Na + ) in recharge may displace calcium (Ca 2+ ), magnesium (Mg 2+ ), potassium (K + ), and trace metals by reverse cation exchange. These changing ion fluxes can result in adverse impacts on groundwater and surface waters used for municipal supplies. Few datasets exist to quantify the FSS on a watershed scale or link its manifestation to potential controlling factors such as changes in urban development, land use/land cover (LULC), or wastewater treatment plant (WWTP) discharges in upstream areas. Here, we use two decades (1999–2019) of monthly streamwater quality data combined with daily streamflow for six exurban and suburban watersheds in southeastern Pennsylvania to examine the relations among Ca 2+ , Mg 2+ , K + , Na + , chloride (Cl − ), sulfate (SO 4 2- ), and alkalinity (HCO 3 − ) concentrations and upstream controlling factors. Flow-normalized annual and baseflow (August ̶ November) concentrations for Ca 2+ , Mg 2+ , Na + , and Cl − increased in all six watersheds over the 20-year study, providing evidence of FSS’s impacts on groundwater that sustains streamflow. Additionally, a redundancy analysis using 2019 flow-normalized values identified the following positive associations between solute concentrations and controlling variables: 1) Cl − , Mg 2+ , and Ca 2+ with impervious surface cover (ISC), 2) Na + and SO 4 2- with ISC and total WWTP discharge volume, and 3) HCO 3 − with agriculture and total WWTP discharge volume. From a human health perspective, 2019 flow-normalized Na + concentrations exceeded the U.S. Environmental Protection Agency’s 20 mg L -1 threshold for individuals restricted to a low sodium diet. Furthermore, indices used to evaluate the corrosivity of source waters to drinking water infrastructure and inform municipal water treatment practices, such as the Chloride to Sulfate Mass Ratio and Larson Ratio, increased between two- and seven-fold over the 20-year time. Collectively, the results elucidate the causal factors of the FSS in suburban and exurban watersheds and its potential impacts on human health and drinking water infrastructure.

Pennsylvania↗