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At least 37 records · Page 2Linked to original sources

Comparative effects of energy-related saline wastewaters and sodium chloride on hatching, survival, and fitness-associated traits of two amphibian species

Salinity (sodium chloride [NaCl]) is a prevalent and persistent contaminant that negatively affects freshwater ecosystems. Although most studies focus on effects of salinity from road salts (primarily NaCl), high-salinity wastewaters from energy extraction (wastewaters) could be more harmful because they contain NaCl and other toxic components. Many amphibians are sensitive to salinity, and their eggs are thought to be the most sensitive life-history stage. However, there are few investigations with salinity that include eggs and larvae sequentially in long-term exposures. We investigated the relative effects of wastewaters from a large energy reserve, the Williston Basin (USA), and NaCl on northern leopard ( Rana pipiens ) and boreal chorus ( Pseudacris maculata ) frogs. We exposed eggs and tracked responses through larval stages (for 24 days). Wastewaters and NaCl caused similar reductions in hatching and larval survival, growth, development, and activity, while also increasing deformities. Chorus frog eggs and larvae were more sensitive to salinity than leopard frogs, suggesting species-specific responses. Contrary to previous studies, eggs of both species were less sensitive to salinity than larvae. Our ecologically relevant exposures suggest that accumulating effects can reduce survival relative to starting experiments with unexposed larvae. Alternatively, egg casings of some species may provide some protection against salinity. Notably, effects of wastewaters on amphibians were predominantly due to NaCl rather than other components. Therefore, findings from studies with other sources of increased salinity (e.g., road salts) could guide management of wastewater-contaminated ecosystems, and vice versa, to mitigate effects of salinization.

Montana, Wyoming

Occurrence and geochemistry of lead-210 and polonium-210 radionuclides in public-drinking-water supplies from principal aquifers of the United States

On the basis of lifetime cancer risks, lead-210 ( 210 Pb) and polonium-210 ( 210 Po) ≥ 1.0 and 0.7 pCi/L (picocuries per liter), respectively, in drinking-water supplies may pose human-health concerns. 210 Pb and 210 Po were detected at concentrations greater than these thresholds at 3.7 and 1.5%, respectively, of filtered untreated groundwater samples from 1263 public-supply wells in 19 principal aquifers across the United States. Nationally, 72% of samples with radon-222 ( 222 Rn) concentrations > 4000 pCi/L had 210 Pb ≥ 1.0 pCi/L. 210 Pb is mobilized by alpha recoil associated with the decay of 222 Rn and short-lived progeny. 210 Pb concentrations ≥ 1.0 pCi/L occurred most frequently where acidic groundwaters inhibited 210 Pb readsorption (felsic-crystalline rocks) and where reducing alkaline conditions favored dissolution of iron–manganese- (Fe–Mn-) oxyhydroxides (which adsorb 210 Pb) and formation of lead–carbonate complexes (enhancing lead (Pb) mobility). 210 Po concentrations ≥ 0.7 pCi/L occurred almost exclusively in confined Coastal Plain aquifers where old (low percent-modern carbon-14) groundwaters were reducing, with high pH (>7.5) and high sodium/chloride (Na/Cl) ratios resulting from cation exchange. In high-pH environments, aqueous polonium (Po) is poorly sorbed, occurring as dihydrogen polonate (H 2 PoO 3 (aq)) or, under strongly reducing conditions, as a hydrogen-polonide anion (HPo – ). Fe–Mn- and sulfate-reduction and cation-exchange processes may mobilize polonium from mineral surfaces. Po 2+ occurrence in low-to-neutral-pH waters is attenuated by adsorption.

Environmental Science Technology

Polymeric nanofiber-carbon nanotube composite mats as fast-equilibrium passive samplers for polar organic pollutants

To improve the performance of polymeric electrospun nanofiber mats (ENMs) for equilibrium passive sampling applications in water, we integrated two types of multiwalled carbon nanotubes (CNTs; with and without surface carboxyl groups) into polyacrylonitrile (PAN) and polystyrene (PS) ENMs. For 11 polar and moderately hydrophobic compounds (−0.07 ≤ log K OW ≤ 3.13), 90% of equilibrium uptake was achieved in under 0.8 days ( t 90% values) in nonmixed ENM-CNT systems. Sorption capacity of ENM-CNTs was between 2- and 50-fold greater than pure polymer ENMs, with equilibrium partition coefficients ( K ENM-W values) ranging from 1.4 to 3.1 log units (L/kg) depending on polymer type (hydrophilic PAN or hydrophobic PS), CNT loading (i.e., values increased with weight percent (wt %) of CNTs), and CNT type (i.e., greater uptake with carboxylated CNTs composites). During field deployment at Muddy Creek in North Liberty, Iowa, optimal ENM-CNTs (PAN with 20 wt % carboxylated CNTs) yielded atrazine concentrations in surface water with a 40% difference relative to analysis of a same-day grab sample. We also observed a mean percent difference of 30 (±20)% when comparing ENM-CNT sampler results to grab sample data collected within 1 week of deployment. With their rapid, high capacity uptake and small material footprint, ENM-CNT equilibrium passive samplers represent a promising alternative to complement traditional integrative passive samplers while offering convenience over large volume grab sampling.

Environmental Science & Technology

Biological effects of hydrocarbon degradation intermediates: Is the total petroleum hydrocarbon analytical method adequate for risk assessment?

In crude oil contaminant plumes, the dissolved organic carbon (DOC) is mainly hydrocarbon degradation intermediates only partly quantified by the diesel range total petroleum hydrocarbon (TPHd) method. To understand potential biological effects of degradation intermediates, we tested three fractions of DOC: (1) solid-phase extract (HLB); (2) dichloromethane (DCM-total) extract used in TPHd; and (3) DCM extract with hydrocarbons isolated by silica gel cleanup (DCM-SGC). Bioactivity of extracts from five wells spanning a range of DOC was tested using an in vitro multiplex reporter system that evaluates modulation of the activity of 46 transcription factors; extracts were evaluated at concentrations equivalent to the well water samples. The aryl hydrocarbon receptor (AhR) and pregnane X receptor (PXR) transcription factors showed the greatest upregulation, with HLB exceeding DCM-total, and no upregulation in the hydrocarbon fraction (DCM-SGC). The HLB extracts were further studied with HepG2 chemically activated luciferase expression (CALUX) in vitro assays at nine concentrations ranging from 40 to 0.01 times the well water concentrations. Responses decreased with distance from the source but were still present at two wells without detectable hydrocarbons. Thus, our in vitro assay results indicate that risks associated with degradation intermediates of hydrocarbons in groundwater will be underestimated when protocols that remove these chemicals are employed.

Minnesota

Occurrence and spatiotemporal dynamics of pharmaceuticals in a temperate-region wastewater effluent-dominated stream: Variable inputs and differential attenuation yield evolving complex exposure mixtures

Effluent-dominated streams are becoming increasingly common in temperate regions and generate complex pharmaceutical mixture exposure conditions that may impact aquatic organisms via drug–drug interactions. Here, we quantified spatiotemporal pharmaceutical exposure concentrations and composition mixture dynamics during baseflow conditions at four sites in a temperate-region effluent-dominated stream (upstream, at, and progressively downstream from effluent discharge). Samples were analyzed monthly for 1 year for 109 pharmaceuticals/degradates using a comprehensive U.S. Geological Survey analytical method and biweekly for 2 years focused on 14 most common pharmaceuticals/degradates. We observed a strong chemical gradient with pharmaceuticals only sporadically detected upstream from the effluent. Seventy-four individual pharmaceuticals/degradates were detected, spanning 5 orders of magnitude from 0.28 to 13 500 ng/L, with 38 compounds detected in >50% of samples. “Biweekly” compounds represented 77 ± 8% of the overall pharmaceutical concentration. The antidiabetic drug metformin consistently had the highest concentration with limited in-stream attenuation. The antihistamine drug fexofenadine inputs were greater during warm- than cool-season conditions but also attenuated faster. Differential attenuation of individual pharmaceuticals (i.e., high = citalopram; low = metformin) contributed to complex mixture evolution along the stream reach. This research demonstrates that variable inputs over multiple years and differential in-stream attenuation of individual compounds generate evolving complex mixture exposure conditions for biota, with implications for interactive effects.

Environmental Science & Technology

Utica shale play oil and gas brines: Geochemistry and factors influencing wastewater management

The Utica and Marcellus Shale Plays in the Appalachian Basin are the fourth and first largest natural gas producing plays in the United States, respectively. Hydrocarbon production generates large volumes of brine (“produced water”) that must be disposed of, treated, or reused. Though Marcellus brines have been studied extensively, there are few studies from the Utica Shale Play. This study presents new brine chemical analyses from 16 Utica Shale Play wells in Ohio and Pennsylvania. Results from Na–Cl–Br systematics and stable and radiogenic isotopes suggest that the Utica Shale Play brines are likely residual pore water concentrated beyond halite saturation during the formation of the Ordovician Beekmantown evaporative sequence. The narrow range of chemistry for the Utica Shale Play produced waters (e.g., total dissolved solids = 214–283 g/L) over both time and space implies a consistent composition for disposal and reuse planning. The amount of salt produced annually from the Utica Shale Play is equivalent to 3.4% of the annual U.S. halite production. Utica Shale Play brines have radium activities 580 times the EPA maximum contaminant level and are supersaturated with respect to barite, indicating the potential for surface and aqueous radium hazards if not properly disposed of.

Kentucky, Maryland, New York, Ohio, Pennsylvania,

Uranium bioaccumulation dynamics in the mayfly Neocloeon triangulifer and application to site-specific prediction

Little is known about the underlying mechanisms governing the bioaccumulation of uranium (U) in aquatic insects. We experimentally parameterized conditional rate constants for aqueous U uptake, dietary U uptake, and U elimination for the aquatic baetid mayfly Neocloeon triangulifer . Results showed that this species accumulates U from both the surrounding water and diet, with waterborne uptake prevailing. Elevated dietary U concentrations decreased feeding rates, presumably by altering food palatability or impairing the mayfly’s digestive processes, or both. Nearly 90% of the accumulated U was eliminated within 24 h after the waterborne exposure ceased, reflecting the desorption of weakly bound U from the insect’s integument. To examine whether the experimentally derived rate constants for N. triangulifer could be generalized to baetid mayflies, mayfly U concentrations were predicted using the water chemistry and U measured in periphyton from springs in Grand Canyon (United States) and were compared to U concentrations in spring-dwelling mayflies. Predicted and observed mayfly U concentrations were in good agreement. Under the modeled site-specific conditions, waterborne U uptake accounted for 52–93% of the bioaccumulated U. U accumulation was limited in these wild populations due to a combination of factors including low concentrations of bioavailable dissolved U species, slow U uptake rates from food, and fast U elimination.

Environmental Science & Technology

Critical shifts in trace metal transport and remediation performance under future low river flows

Exceptionally low river flows are predicted to become more frequent and more severe across many global regions as a consequence of climate change. Investigations of trace metal transport dynamics across streamflows reveal stark changes in water chemistry, metal transformation processes, and remediation effectiveness under exceptionally low-flow conditions. High spatial resolution hydrological and water quality datasets indicate that metal-rich groundwater will exert a greater control on stream water chemistry and metal concentrations because of climate change. This is because the proportion of stream water sourced from mined areas and mineralized strata will increase under predicted future low-flow scenarios (from 25% under Q45 flow to 66% under Q99 flow in this study). However, mineral speciation modelling indicates that changes in stream pH and hydraulic conditions at low flow will decrease aqueous metal transport and increase sediment metal concentrations by enhancing metal sorption directly to streambed sediments. Solute transport modelling further demonstrates how increases in the importance of metal-rich diffuse groundwater sources at low flow could minimize the benefits of point source metal contamination treatment. Understanding metal transport dynamics under exceptionally low flows, as well as under high flows, is crucial to evaluate ecosystem service provision and remediation effectiveness in watersheds under future climate change scenarios.

Environmental Science & Technology

Demethylation of methylmercury in bird, fish, and earthworm

Toxicity of methylmercury (MeHg) to wildlife and humans results from its binding to cysteine residues of proteins, forming MeHg-cysteinate (MeHgCys) complexes that hinder biological functions. MeHgCys complexes can be detoxified in vivo, yet how this occurs is unknown. We report that MeHgCys complexes are transformed into selenocysteinate (Hg(Sec)4) complexes in multiple animals from two phyla (a waterbird, freshwater fish, and earthworms) sampled in different geographical areas and contaminated by different Hg sources. In addition, high energy-resolution X-ray absorption spectroscopy and chromatography-ICP mass spectrometry of the waterbird liver support the binding of Hg(Sec)4 to selenoprotein P and biomineralization of Hg(Sec)4 to chemically inert nanoparticulate mercury selenide (HgSe). The results provide a foundation for understanding mercury detoxification in higher organisms, and suggest that the identified MeHgCys to Hg(Sec)4 demethylation pathway is common in nature.

Environmental Science & Technology

Pesticides and pesticide degradates in groundwater used for public supply across the United States: Occurrence and human-health context

This is the first assessment of groundwater from public-supply wells across the United States to analyze for >100 pesticide degradates and to provide human-health context for degradates without benchmarks. Samples from 1204 wells in aquifers representing 70% of the volume pumped for drinking supply were analyzed for 109 pesticides (active ingredients) and 116 degradates. Among the 41% of wells where pesticide compounds were detected, nearly two-thirds contained compound mixtures and three-quarters contained degradates. Atrazine, hexazinone, prometon, tebuthiuron, four atrazine degradates, and one metolachlor degradate were each detected in >5% of wells. Detection frequencies were largest for aquifers with more shallow, unconfined wells producing modern-age groundwater. To screen for potential human-health concerns, benchmark quotients (BQs) were calculated by dividing concentrations by the human-health benchmark, when available. For degradates without benchmarks, estimated values (estimated benchmark quotients (BQE)) were first calculated by assuming equimolar toxicity to the most toxic parent; final analysis excluded degradates with likely overestimated toxicity. Six pesticide compounds and 1.6% of wells had concentrations approaching levels of potential concern (individual or summed BQ or BQE values >0.1), and none exceeded these levels (values >1). Therefore, although pesticide compounds occurred frequently, concentrations were low, even accounting for mixtures and degradates without benchmarks.

Continental United States

The role of hydrates, competing chemical constituents, and surface composition on CLNO2 formation

Atomic chlorine (Cl • ) affects air quality and atmospheric oxidizing capacity. Nitryl chloride (ClNO 2 ) – a common Cl • source–forms when chloride-containing aerosols react with dinitrogen pentoxide (N 2 O 5 ). A recent study showed that saline lakebed (playa) dust is an inland source of particulate chloride (Cl – ) that generates high ClNO 2 . However, the underlying physiochemical factors responsible for observed yields are poorly understood. To elucidate these controlling factors, we utilized single particle and bulk techniques to determine the chemical composition and mineralogy of playa sediment and dust samples from the southwest United States. Single particle analysis shows trace highly hygroscopic magnesium and calcium Cl-containing minerals are present and likely facilitate ClNO 2 formation at low humidity. Single particle and mineralogical analysis detected playa sediment organic matter that hinders N 2 O 5 uptake as well as 10 Å-clay minerals (e.g., Illite) that compete with water and chloride for N 2 O 5 . Finally, we show that the composition of the aerosol surface, rather than the bulk, is critical in ClNO 2 formation. These findings underscore the importance of mixing state, competing reactions, and surface chemistry on N 2 O 5 uptake and ClNO 2 yield for playa dusts and, likely, other aerosol systems. Therefore, consideration of particle surface composition is necessary to improve ClNO 2 and air quality modeling.

Environmental Science Technology

Spatial distribution of microplastics in surficial benthic sediment of Lake Michigan and Lake Erie

The spatial distribution, concentration, particle size, and polymer compositions of microplastics in Lake Michigan and Lake Erie sediment were investigated. Fibers/lines were the most abundant of the five particle types characterized. Microplastic particles were observed in all samples with mean concentrations for particles greater than 0.355 mm of 65.2 p kg –1 in Lake Michigan samples ( n = 20) and 431 p kg –1 in Lake Erie samples ( n = 12). Additional analysis of particles with size 0.1250–0.3549 mm in Lake Erie resulted in a mean concentration of 631 p kg –1 . The majority of polymers in Lake Michigan samples were poly(ethylene terephthalate) (PET), high-density polyethylene (HDPE), and semisynthetic cellulose (S.S. Cellulose), and in Lake Erie samples were S.S. Cellulose, polypropylene (PP), and poly(vinyl chloride) (PVC). Polymer density estimates indicated that 85 and 74% of observed microplastic particles have a density greater than 1.1 g cm –3 for Lake Michigan and Lake Erie, respectively. The current study provided a multidimensional dataset on the spatial distribution of microplastics in benthic sediment from Lake Michigan and Lake Erie and valuable information for assessment of the fate of microplastics in the Great Lakes.

Lake Ontario, Lake Erie

Machine-learning predictions of high arsenic and high manganese at drinking water depths of the glacial aquifer system, northern continental United States

Globally, over 200 million people are chronically exposed to arsenic (As) and/or manganese (Mn) from drinking water. We used machine-learning (ML) boosted regression tree (BRT) models to predict high As (>10 μg/L) and Mn (>300 μg/L) in groundwater from the glacial aquifer system (GLAC), which spans 25 states in the northern United States and provides drinking water to 30 million people. Our BRT models’ predictor variables (PVs) included recently developed three-dimensional estimates of a suite of groundwater age metrics, redox condition, and pH. We also demonstrated a successful approach to significantly improve ML prediction sensitivity for imbalanced data sets (small percentage of high values). We present predictions of the probability of high As and high Mn concentrations in groundwater, and uncertainty, at two nonuniform depth surfaces that represent moving median depths of GLAC domestic and public supply wells within the three-dimensional model domain. Predicted high likelihood of anoxic condition (high iron or low dissolved oxygen), predicted pH, relative well depth, several modeled groundwater age metrics, and hydrologic position were all PVs retained in both models; however, PV importance and influence differed between the models. High-As and high-Mn groundwater was predicted with high likelihood over large portions of the central part of the GLAC.

Environmental Science & Technology

Atmospheric processing of iron-bearing mineral dust aerosol and its effect on growth of a marine diatom, Cyclotella meneghiniana

Iron (Fe) is a growth-limiting micronutrient for phytoplankton in major areas of oceans and deposited wind-blown desert dust is a primary Fe source to these regions. Simulated atmospheric processing of four mineral dust proxies and two natural dust samples followed by subsequent growth studies of the marine planktic diatom Cyclotella meneghiniana in artificial sea-water (ASW) demonstrated higher growth response to ilmenite (FeTiO 3 ) and hematite (α-Fe 2 O 3 ) mixed with TiO 2 than hematite alone. The processed dust treatment enhanced diatom growth owing to dissolved Fe (DFe) content. The fresh dust-treated cultures demonstrated growth enhancements without adding such dissolved Fe. These significant growth enhancements and dissolved Fe measurements indicated that diatoms acquire Fe from solid particles. When diatoms were physically separated from mineral dust particles, the growth responses become smaller. The post-mineralogy analysis of mineral dust proxies added to ASW showed a diatom-induced increased formation of goethite, where the amount of goethite formed correlated with observed enhanced growth. The current work suggests that ocean primary productivity may not only depend on dissolved Fe but also on suspended solid Fe particles and their mineralogy. Further, the diatom C. meneghiniana benefits more from mineral dust particles in direct contact with cells than from physically impeded particles, suggesting the possibility for alternate Fe-acquisition mechanism/s.

Environmental Science & Technology

Isolating the AFFF signature in coastal watersheds using oxidizable PFAS precursors and unexplained organofluorine

Water supplies for millions of U.S. individuals exceed maximum contaminant levels for per- and polyfluoroalkyl substances (PFAS). Contemporary and legacy use of aqueous film forming foams (AFFF) is a major contamination source. However, diverse PFAS sources are present within watersheds, making it difficult to isolate their predominant origins. Here we examine PFAS source signatures among six adjacent coastal watersheds on Cape Cod, MA, U.S.A. using multivariate clustering techniques. A distinct signature of AFFF contamination enriched in precursors with six perfluorinated carbons (C6) was identified in watersheds with an AFFF source, while others were enriched in C4 precursors. Principal component analysis of PFAS composition in impacted watersheds showed a decline in precursor composition relative to AFFF stocks and a corresponding increase in terminal perfluoroalkyl sulfonates with < C6 but not those with ≥ C6. Prior work shows that in AFFF stocks, all extractable organofluorine (EOF) can be explained by targeted PFAS and precursors inferred using Bayesian inference on the total oxidizable precursor assay. Using the same techniques for the first time in impacted watersheds, we find that only 24%–63% of the EOF can be explained by targeted PFAS and oxidizable precursors. Our work thus indicates the presence of large non-AFFF organofluorine sources in these coastal watersheds.

Massachusetts

Untargeted lipidomics for determining cellular and sub-cellular responses in Zebrafish (Danio rerio) liver cells following exposure to complex mixtures in U.S. streams

Surface waters often contain a variety of chemical contaminants potentially capable of producing adverse outcomes in both humans and wildlife due to impacts from industrial, urban, and agricultural activity. Here, we report the results of a zebrafish liver (ZFL) cell-based lipidomics approach to assess the potential ecotoxicological effects of complex contaminant mixtures using water collected from eight impacted streams across the United States mainland and Puerto Rico. We initially characterized the ZFL lipidome using high resolution mass spectrometry, resulting in the annotation of 508 lipid species covering 27 classes. We then identified lipid changes induced by all streamwater samples (nonspecific stress indicators) as well as those unique to water samples taken from specific streams. Subcellular impacts were classified based on organelle-specific lipid changes, including increased lipid saturation (endoplasmic reticulum stress), elevated bis(monoacylglycero)phosphate (lysosomal overload), decreased ubiquinone (mitochondrial dysfunction), and elevated ether lipids (peroxisomal stress). Finally, we demonstrate how these results can uniquely inform environmental monitoring and risk assessments of surface waters.

Environmental Science & Technology

Discrete sample introduction module for quantitative and isotopic analysis of methane and other gases by cavity ring-down spectroscopy

Carbon dioxide (CO 2 ) and methane (CH 4 ) are natural and anthropogenic products that play a central role in the global carbon cycle and regulating Earth’s climate. Applications utilizing laser absorption spectroscopy, which continuously measure concentrations and stable isotope ratios of these greenhouse gases, are routinely employed to measure the source and magnitude of atmospheric inputs. We developed a discrete sample introduction module (DSIM) to enable measurements of methane and CO 2 concentrations and δ 13 C values from limited volume (5–100 mL) gas samples when interfaced with a commercially available cavity ring-down spectroscopy (CRDS) analyzer. The analysis has a dynamic range that spans six orders of magnitude from 100% analyte to the lower limit of instrument detection (2 ppm). We demonstrate system performance for methane by comparing concentrations and δ 13 C results from the DSIM-CRDS system and traditional methods for a variety of sample types, including low concentration (nanomolar CH 4 ) seawater and high concentration (>90% CH 4 ) natural gas. The expansive concentration range of the field-portable DSIM-CRDS system can measure enhances analytical performance for investigating methane and CO 2 dynamics and, potentially, other gases measured by laser absorption spectroscopy.

Environmental Science & Technology

Exposure and transport of alkaloids and phytoestrogens from soybeans to agricultural soils and streams in the Midwestern United States

Phytotoxins are naturally produced toxins with potencies similar/higher than many anthropogenic micropollutants. Nevertheless, little is known regarding their environmental fate and off-field transport to streams. To fill this research gap, a network of six basins in the Midwestern United States with substantial soybean production was selected for the study. Stream water ( n = 110), soybean plant tissues ( n = 8), and soil samples ( n = 16) were analyzed for 12 phytotoxins (5 alkaloids and 7 phytoestrogens) and 2 widely used herbicides (atrazine and metolachlor). Overall, at least 1 phytotoxin was detected in 82% of the samples, with as many as 11 phytotoxins detected in a single sample (median = 5), with a concentration range from below detection to 37 and 68 ng/L for alkaloids and phytoestrogens, respectively. In contrast, the herbicides were ubiquitously detected at substantially higher concentrations (atrazine: 99% and metolachlor: 83%; the concentrations range from below detection to 150 and 410 ng/L, respectively). There was an apparent seasonal pattern for phytotoxins, where occurrence prior to and during harvest season (September to November) and during the snow melt season (March) was higher than that in December–January. Runoff events increased phytotoxin and herbicide concentrations compared to those in base-flow conditions. Phytotoxin plant concentrations were orders of magnitude higher compared to those measured in soil and streams. These results demonstrate the potential exposure of aquatic and terrestrial organisms to soybean-derived phytotoxins.

Illinois, Indiana, Iowa, Minnesota, Missouri, Sout