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USGS1990

Relationships among macerals, minerals, miospores and paleoecology in a column of Redstone coal (Upper Pennsylvanian) from north-central West Virginia (U.S.A.)

Two distinct paleoenvironments are represented in vertical succession in a column of Redstone coal in north-central West Virginia as indicated by a study of 37 consecutive 3-cm (0.1 ft) increments analyzed for ash yield, petrographic composition, low-temperature ash mineralogy and palynomorph abundances. Abundance profiles were constructed for ash, 12 petrographic components, 3 minerals and 5 miospore assemblages. The profiles and calculated correlation coefficients show close relationships between several constituents. Components that increased in abundance upward in the coal bed were a collinite type > 50 microns in thickness, cutinite, and miospores affiliated with calamites, herbaceous lycopods, cordaites and herbaceous ferns. Components that decreased in abundance upward were a collinite type < 50 microns in thickness, inertodetrinite, tree fern miospores, quartz, illite and ash yield. Components were correlated with ash yield to infer the swamp geochemical conditions that contributed to the low-ash (7%) upper one-third of the coal bed and the higher-ash (16%) lower two-thirds of the coal bed. Components that correlate positively with increased ash were the collinite type < 50 μ m thickness, inertodetrinite, tree fern miospores, illite and quartz. Components that correlate negatively with increased ash were the collinite type > 50 μ m in thickness, cutinite, calamite and cordaite miospores and kaolinite. Significant correlations occurred between ash yield and the collinite types > 50 and < 50 μ m in thickness but no significant correlation was found between ash yield and total vitrinite-group content. This is interpreted to show that division of vitrinite macerals by size is important in petrographic paleoenvironmental studies. Paleoecologic interpretations based upon these correlations suggest that two distinct, planar, probably topogenous paleoecologic environments are represented in this column of the Redstone coal. The lower two-thirds of the coal bed was interpreted to have accumulated in a planar swamp in which significant introduction of detrital or dissolved mineral matter, and significant anaerobic and moderate oxidative degradation of the peat occurred. The flora of this paleoenvironment was dominated by tree ferns. The paleoenvironment during accumulation of the upper one-third of the coal bed was also interpreted to have been a planar swamp, but one in which moderate to low introduction of detrital or dissolved mineral matter, and minor anaerobic and oxidative degradation of the peat occurred. The dominant flora of this paleoenvironment consisted mainly of calamites with fewer cordaites and herbaceous ferns. This study shows that valuable paleoecologic information may be obtained by sampling closely spaced vertical increments. No mixing of detrital sediments with the peat was observed in coal layers immediately adjacent to the parting or the overlying sandstone unit.

International Journal of Coal Geology↗

USGS1991

Release of 226Ra from uranium mill tailings by microbial Fe(III) reduction

Uranium mill tailings were anaerobically incubated in the presence of H 2 with Alteromonas putrefaciens , a bacterium known to couple the oxidation of H 2 and organic compounds to the reduction of Fe(III) oxides. There was a direct correlation between the extent of Fe(III) reduction and the accumulation of dissolved 226 Ra. In sterile tailings in which Fe(III) was not reduced, there was negligible leaching of 226 Ra. The behavior of Ba was similar to that of Ra in inoculated and sterile systems. These results demonstrate that under anaerobic conditions, microbial reduction of Fe(III) may result in the release of dissolved 226 Ra from uranium mill tailings.

Applied Geochemistry↗

USGS2011

Biogeochemical factors affecting the presence of 210 Po in groundwater

The discovery of natural 210 Po enrichment at levels exceeding 500 mBq/L in numerous domestic wells in northern Nevada, USA, led to a geochemical investigation of the processes responsible for its mobilization. 210 Po activities in 63 domestic and public-supply wells ranged from below 1 mBq/L to 6590 ± 590 mBq/L, among the highest reported levels in the USA. There is little spatial or depth variability in 210Pb activity in study-area sediments and mobilization of a few percent of the 210 Po in the sediments would account for all of the 210 Po in water. Stable-isotope measurements indicate SO 4 reduction has occurred in all 210 Po contaminated wells. Sulfide species are not accumulating in the groundwater in much of Lahontan Valley, probably because of S cycling involving microbial SO 4 reduction, abiotic oxidation of H 2 S to S 0 by Mn(IV), followed by microbial disproportionation of S 0 to H 2 S and SO 4 . The high pH, Ca depletion, MnCO3 saturation, and presence of S 0 in Lahontan Valley groundwater may be consequences of the anaerobic S cycling. Consistent with data from naturally-enriched wells in Florida, 210 Po activities begin to decrease when aqueous sulfide species begin to accumulate. This may be due to formation and precipitation of PoS, however, Eh–pH diagrams suggest PoS would not be stable in study-area groundwater. An alternative explanation for the study area is that H 2 S accumulation begins when anaerobic S cycling stops because Mn oxides are depleted and their reduction is no longer releasing 210 Po. Common features of 210 Po-enriched groundwater were identified by comparing the radiological and geochemical data from Nevada with data from naturally-enriched wells in Finland, and Florida and Maryland in the USA. Values of pH ranged from <5 in Florida wells to >9 in Nevada wells, indicating that pH is not critical in determining whether 210 Po is present. Where U is present in the sediments, the data suggest 210 Po levels may be elevated in aquifers with (1) SO 4 -reducing waters with low H 2 S concentrations, or (2) anoxic or oxic waters with extremely high Rn activities, particularly if the water is turbid.

Applied Geochemistry↗

USGS2007

High arsenic concentrations and enriched sulfur and oxygen isotopes in a fractured-bedrock ground-water system

Ground water with high arsenic concentrations (up to 26.6????mol L- 1) has sulfate enriched in 34S and 18O in the fractured-bedrock, ground-water system of the Kelly's Cove watershed, Northport, Maine, USA. The ranges of sulfur and oxygen isotope values in aqueous sulfate, ??34S[SO4] and ??18O[SO4], at the Kelly's Cove watershed are + 3.4 to + 4.9??? and - 2.0 to + 6.7???, respectively. These isotope values are strikingly similar to those of the Goose River, Maine watershed which has ??34S[SO4] and ??18O[SO4] ranges of + 3.7 to + 4.6 ??? and - 2.6 to + 7.5???, respectively. In both systems, high arsenic concentrations occur with high ??34S[SO4] and ??18O[SO4] values, yet redox conditions and underlying rock types are quite different. The isotope values of sulfide minerals, ??34S[min], from four bedrock cores vary over short distances and range from - 5.1 to + 7.5???. The ??34S[SO4] values are controlled by the ??34S[min] values with minor input of atmospheric SO4. The much narrower range in ??34S[SO4] values than ??34S[min] values is probably due to sufficient ground-water mixing at a scale greater than the ??34S[min] variability. The ??34S[SO4] values are about 2??? higher than the average ??34S[min] value and fall within the range of ??34S[min] values, indicating only minor fractionation due to bacterial reduction of SO4. The highest ??18O[SO4] values were measured in the downgradient, confined, arsenic-rich ground water. High ??18O[SO4] values there cannot be due to aeration by atmospheric oxygen, but may arise from reoxidation of reduced SO4 products. The enrichment factors of ??18O in SO4 compared to H2O, + 7.2 to + 15.5???, in the Kelly's Cove ground water and the negligible 34S enrichment is very similar to those derived from experimental data of anaerobic sulfide oxidation in the presence of Mn and Fe oxides. Sea level at the Kelly's Cove watershed was approximately 80??m above present sea level about 13 000??years before present, imposing reducing conditions on that area of the watershed. Sea level dropped approximately 60??m below present sea level about 11 000??years before present, allowing for possible oxidation of sulfide minerals and precipitation of arsenic in ferric oxyhydroxides during aeration of the ground-water system. Under present redox conditions, there is evidence that bacteria reduction of ferric oxyhydroxides releases arsenic. The fractionation of 18O in the SO4 during anaerobic oxidation of sulfide in the presence of Mn and Fe oxides and subsequent release of arsenic during Mn and Fe oxide reduction may explain the relationship between high arsenic concentrations and elevated 18O[SO4] at Kelly's Cove. ?? 2007 Elsevier B.V. All rights reserved.

Chemical Geology↗

USGS2011

Mineral transformations associated with goethite reduction by Methanosarcina barkeri

To investigate the interaction between methanogens and iron-containing minerals in anoxic environments, we conducted batch culture experiments with Methanosarcina barkeri in a phosphate-buffered basal medium (PBBM) to bioreduce structural Fe(III) in goethite with hydrogen as the sole substrate. Fe(II) and methane concentrations were monitored over the course of the bioreduction experiments with wet chemistry and gas chromatography, respectively. Subsequent mineralogical changes were characterized with X-ray diffraction (XRD) and scanning electron microscopy (SEM). In the presence of an electron shuttle anthraquinone-2,6-disulfonate (AQDS), 30% Fe(III) in goethite (weight basis) was reduced to Fe(II). In contrast, only 2% Fe(III) (weight basis) was bioreduced in the absence of AQDS. Most of the bioproduced Fe(II) was incorporated into secondary minerals including dufrénite and vivianite. Our data implied a dufrénite–vivianite transformation mechanism where a metastable dufrénite transformed to a more stable vivianite over extended time in anaerobic conditions. Methanogenesis was greatly inhibited by bioreduction of goethite Fe(III). These results have important implications for the methane flux associated with Fe(III) bioreduction and ferrous iron mineral precipitation in anaerobic soils and sediments.

Chemical Geology↗

USGS2011

Microtopography enhances nitrogen cycling and removal in created mitigation wetlands

Natural wetlands often have a heterogeneous soil surface topography, or microtopography (MT), that creates microsites of variable hydrology, vegetation, and soil biogeochemistry. Created mitigation wetlands are designed to mimic natural wetlands in structure and function, and recent mitigation projects have incorporated MT as one way to attain this goal. Microtopography may influence nitrogen (N) cycling in wetlands by providing adjacent areas of aerobic and anaerobic conditions and by increasing carbon storage, which together facilitate N cycling and removal. This study investigated three created wetlands in the Virginia Piedmont that incorporated disking-induced MT during construction. One site had paired disked and undisked plots, allowing an evaluation of the effects of this design feature on N flux rates. Microtopography was measured using conventional survey equipment along a 1-m circular transect and was described using two indices: tortuosity (T), describing soil surface roughness and relief, and limiting elevation difference (LD), describing soil surface relief. Ammonification, nitrification, and net N mineralization were determined with in situ incubation of modified ion-exchange resin cores and denitrification potential was determined using denitrification enzyme assay (DEA). Results demonstrated that disked plots had significantly greater LD than undisked plots one year after construction. Autogenic sources of MT (e.g. tussock-forming vegetation) in concert with variable hydrology and sedimentation maintained and in some cases enhanced MT in study wetlands. Tortuosity and LD values remained the same in one wetland when compared over a two-year period, suggesting a dynamic equilibrium of MT-forming and -eroding processes at play. Microtopography values also increased when comparing the original induced MT of a one-year old wetland with MT of older created wetlands (five and eight years old) with disking-induced MT, indicating that MT can increase by natural processes over time. When examined along a hydrologic gradient, LD increased with proximity to an overflow point as a result of differential sediment deposition and erosion during flood events. Nitrification increased with T and denitrification potential increased with LD, indicating that microtopographic heterogeneity enhances coupled N fluxes. The resulting N flux patterns may be explained by the increase in oxygen availability elicited by greater T (enhancing nitrification) and by the adjacent zones of aerobic and anaerobic conditions elicited by greater LD (enhancing coupled nitrification and denitrification potential). Findings of this study support the incorporation of MT into the design and regulatory evaluation of created wetlands in order to enhance N cycling and removal. ?? 2011.

Ecological Engineering↗

USGS2004

Degradation of 1,1,2,2-tetrachloroethane and accumulation of vinyl chloride in wetland sediment microcosms and in situ porewater: Biogeochemical controls and associations with microbial communities

The biodegradation pathways of 1,1,2,2-tetrachloroethane (TeCA) and 1,1,2-trichloroethane (112TCA) and the associated microbial communities in anaerobic wetland sediments were evaluated using concurrent geochemical and genetic analyses over time in laboratory microcosm experiments. Experimental results were compared to in situ porewater data in the wetland to better understand the factors controlling daughter product distributions in a chlorinated solvent plume discharging to a freshwater tidal wetland at Aberdeen Proving Ground, Maryland. Microcosms constructed with wetland sediment from two sites showed little difference in the initial degradation steps of TeCA, which included simultaneous hydrogenolysis to 112TCA and dichloroelimination to 1,2-dichloroethene (12DCE). The microcosms from the two sites showed a substantial difference, however, in the relative dominance of subsequent dichloroelimination of 112TCA. A greater dominance of 112TCA dichloroelimination in microcosms constructed with sediment that was initially iron-reducing and subsequently simultaneously iron-reducing and methanogenic caused approximately twice as much vinyl chloride (VC) production as microcosms constructed with sediment that was methanogenic only throughout the incubation. The microcosms with higher VC production also showed substantially more rapid VC degradation. Field measurements of redox-sensitive constituents, TeCA, and its anaerobic degradation products along flowpaths in the wetland porewater also showed greater production and degradation of VC with concurrent methanogenesis and iron reduction. Molecular fingerprinting indicated that bacterial species [represented by a peak at a fragment size of 198 base pairs (bp) by MnlI digest] are associated with VC production from 112TCA dichloroelimination, whereas methanogens (190 and 307 bp) from the Methanococcales or Methanobacteriales family are associated with VC production from 12DCE hydrogenolysis. Acetate-utilizing methanogens (acetotrophs) appear to be involved in the biodegradation of VC. The relative abundance of Methanosarcinaceae, the only methanogen group with acetotrophic members, doubled in microcosms in which degradation of VC was observed. In addition, molecular analyses using primers specific for known dehalorespiring bacteria in the Dehalococcoides and Desulfuromonas groups showed the presence of these bacteria in microcosm slurry from the site that showed the highest VC production and degradation. Determination of biogeochemical controls and microbial consortia involved in TeCA degradation is leading to a better understanding of the heterogeneity in biodegradation rates and daughter product distribution in the wetland, improving capabilities for developing remediation and monitoring plans.

Journal of Contaminant Hydrology↗

USGS2011

Role of back diffusion and biodegradation reactions in sustaining an MTBE/TBA plume in alluvial media

A methyl tert-butyl ether (MTBE) / tert-butyl alcohol (TBA) plume originating from a gasoline spill in late 1994 at Vandenberg Air Force Base (VAFB) persisted for over 15 years within 200 feet of the original spill source. The plume persisted until 2010 despite excavation of the tanks and piping within months after the spill and excavations of additional contaminated sediments from the source area in 2007 and 2008. The probable history of MTBE concentrations along the plume centerline at its source was estimated using a wide variety of available information, including published details about the original spill, excavations and monitoring by VAFB consultants, and our own research data. Two-dimensional reactive transport simulations of MTBE along the plume centerline were conducted for a 20-year period following the spill. These analyses suggest that MTBE diffused from the thin anaerobic aquifer into the adjacent anaerobic silts and transformed to TBA in both aquifer and silt layers. The model reproduces the observation that after 2004 TBA was the dominant solute, diffusing back out of the silts into the aquifer and sustaining plume concentrations much longer than would have been the case in the absence of such diffusive exchange. Simulations also suggest that aerobic degradation of MTBE or TBA at the water table in the overlying silt layer significantly affected concentrations of MTBE and TBA by limiting the chemical mass available for back diffusion to the aquifer.

California↗

USGS2007

Evidence of CFC degradation in groundwater under pyrite-oxidizing conditions

A detailed local-scale monitoring network was used to assess CFC distribution in an unconfined sand aquifer in southwestern Ontario where the zone of 1–5-year-old groundwater was known with certainty because of prior use of a bromide tracer. Groundwater ⩽5 years old was confined to an aerobic zone at ⩽5 m depth and had CFC concentrations consistent with modern atmospheric mixing ratios at recharge temperatures of 7–11 °C, as was observed in the 3-m thick vadose zone at the site. At depths below 6 m, the groundwater became progressively more reducing, however, with a denitrifying horizon at 6–7 m depth, and a Mn and Fe reducing zone below 7 m depth. In the anaerobic zone, 3 H/ 3 He ratios indicated that groundwater-age continued to increase uniformly with depth, to a maximum value of 27 years at 13 m depth. CFC concentrations, however, decreased abruptly within the denitrifying zone, leading to substantial age overestimation compared to the 3 H/ 3 He ages. Noble gas data indicated that the apparent CFC mass loss was not likely the result of gas stripping from possible bubble formation; thus, CFC degradation was indicated in the anoxic zone. The field data are consistent with first-order degradation rates of 0.3 yr −1 for CFC-12, 0.7 yr −1 for CFC-11, and 1.6 yr −1 for CFC-113. CFC attenuation at this site coincides with a zone where reduced S (pyrite) is actively oxidized by NO 3 and dissolved oxygen (DO). Similar behavior has been observed at other sites [Tesoriero, A.J., Liebscher, H., Cox, S.E., 2000. Mechanism and rate of denitrification in an agricultural watershed: electron and mass balance along groundwater flow path. Water Resour. Res. 36 (6), 1545–1559; Hinsby, K., Hojberg, A.L., Engesgaard, P., Jensen, K.H., Larsen, F., Plummer, L.N., Busenberg, E., Accepted for publication. Transport and degradation of chlorofluorocarbons (CFCs) in a pyritic aquifer, Rabis Creek, Denmark. Water Resour. Res.], further demonstrating that the use of CFCs for age-dating anaerobic groundwater should be approached with caution, particularly if the sediment contains pyrite.

Journal of Hydrology↗

USGS2017

Virulence and biodegradation potential of dynamic microbial communities associated with decaying Cladophora in Great Lakes

Cladophora mats that accumulate and decompose along shorelines of the Great Lakes create potential threats to the health of humans and wildlife. The decaying algae create a low oxygen and redox potential environment favoring growth and persistence of anaerobic microbial populations, including Clostridium botulinum , the causal agent of botulism in humans, birds, and other wildlife. In addition to the diverse population of microbes, a dynamic chemical environment is generated, which involves production of numerous organic and inorganic substances, many of which are believed to be toxic to the sand and aquatic biotic communities. In this study, we used 16S-rDNA-based-amplicon sequencing and microfluidic-based quantitative PCR approaches to characterize the bacterial community structure and the abundances of human pathogens associated with Cladophora at different stages (up to 90 days) of algal decay in laboratory microcosms. Oxygen levels were largely depleted after a few hours of incubation. As Cladophora decayed, the algal microbial biodiversity decreased within 24 h, and the mat transitioned from an aerobic to anaerobic environment. There were increasing abundances of enteric and pathogenic bacteria during decomposition of Cladophora , including Acinetobacter , Enterobacter , Kluyvera , Cedecea , and others. In contrast, there were no or very few sequences (< 0.07%) assigned to such groups in fresh Cladophora samples. Principal coordinate analysis indicated that the bacterial community structure was dynamic and changed significantly with decay time. Knowledge of microbial communities and chemical composition of decaying algal mats is critical to our further understanding of the role that Cladophora plays in a beach ecosystem's structure and function, including the algal role in trophic interactions. Based on these findings, public and environmental health concerns should be considered when decaying Cladophora mats accumulate Great Lakes shorelines.

Great Lakes↗

USGS2000

Bacterial dissimilatory reduction of arsenate and sulfate in meromictic Mono Lake, California

The stratified (meromictic) water column of alkaline and hypersaline Mono Lake, California, contains high concentrations of dissolved inorganic arsenic (~200 ??mol/L). Arsenic speciation changes from arsenate [As (V)] to arsenite [As (III)] with the transition from oxic surface waters (misolimnion) to anoxic bottom waters (monimolimnion). A radioassay was devised to measure the reduction of 73As (V) to 73As (III) and tested using cell suspensions of the As (V)-respiring Bacillus selenitireducens, which completely reduced the 73As (V). In field experiments, no significant activity was noted in the aerobic mixolimnion waters, but reduction of 73As (V) to 73As (III) was observed in all the monimolimnion samples. Rate constants ranged from 0.02 to 0.3/day, with the highest values in the samples from the deepest depths (24 and 28 m). The highest activities occurred between 18 and 21 m, where As (V) abundant (rate, ~5.9 ??mol/L per day). In contrast, sulfate reduction occurred at depths below 21 m, with the highest rates attained at 28 m (rate, ~2.3 ??mol/L per day). These results indicate that As (V) ranks second in importance, after sulfate, as an electron acceptor for anaerobic bacterial respiration in the water column. Annual arsenate respiration may mineralize as much as 14.2% of the pelagic photosynthetic carbon fixed during meromixis. When combined with sulfate-reduction data, anaerobic respiration in the water column can mineralize 32-55% of this primary production. As lakes of this type approach salt saturation, As (V) can become the most important electron acceptor for the biogeochemical cycling of carbon.

California↗

USGS2000

Geochemical modeling of iron, sulfur, oxygen and carbon in a coastal plain aquifer

Fe(III) reduction in the Magothy aquifer of Long Island, NY, results in high dissolved-iron concentrations that degrade water quality. Geochemical modeling was used to constrain iron-related geochemical processes and redox zonation along a flow path. The observed increase in dissolved inorganic carbon is consistent with the oxidation of sedimentary organic matter coupled to the reduction of O2 and SO4/2- in the aerobic zone, and to the reduction of SO4/2- in the anaerobic zone; estimated rates of CO2 production through reduction of Fe(III) were relatively minor by comparison. The rates of CO2 production calculated from dissolved inorganic carbon mass transfer (2.55 x 10-4 to 48.6 x 10-4 mmol 1-1 yr-1) generally were comparable to the calculated rates of CO2 production by the combined reduction of O2, Fe(III) and SO4/2- (1.31 x 10-4 to 15 x 10-4 mmol 1-1 yr-1). The overall increase in SO4/2- concentrations along the flow path, together with the results of mass-balance calculations, and variations in ??34S values along the flow path indicate that SO4/2- loss through microbial reduction is exceeded by SO4/2- gain through diffusion from sediments and through the oxidation of FeS2. Geochemichal and microbial data on cores indicate that Fe(III) oxyhydroxide coatings on sediment grains in local, organic carbon- and SO4/2- -rich zones have localized SO4/2- -reducing zones in which the formation of iron disulfides been depleted by microbial reduction and resulted in decreases dissolved iron concentrations. These localized zones of SO4/2- reduction, which are important for assessing zones of low dissolved iron for water-supply development, could be overlooked by aquifer studies that rely only on groundwater data from well-water samples for geochemical modeling. (C) 2000 Elsevier Science B.V.Fe(III) reduction in the Magothy aquifer of Long Island, NY, results in high dissolved-iron concentrations that degrade water quality. Geochemical modeling was used to constrain iron-related geochemical processes and redox zonation along a flow path. The observed increase in dissolved inorganic carbon is consistent with the oxidation of sedimentary organic matter coupled to the reduction of O2 and SO42- in the aerobic zone, and to the reduction of SO42- in the anaerobic zone; estimated rates of CO2 production through reduction of Fe(III) were relatively minor by comparison. The rates of CO2 production calculated from dissolved inorganic carbon mass transfer (2.55??10-4 to 48.6??10-4mmol l-1yr-1) generally were comparable to the calculated rates of CO2 production by the combined reduction of O2, Fe(III) and SO42- (1.31??10-4 to 15??10-4mmol l-1yr-1). The overall increase in SO42- concentrations along the flow path, together with the results of mass-balance calculations, and variations in ??34S values along the flow path indicate that SO42- loss through microbial reduction is exceeded by SO42- gain through diffusion from sediments and through the oxidation of FeS2. Geochemical and microbial data on cores indicate that Fe(III) oxyhydroxide coatings on sediment grains in local, organic carbon- and SO42--rich zones have been depleted by microbial reduction and resulted in localized SO42--reducing zones in which the formation of iron disulfides decreases dissolved iron concentrations. These localized zones of SO42- reduction, which are important for assessing zones of low dissolved iron for water-supply development, could be overlooked by aquifer studies that rely only on groundwater data from well-water samples for geochemical modeling.

Journal of Hydrology↗

USGS2000

Mobilization of arsenite by dissimilatory reduction of adsorbed arsenate

Sulfurospirillum barnesii is capable of anaerobic growth using ferric iron or arsenate as electron acceptors. Cell suspensions of S. barnesii were able to reduce arsenate to arsenite when the former oxyanion was dissolved in solution, or when it was adsorbed onto the surface of ferrihydrite, a common soil mineral, by a variety of mechanisms (e.g., coprecipitation, presorption). Reduction of Fe(III) in ferrihydrite to soluble Fe(II) also occurred, but dissolution of ferrihydrite was not required in order for adsorbed arsenate reduction to be achieved. This was illustrated by bacterial reduction of arsenate coprecipitated with aluminum hydroxide, a mineral that does not undergo reductive dissolution. The rate of arsenate reduction was influenced by the method in which arsenate became associated with the mineral phases and may have been strongly coupled with arsenate desorption rates. The extent of release of arsenite into solution was governed by adsorption of arsenite onto the ferrihydrite or alumina phases. The results of these experiments have interpretive significance to the mobilization of arsenic in large alluvial aquifers, such as those of the Ganges in India and Bangladesh, and in the hyporheic zones of contaminated streams.Sulfurospirillum barnesii is capable of anaerobic growth using ferric iron or arsenate as electron acceptors. Cell suspensions of S. barnesii were able to reduce arsenate to arsenite when the former oxyanion was dissolved in solution, or when it was adsorbed onto the surface of ferrihydrite a common soil mineral, by a variety of mechanisms (e.g., coprecipitation, presorption). Reduction of Fe(III) in ferrihydrite to soluble Fe(II) also occurred, but dissolution of ferrihydrite was not required in order for adsorbed arsenate reduction to be achieved. This was illustrated by bacterial reduction of arsenate coprecipitated with aluminum hydroxide, a mineral that does not undergo reductive dissolution. The rate of arsenate reduction was influenced by the method in which arsenate became associated with the mineral phases and may have been strongly coupled with arsenate desorption rates. The extent of release of arsenite into solution was governed by adsorption of arsenite onto the ferrihydrite or alumina phases. The results of these experiments have interpretive significance to the mobilization of arsenic in large alluvial aquifers, such as those of the Ganges in India and Bangladesh, and in the hyporheic zones of contaminated streams.

Environmental Science & Technology↗

USGS2000

Methyl-mercury degradation pathways: A comparison among three mercury impacted ecosystems

We examined microbial methylmercury (MeHg) degradation in sediment of the Florida Everglades, Carson River (NV), and San Carlos Creek (CA), three freshwater environments that differ in the extent and type of mercury contamination and sediment biogeochemistry. Degradation rate constant ( k deg ) values increased with total mercury (Hg t ) contamination both among and within ecosystems. The highest k deg 's (2.8−5.8 d - 1 ) were observed in San Carlos Creek, at acid mine drainage impacted sites immediately downstream of the former New Idria mercury mine, where Hg t ranged from 4.5 to 21.3 ppm (dry wt). A reductive degradation pathway (presumably mer -detoxification) dominated degradation at these sites, as indicated by the nearly exclusive production of 14 CH 4 from 14 C-MeHg, under both aerobic and anaerobic conditions. At the upstream control site, and in the less contaminated ecosystems (e.g. the Everglades), k deg 's were low (≤0.2 d - 1 ) and oxidative demethylation (OD) dominated degradation, as evident from 14 CO 2 production. k deg increased with microbial CH 4 production, organic content, and reduced sulfur in the Carson River system and increased with decreasing pH in San Carlos Creek. OD associated CO 2 production increased with pore-water SO 4 2- in Everglades samples but was not attributable to anaerobic methane oxidation, as has been previously proposed. This ecosystem comparison indicates that severely contaminated sediments tend to have microbial populations that actively degrade MeHg via mer -detoxification, whereas OD occurs in heavily contaminated sediments as well but dominates in those less contaminated.

Environmental Science & Technology↗

USGS2004

Chemical characterization and sorption capacity measurements of degraded newsprint from a landfill

Newsprint samples collected from 12−16 ft (top layer (TNP)), 20−24 ft (middle layer (MNP)), and 32−36 ft (bottom layer (BNP)) below the surface of the Norman Landfill (NLF) were characterized by infrared (IR) spectroscopy, cross-polarization, magic-angle spinning 13 C nuclear magnetic resonance (CP-MAS 13 C NMR) spectroscopy, and tetramethylammonium hydroxide (TMAH) thermochemolysis gas chromatography/mass spectrometry (GC/MS). The extent of NLF newsprint degradation was evaluated by comparing the chemical composition of NLF newsprint to that of fresh newsprint (FNP) and newsprint degraded in the laboratory under methanogenic conditions (DNP). The O -alkyl/alkyl, cellulose/lignin, and lignin/resin acid ratios showed that BNP was the most degraded, and that all three NLF newsprint samples were more degraded than DNP. 13 C NMR and TMAH thermochemolysis data demonstrated selective enrichment of lignin over cellulose, and TMAH thermochemolysis further exhibited selective enrichment of resin acids over lignin. In addition, the crystallinity of cellulose in NLF newsprint samples was significantly lower relative to that of FNP and DNP as shown by 13 C NMR spectra. The yield of lignin monomers from TMAH thermochemolysis suggested that hydroxyl groups were removed from the propyl side chain of lignin during the anaerobic decomposition of newsprint in the NLF. Moreover, the vanillyl acid/aldehyde ratio, which successfully describes aerobic lignin degradation, was not a good indicator of the anaerobic degradation of lignin on the basis of the TMAH data. The toluene sorption capacity increased as the degree of newsprint degradation increased or as the O -alkyl/alkyl ratio of newsprint decreased. The results of this study further verified that the sorbent O -alkyl/alkyl ratio is useful for predicting sorption capacities of natural organic materials for hydrophobic organic contaminants.

Environmental Science & Technology↗

USGS2014

Transformation products and human metabolites of triclocarban and tricllosan in sewage sludge across the United States

Removal of triclocarban (TCC) and triclosan (TCS) from wastewater is a function of adsorption, abiotic degradation, and microbial mineralization or transformation, reactions that are not currently controlled or optimized in the pollution control infrastructure of standard wastewater treatment. Here, we report on the levels of eight transformation products, human metabolites, and manufacturing byproducts of TCC and TCS in raw and treated sewage sludge. Two sample sets were studied: samples collected once from 14 wastewater treatment plants (WWTPs) representing nine states, and multiple samples collected from one WWTP monitored for 12 months. Time-course analysis of significant mass fluxes (α = 0.01) indicate that transformation of TCC (dechlorination) and TCS (methylation) occurred during sewage conveyance and treatment. Strong linear correlations were found between TCC and the human metabolite 2′-hydroxy-TCC ( r = 0.84), and between the TCC-dechlorination products dichlorocarbanilide (DCC) and monochlorocarbanilide ( r = 0.99). Mass ratios of DCC-to-TCC and of methyl-triclosan (MeTCS)-to-TCS, serving as indicators of transformation activity, revealed that transformation was widespread under different treatment regimes across the WWTPs sampled, though the degree of transformation varied significantly among study sites (α = 0.01). The analysis of sludge sampled before and after different unit operation steps (i.e., anaerobic digestion, sludge heat treatment, and sludge drying) yielded insights into the extent and location of TCC and TCS transformation. Results showed anaerobic digestion to be important for MeTCS transformation (37–74%), whereas its contribution to partial TCC dechlorination was limited (0.4–2.1%). This longitudinal and nationwide survey is the first to report the occurrence of transformation products, human metabolites, and manufacturing byproducts of TCC and TCS in sewage sludge.

Environmental Science & Technology↗

USGS2009

Arsenite and ferrous iron oxidation linked to chemolithotrophic denitrification for the immobilization of arsenic in anoxic environments

The objective of this study was to explore a bioremediation strategy based on injecting NO 3 − to support the anoxic oxidation of ferrous iron (Fe(II)) and arsenite (As(III)) in the subsurface as a means to immobilize As in the form of arsenate (As(V)) adsorbed onto biogenic ferric (Fe(III)) (hydr)oxides. Continuous flow sand filled columns were used to simulate a natural anaerobic groundwater and sediment system with co-occurring As(III) and Fe(II) in the presence (column SF1) or absence (column SF2) of nitrate, respectively. During operation for 250 days, the average influent arsenic concentration of 567 μg L −1 was reduced to 10.6 (±9.6) μg L −1 in the effluent of column SF1. The cumulative removal of Fe(II) and As(III) in SF1 was 6.5 to 10-fold higher than that in SF2. Extraction and measurement of the mass of iron and arsenic immobilized on the sand packing of the columns were close to the iron and arsenic removed from the aqueous phase during column operation. The dominant speciation of the immobilized iron and arsenic was Fe(III) and As(V) in SF1, compared with Fe(II) and As(III) in SF2. The speciation was confirmed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The results indicate that microbial oxidation of As(III) and Fe(II) linked to denitrification resulted in the enhanced immobilization of aqueous arsenic in anaerobic environments by forming Fe(III) (hydr)oxide coated sands with adsorbed As(V).

Environmental Science & Technology↗

USGS1998

Bacterial methylmercury degradation in Florida Everglades peat sediment

Methylmercury (MeHg) degradation was investigated along an eutrophication gradient in the Florida Everglades by quantifying 14 CH 4 and 14 CO 2 production after incubation of anaerobic sediments with [ 14 C]MeHg. Degradation rate constants ( k ) were consistently ≤0.1 d - 1 and decreased with sediment depth. Higher k values were observed when shorter incubation times and lower MeHg amendment levels were used, and k increased 2-fold as in-situ MeHg concentrations were approached. The average floc layer k was 0.046 ± 0.023 d - 1 ( n = 17) for 1−2 day incubations. In-situ degradation rates were estimated to be 0.02−0.5 ng of MeHg (g of dry sediment) - 1 d - 1 , increasing from eutrophied to pristine areas. Nitrate-respiring bacteria did not demethylate MeHg, and NO 3 - addition partially inhibited degradation in some cases. MeHg degradation rates were not affected by PO 4 3 - addition. 14 CO 2 production in all samples indicated that oxidative demethylation (OD) was an important degradation mechanism. OD occurred over 5 orders of magnitude of applied MeHg concentration, with lowest limits [1−18 ng of MeHg (g of dry sediment) - 1 ] in the range of in-situ MeHg levels. Sulfate reducers and methanogens were the primary agents of anaerobic OD, although it is suggested that methanogens dominate degradation at in-situ MeHg concentrations. Specific pathways of OD by these two microbial groups are proposed.

Florida↗