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At least 343 records · Page 19Linked to original sources
USGS2006

Role of microbial iron reduction in the dissolution of iron hydroxysulfate minerals

Iron-hydroxysulfate minerals can be important hosts for metals such as lead, mercury, copper, zinc, silver, chromium, arsenic, and selenium and for radionuclides such as 226Ra. These mineral-bound contaminants are considered immobilized under oxic conditions. However, when anoxic conditions develop, the activities of sulfate- or iron-reducing bacteria could result in mineral dissolution, releasing these bound contaminants. Reduction of structural sulfate in the iron-hydroxysulfate mineral jarosite by sulfate-reducing bacteria has previously been demonstrated. The primary objective of this work was to evaluate the potential for anaerobic dissolution of the iron-hydroxysulfate minerals jarosite and schwertmannite at neutral PH by iron-reducing bacteria. Mineral dissolution was tested using a long-term cultivar, Geobacter metallireducens strain GS-15, and a fresh isolate Geobacter sp. strain ENN1, previously undescribed. ENN1 was isolated from the discharge site of Shadle Mine, in the southern anthracite coalfield of Pennsylvania, where schwertmannite was the predominant iron-hydroxysulfate mineral. When jarosite from Elizabeth Mine (Vermont) was provided as the sole terminal electron acceptor, resting cells of both G. metallireducens and ENN1 were able to reduce structural Fe(III), releasing Fe+2, SO4-2, and K+ ions. A lithified jarosite sample from Utah was more resistant to microbial attack, but slow release of Fe+2 was observed. Neither bacterium released Fe+2 from poorly crystalline synthetic schwertmannite. Our results indicate that exposure of jarosite to iron-reducing conditions at neutral pH is likely to promote the mobility of hazardous constituents and should therefore be considered in evaluating waste disposal and/or reclamation options involving jarosite-bearing materials.

Journal of Geophysical Research G: Biogeosciences↗
USGS2008

Dating groundwater with trifluoromethyl sulfurpentafluoride (SF 5CF3), sulfur hexafluoride (SF6), CF 3Cl (CFC-13), and CF2Cl2 (CFC-12)

[1] A new groundwater dating procedure using the transient atmospheric signal of the environmental tracers SF5CF3, CFC-13, SF6, and CFC-12 was developed. The analytical procedure determines concentrations of the four tracers in air and water samples. SF 5CF3 and CFC-13 can be used to date groundwaters in some environments where the CFCs and SF6 have previously failed because these new tracers have increasing atmospheric input functions, no known terrigenic source, and are believed to be stable under reducing conditions. SF5CF3 has a dating range from 1970 to modern; the mixing ratio (mole fraction) in North American air has increased from the detection limit of 0.005 parts per trillion (ppt) to the 2006 mole fraction of about 0.16 ppt. No evidence was found for degradation of SF5CF3 in laboratory anaerobic systems. The solubility of SF5CF3 was measured in water from 1 to 35??C. Groundwater samples that contained large amounts of terrigenic SF6 did not contain terrigenic SF 5CF3. CFC-13 is a trace atmospheric gas with a dating range in groundwater of about 1965 to modem. CFC-13 has been used primarily in very low-temperature refrigeration; thus groundwater environments are less likely to be contaminated with nonatmospheric sources as compared to other widely used CFCs. Because of the low solubility of SF5CF3 and CFC-13 in water, an excess air correction must be applied to the apparent ages. The new dating procedure was tested in water samples from wells and springs from Maryland, Virginia, and West Virginia.

Water Resources Research↗
USGS2011

Magnetic susceptibility as a proxy for investigating microbially mediated iron reduction

We investigated magnetic susceptibility (MS) variations in hydrocarbon contaminated sediments. Our objective was to determine if MS can be used as an intrinsic bioremediation indicator due to the activity of iron-reducing bacteria. A contaminated and an uncontaminated core were retrieved from a site contaminated with crude oil near Bemidji, Minnesota and subsampled for MS measurements. The contaminated core revealed enriched MS zones within the hydrocarbon smear zone, which is related to iron-reduction coupled to oxidation of hydrocarbon compounds and the vadose zone, which is coincident with a zone of methane depletion suggesting aerobic or anaerobic oxidation of methane is coupled to iron-reduction. The latter has significant implications for methane cycling. We conclude that MS can serve as a proxy for intrinsic bioremediation due to the activity of iron-reducing bacteria iron-reducing bacteria and for the application of geophysics to iron cycling studies.

Minnesota↗
USGS2018

Direct observations of hydrologic exchange occurring with less‐mobile porosity and the development of anoxic microzones in sandy lakebed sediments

Quantifying coupled mobile/less‐mobile porosity dynamics is critical to the prediction of biogeochemical storage, release, and transformation processes in the zone where groundwater and surface water exchange. The recent development of fine‐scale geoelectrical monitoring paired with pore‐water sampling in groundwater systems enables direct characterization of hydrologic exchange between more‐ and less‐mobile porosity during tracer tests. We adapt this technique to sandy interface sediments at a groundwater flow‐through kettle lake. Tracer experiments were conducted within controlled‐head permeameters over a range of specified downward flow conditions over several days. Although the bed was predominantly composed of highly permeable sands and gravels, cobble inclusions created less‐mobile flow zones at the centimeter scale. Less‐mobile porosity fractions, residence times, and rates of exchange were inferred from paired bulk and fluid electrical conductivity data, without the need for inverse model calibration. The conservative solute experiments were paired with 15 NO 3 − and other reactive amendments, revealing anaerobic processes occurring at shallow sediment depths where pore‐water sampling indicated bulk‐oxic conditions. The average less‐mobile porosity residence times as evaluated with the geoelectrical method were on 1‐hr timescales, which appear to be biogeochemically important in the context of creating anoxic microzones within less‐mobile porosity of sandy interface sediments.

Water Resources Research↗
USGS2020

Formation criteria for hyporheic anoxic microzones: Assessing interactions of hydraulics, nutrients and biofilms

Recent experimental studies have detected the presence of anoxic microzones in hyporheic sediments. These microzones are small‐scale anoxic pores, embedded within oxygen‐rich porous media and can act as anaerobic reaction sites producing reduction compounds such as nitrous oxide, a potent greenhouse gas. Microbes are a key control on nutrient transformation in hyporheic sediment, but their associated biomass growth is also capable of altering hydraulic flux, leading to potential bioclogging. Here, we developed one of the first computational modeling approaches that combined hydraulics and microbial conditions to explore the continuous evolution of microzones in stream sediments. The model assessed stream and sediment conditions with different hydraulic flux (0.1–1.0 m/day Darcy flux), nutrient concentrations (O 2 = 8 mg/L, OrgC = 20 mg/L, NO − 3 = 1.5–3 mg/L, and NH 3 = 0.5–1 mg/L), and biomass scenarios (with and without). The model domain is a pore network model with random sized pore‐throat radii creating heterogeneous and anisotropic flow that is representative of a natural streambed composed of medium sand with a hydraulic conductivity of 0.8 m/day. Results from 30 day simulations indicate that hyporheic microzone formation will occur and microzone distributions are not simply controlled by residence time alone, rather by the complex interactions of hydraulic flux, nutrient concentrations, and biomass, with bioclogging having strong feedbacks on both hydraulics and nutrients. Under all conditions with biomass growth, anoxic microzones were unstable, perishing a few days after formation, because bioclogging primarily occurs near the influent (downwelling) area of the hyporheic zone. In turn, this bioclogging shifts transport conditions from advection‐dominated to diffusion‐dominated transport, removing all oxic regions in the hyporheic zone. Overall, results from the modeling show that anoxic microzones are likely to form under many hyporheic zone conditions, and be dynamic through space and time as they are dependent on both hydraulic flux and nutrient transport.

Water Resources Research↗
USGS2021

Isolating detrital and diagenetic signals in magnetic susceptibility records from methane-bearing marine sediments

Volume-dependent magnetic susceptibility (κ) is commonly used for paleoenvironmental reconstructions in both terrestrial and marine sedimentary environments where it reflects a mixed signal between primary deposition and secondary diagenesis. In the marine environment, κ is strongly influenced by the abundance of ferrimagnetic minerals regulated by sediment transport processes. Post-depositional alteration by H 2 S, however, can dissolve titanomagnetite, releasing reactive Fe that promotes pyritization and subsequently decreases κ. Here, we provide a new approach for isolating the detrital signal in κ and identifying intervals of diagenetic alteration of κ driven by organoclastic sulfate reduction (OSR) and the anaerobic oxidation of methane (AOM) in methane-bearing marine sediments offshore India. Using the correlation of a heavy mineral proxy from X-ray fluorescence data (Zr/Rb) and κ in unaltered sediments, we predict the primary detrital κ signal and identify intervals of decreased κ, which correspond to increased total sulfur content. Our approach is a rapid, high-resolution method that can identify overprinted κ resulting from pyritization of titanomagnetite due to H 2 S production in marine sediments. In addition, total organic carbon, total sulfur, and authigenic carbonate δ 13 C measurements indicate that both OSR and AOM can drive the observed κ loss, but AOM drives the greatest decreases in κ. Overall, our approach can enhance paleoenvironmental reconstructions and provide insight into paleo-positions of the sulfate-methane transition zone, past enhancements of OSR or paleo-methane seepage, and the role of detrital iron oxide minerals on the marine sediment sulfur sink, with consequences influencing the development of chemosynthetic biological communities at methane seeps.

Geochemistry, Geophysics, Geosystems↗
USGS2023

Comparing sediment microbial communities of Arctic beaver ponds to tundra lakes and streams

In recent decades the habitat of North American beaver ( Castor canadensis ) has expanded from boreal forests into Arctic tundra ecosystems. Beaver ponds in Arctic watersheds are known to alter stream biogeochemistry, which is likely coupled with changes in the activity and composition of microbial communities inhabiting beaver pond sediments. We investigated bacterial, archaeal, and fungal communities in beaver pond sediments along tundra streams in northwestern Alaska (AK), USA and compared them to those of tundra lakes and streams in north-central Alaska that are unimpacted by beavers. β -glucosidase activity assays indicated higher cellulose degradation potential in beaver ponds than in unimpacted streams and lakes within a watershed absent of beavers. Beta diversity analyses showed that dominant lineages of bacteria and archaea in beaver ponds differed from those in tundra lakes and streams, but dominant fungal lineages did not differ between these sample types. Beaver pond sediments displayed lower relative abundances of Crenarchaeota and Euryarchaeota archaea and of bacteria from typically anaerobic taxonomic groups, suggesting differences in rates of fermentative organic matter (OM) breakdown, syntrophy, and methane generation. Beaver ponds also displayed low relative abundances of Chytridiomycota (putative non-symbiotic) fungi and high relative abundances of ectomycorrhizal (plant symbionts) Basidiomycota fungi, suggesting differences in the occurrence of plant and fungi mutualistic interactions. Beaver ponds also featured microbes with taxonomic identities typically associated with the cycling of nitrogen and sulfur compounds in higher relative abundances than tundra lakes and streams. These findings help clarify the microbiological implications of beavers expanding into high latitude regions.

Alaska↗
USGS2024

Subsurface redox interactions regulate ebullitive methane flux in heterogeneous Mississippi River deltaic wetland

As interfaces connecting terrestrial and ocean ecosystems, coastal wetlands develop temporally and spatially complex redox conditions, which drive uncertainties in greenhouse gas emission as well as the total carbon budget of the coastal ecosystem. To evaluate the role of complex redox reactions in methane emission from coastal wetlands, a coupled reactive-transport model was configured to represent subsurface biogeochemical cycles of carbon, nitrogen, and sulfur, along with production and transport of multiple gas species through diffusion and ebullition. This model study was conducted at multiple sites along a salinity gradient in the Barataria Basin at the Mississippi River Deltaic Plain. Over a freshwater to saline gradient, simulated total flux of methane was primarily controlled by its subsurface production and consumption, which were determined by redox reactions directly (e.g., methanogenesis, methanotrophy) and indirectly (e.g., competition with sulfate reduction) under aerobic and/or anaerobic conditions. At fine spatiotemporal scales, surface methane fluxes were also strongly dependent on transport processes, with episodic ebullitive fluxes leading to higher spatial and temporal variability compared to the gradient-driven diffusion flux. Ebullitive methane fluxes were determined by methane fraction in total ebullitive gas and the frequency of ebullitive events, both of which varied with subsurface methane concentrations and other gas species. Although ebullition thresholds are constrained by local physical factors, this study indicates that redox interactions not only determine gas composition in ebullitive fluxes but can also regulate ebullition frequency through gas production.

Journal of Advances in Modeling Earth Systems↗
USGS2025

Organic matter availability and the production of methane-derived dissolved organic carbon at methane seeps

Methane seeps located along continental margins and slopes export sedimentary methane and dissolved organic carbon (DOC) into the ocean. The flux of these reduced carbon molecules from the seafloor into the ocean impacts ocean chemistry and supports deep-sea life. While significant effort has been made to understand how the anaerobic oxidation of methane (AOM) regulates the release of methane from the seafloor, little is known about the production of DOC in association with AOM or its flux and fate in the ocean. We hypothesize a mechanism for methane incorporation into DOC at seeps and investigate the relationship between sediment total organic carbon (TOC) availability and the incorporation of methane-derived carbon into DOC at four methane seep regions along the Cascadia margin, with a range of microbial and thermogenic methane sources. At sites with <2.0 wt.% TOC (Hydrate Ridge and Bullseye Vent), up to 60%–80% of carbon in DOC is methane-carbon, much more than sites with >2.0 wt.% TOC (Astoria Canyon and Barkley Canyon). We attribute the greater methane contribution at the more TOC-limited sites to a greater role of AOM in the carbon cycle, whereas at the organic matter-rich sites, microbial competition for sulfate as an electron acceptor for organic matter decomposition limits AOM and hence the transfer of carbon from methane to DOC. We estimate that the global diffusive flux of methane-derived DOC from the seafloor is 0.07–10.1 Tg C/yr, contributing to the stock of DOC present in the deep ocean and/or fueling the deep-sea microbial loop.

California, Oregon, Washington↗
USGS2010

Long-term frozen storage of stream water samples for dissolved orthophosphate, nitrate plus nitrite, and ammonia analysis

Many researchers have used freezing as an effective, short-term, water sample preservation method for subsequent nutrient analysis. In this study, filtered samples held at −16±2°C for 4–8 years were reanalyzed for orthophosphate, nitrate plus nitrite, and ammonia. Orthophosphate and ammonia concentrations decreased by 0.2 μg P/L and 5 μg N/L, respectively, at mean concentrations of 69.4 μg P/L and 246 μg N/L. Nitrate plus nitrite increased by 1.1 μg N/L at a mean concentration of 139.1 μg N/L. An anaerobic well sample proved to be unsuitable for freezing because it lost significant amounts of orthophosphate during the freezing process. None of the differences observed over long periods of frozen storage were more than twice the estimated standard deviation of the analytical methods used in the study. The small changes observed demonstrate the effectiveness of frozen storage as a means of nutrient preservation in water samples that are unaffected by the freezing process itself.

Water Resources Research↗
USGS2010

Chemical evolution of groundwater near a sinkhole lake, northern Florida: 2. Chemical patterns, mass-transfer modeling, and rates of chemical reactions

Chemical patterns along evolutionary groundwater flow paths in silicate and carbonate aquifers were interpreted using solute tracers, carbon and sulfur isotopes, and mass balance reaction modeling for a complex hydrologic system involving groundwater inflow to and outflow from a sinkhole lake in northern Florida. Rates of dominant reactions along defined flow paths were estimated from modeled mass transfer and ages obtained from CFC-modeled recharge dates. Groundwater upgradient from Lake Barco remains oxic as it moves downward, reacting with silicate minerals in a system open to carbon dioxide (CO 2 ), producing only small increases in dissolved species. Beneath and downgradient of Lake Barco the oxic groundwater mixes with lake water leakage in a highly reducing, silicate-carbonate mineral environment. A mixing model, developed for anoxic groundwater downgradient from the lake, accounted for the observed chemical and isotopic composition by combining different proportions of lake water leakage and infiltrating meteoric water. The evolution of major ion chemistry and the 13 C isotopic composition of dissolved carbon species in groundwater downgradient from the lake can be explained by the aerobic oxidation of organic matter in the lake, anaerobic microbial oxidation of organic carbon, and incongruent dissolution of smectite minerals to kaolinite. The dominant process for the generation of methane was by the CO 2 reduction pathway based on the isotopic composition of hydrogen (δ 2 H(CH 4 ) = −186 to −234‰) and carbon (δ 13 C(CH 4 ) = −65.7 to −72.3‰). Rates of microbial metabolism of organic matter, estimated from the mass transfer reaction models, ranged from 0.0047 to 0.039 mmol L −1 yr −1 for groundwater downgradient from the lake.

Water Resources Research↗
USGS2010

Chemical evolution of groundwater near a sinkhole lake, northern Florida: 1. Flow patterns, age of groundwater, and influence of lakewater leakage

Leakage from sinkhole lakes significantly influences recharge to the Upper Floridan aquifer in poorly confined sediments in northern Florida. Environmental isotopes (oxygen 18, deuterium, and tritium), chlorofluorocarbons (CFCs: CFC-11, CCl 3 F; CFC-12, CCl 2 F 2 ; and CFC-113, C 2 Cl 3 F 3 ), and solute tracers were used to investigate groundwater flow patterns near Lake Barco, a seepage lake in a mantled karst setting in northern Florida. Stable isotope data indicated that the groundwater downgradient from the lake contained 11–67% lake water leakage, with a limit of detection of lake water in groundwater of 4.3%. The mixing fractions of lake water leakage, which passed through organic-rich sediments in the lake bottom, were directly proportional to the observed methane concentrations and increased with depth in the groundwater flow system. In aerobic groundwater upgradient from Lake Barco, CFC-modeled recharge dates ranged from 1987 near the water table to the mid 1970s for water collected at a depth of 30 m below the water table. CFC-modeled recharge dates (based on CFC-12) for anaerobic groundwater downgradient from the lake ranged from the late 1950s to the mid 1970s and were consistent with tritium data. CFC-modeled recharge dates based on CFC-11 indicated preferential microbial degradation in anoxic waters. Vertical hydraulic conductivities, calculated using CFC-12 modeled recharge dates and Darcy's law, were 0.17, 0.033, and 0.019 m/d for the surficial aquifer, intermediate confining unit, and lake sediments, respectively. These conductivities agreed closely with those used in the calibration of a three-dimensional groundwater flow model for transient and steady state flow conditions.

Florida↗
USGS1982

Methane production and simultaneous sulphate reduction in anoxic, salt marsh sediments

It has been generally believed that sulphate reduction precludes methane generation during diagenesis of anoxic sediments1,2. Because most biogenic methane formed in nature is thought to derive either from acetate cleavage or by hydrogen reduction of carbon dioxide3-6, the removal of these compounds by the energetically more efficient sulphate-reducing bacteria can impose a substrate limitation on methanogenic bacteria 7-9. However, two known species of methanogens, Methanosarcina barkeri and Methanococcus mazei, can grow on and produce methane from methanol and methylated amines10-13. In addition, these compounds stimulate methane production by bacterial enrichments from the rumen11,14 and aquatic muds13,14. Methanol can enter anaerobic food webs through bacterial degradation of lignins15 or pectin16, and methylated amines can be produced either from decomposition of substances like choline, creatine and betaine13,14 or by bacterial reduction of trimethylamine oxide17, a common metabolite and excretory product of marine animals. However, the relative importance of methanol and methylated amines as precursors of methane in sediments has not been previously examined. We now report that methanol and trimethylamine are important substrates for methanogenic bacteria in salt marsh sediments and that these compounds may account for the bulk of methane produced therein. Furthermore, because these compounds do not stimulate sulphate reduction, methanogenesis and sulphate reduction can operate concurrently in sulphate-containing anoxic sediments. ?? 1982 Nature Publishing Group.

Nature↗
USGS1991

Microbial production of organic acids in aquitard sediments and its role in aquifer geochemistry

Microbial activity in aquifers plays an important part in the chemical evolution of ground water 1–5 . The most important terminal electron-accepting microbial processes in deeply buried anaerobic aquifers are iron reduction, sulphate reduction and methanogenesis 5–8 , each of which requires simple organic compounds or hydrogen (H 2 ) as electron donors. Until now, the source of these compounds was unknown because the concentrations of dissolved organic carbon and sedimentary organic carbon in aquifers are extremely low 9–11 . Here we show that rates of microbial fermentation exceed rates of respiration in organic-rich aquitards (low-permeability sediments stratigraphically adjacent to higher-permeability aquifer sediments), resulting in a net accumulation of simple organic acids in pore waters. In aquifers, however, respiration outpaces fermentation, resulting in a net consumption of organic acids. The concentration gradient that develops in response to these two processes drives a net diffusive flux of organic acids from aquitards to aquifers. Diffusion calculations demonstrate that rates of organic acid transport are sufficient to account for observed rates of microbial respiration in aquifers. This overall process effectively links the large pool of sedimentary organic carbon in aquitards to microbial respiration in aquifers, and is a principal mechanism driving groundwater chemistry changes in aquifers.

Nature↗
USGS2000

Biogeochemistry: Hexadecane decay by methanogenesis

The potential for the biological conversion of long-chain saturated hydrocarbons to methane under anaerobic conditions has been demonstrated by using an enrichment culture of bacteria to degrade pure-phase hexadecane . The formation of methane in hydrocarbon-rich subsurface zones could be explained if a similar conversion of long-chain alkanes to methane were to take place in subsurface environments. If this process could be stimulated in the subsurface, it could be used to enhance hydrocarbon recovery from petroleum reserves . Parkes , however, questions the environmental significance of the enrichment-culture results 1 on the grounds that alkane conversion to methane is very slow and because sulphate-reducing and methanogenic bacteria might both be necessary for even this slow process to occur, restricting the conversion to specialized, unusual zones in sediments. Here we show that, on the contrary, subsurface bacteria can adapt to convert hexadecane to methane rapidly and in the absence of sulphate-reducing bacteria.

Nature↗
USGS2018

Contribution of hurricane-induced sediment resuspension to coastal oxygen dynamics

Hurricanes passing over the ocean can mix the water column down to great depths and resuspend massive volumes of sediments on the continental shelves. Consequently, organic carbon and reduced inorganic compounds associated with these sediments can be resuspended from anaerobic portions of the seabed and re-exposed to dissolved oxygen (DO) in the water column. This process can drive DO consumption as sediments become oxidized. Previous studies have investigated the effect of hurricanes on DO in different coastal regions of the world, highlighting the alleviation of hypoxic conditions by extreme winds, which drive vertical mixing and re-aeration of the water column. However, the effect of hurricane-induced resuspended sediments on DO has been neglected. Here, using a diverse suite of datasets for the northern Gulf of Mexico, we find that in the few days after a hurricane passage, decomposition of resuspended shelf sediments consumes up to a fifth of the DO added to the bottom of the water column during vertical mixing. Despite uncertainty in this value, we highlight the potential significance of this mechanism for DO dynamics. Overall, sediment resuspension likely occurs over all continental shelves affected by tropical cyclones, potentially impacting global cycles of marine DO and carbon.

Scientific Reports↗
USGS2003

Relationships between metabolic rate, muscle electromyograms and swim performance of adult chinook salmon

Oxygen consumption rates of adult spring chinook salmon Oncorhynchus tshawytscha increased with swim speed and, depending on temperature and fish mass, ranged from 609 mg O2 h-1 at 30 cm s-1 (c. 0.5 BLs-1) to 3347 mg O2 h-1 at 170 cm s -1 (c. 2.3 BLs-1). Corrected for fish mass, these values ranged from 122 to 670 mg O2 kg-1 h-1, and were similar to other Oncorhynchus species. At all temperatures (8, 12.5 and 17??C), maximum oxygen consumption values levelled off and slightly declined with increasing swim speed >170 cm s-1, and a third-order polynomial regression model fitted the data best. The upper critical swim speed (Ucrit) of fish tested at two laboratories averaged 155 cm s -1 (2.1 BLs-1), but Ucrit of fish tested at the Pacific Northwest National Laboratory were significantly higher (mean 165 cm s-1) than those from fish tested at the Columbia River Research Laboratory (mean 140 cm s-1). Swim trials using fish that had electromyogram (EMG) transmitters implanted in them suggested that at a swim speed of c. 135 cm s-1, red muscle EMG pulse rates slowed and white muscle EMG pulse rates increased. Although there was significant variation between individual fish, this swim speed was c. 80% of the Ucrit for the fish used in the EMG trials (mean Ucrit 168.2 cm s-1). Bioenergetic modelling of the upstream migration of adult chinook salmon should consider incorporating an anaerobic fraction of the energy budget when swim speeds are ???80% of the Ucrit. ?? 2003 The Fisheries Society of the British Isles.

Journal of Fish Biology↗
USGS2010

Nitrous oxide emission from denitrification in stream and river networks

Nitrous oxide (N 2 O) is a potent greenhouse gas that contributes to climate change and stratospheric ozone destruction. Anthropogenic nitrogen (N) loading to river networks is a potentially important source of N 2 O via microbial denitrification that converts N to N 2 O and dinitrogen (N 2 ). The fraction of denitrified N that escapes as N 2 O rather than N 2 (i.e., the N 2 O yield) is an important determinant of how much N 2 O is produced by river networks, but little is known about the N 2 O yield in flowing waters. Here, we present the results of whole-stream 15 N-tracer additions conducted in 72 headwater streams draining multiple land-use types across the United States. We found that stream denitrification produces N 2 O at rates that increase with stream water nitrate (NO 3 − ) concentrations, but that <1% of denitrified N is converted to N 2 O. Unlike some previous studies, we found no relationship between the N 2 O yield and stream water NO 3 − . We suggest that increased stream NO 3 − loading stimulates denitrification and concomitant N 2 O production, but does not increase the N 2 O yield. In our study, most streams were sources of N 2 O to the atmosphere and the highest emission rates were observed in streams draining urban basins. Using a global river network model, we estimate that microbial N transformations (e.g., denitrification and nitrification) convert at least 0.68 Tg·y −1 of anthropogenic N inputs to N 2 O in river networks, equivalent to 10% of the global anthropogenic N 2 O emission rate. This estimate of stream and river N 2 O emissions is three times greater than estimated by the Intergovernmental Panel on Climate Change. Humans have more than doubled the availability of fixed nitrogen (N) in the biosphere, particularly through the production of N fertilizers and the cultivation of N-fixing crops ( 1 ). Increasing N availability is producing unintended environmental consequences including enhanced emissions of nitrous oxide (N 2 O), a potent greenhouse gas ( 2 ) and an important cause of stratospheric ozone destruction ( 3 ). The Intergovernmental Panel on Climate Change (IPCC) estimates that the microbial conversion of agriculturally derived N to N 2 O in soils and aquatic ecosystems is the largest source of anthropogenic N 2 O to the atmosphere ( 2 ). The production of N 2 O in agricultural soils has been the focus of intense investigation (i.e., >1,000 published studies) and is a relatively well constrained component of the N 2 O budget ( 4 ). However, emissions of anthropogenic N 2 O from streams, rivers, and estuaries have received much less attention and remain a major source of uncertainty in the global anthropogenic N 2 O budget. Microbial denitrification is a large source of N 2 O emissions in terrestrial and aquatic ecosystems. Most microbial denitrification is a form of anaerobic respiration in which nitrate (NO 3 − , the dominant form of inorganic N) is converted to dinitrogen (N 2 ) and N 2 O gases ( 5 ). The proportion of denitrified NO 3 − that is converted to N 2 O rather than N 2 (hereafter referred to as the N 2 O yield and expressed as the mole ratio) partially controls how much N 2 O is produced via denitrification ( 6 ), but few studies provide information on the N 2 O yield in streams and rivers because of the difficulty of measuring N 2 and N 2 O production in these systems. Here we report rates of N 2 and N 2 O production via denitrification measured using whole-stream 15 NO 3 − -tracer experiments in 72 headwater streams draining different land-use types across the United States. This project, known as the second Lotic Intersite Nitrogen eXperiment (LINX II), provides unique whole-system measurements of the N 2 O yield in streams. Although N 2 O emission rates have been reported for streams and rivers ( 7 , 8 ), the N 2 O yield has been studied mostly in lentic freshwater and marine ecosystems, where it generally ranges between 0.1 and 1.0%, although yields as high as 6% have been observed ( 9 ). These N 2 O yields are low compared with observations in soils (0–100%) ( 10 ), which may be a result of the relatively lower oxygen (O 2 ) availability in the sediments of lakes and estuaries. However, dissolved O 2 in headwater streams is commonly near atmospheric equilibrium and benthic algal biofilms can produce O 2 at the sediment–water interface, resulting in strong redox gradients more akin to those in partially wetted soils. Thus, streams may have variable and often high N 2 O yields, similar to those in soils ( 11 ). The N 2 O yield in headwater streams is of particular interest because much of the NO 3 − input to rivers is derived from groundwater upwelling into headwater streams. Furthermore, headwater streams compose the majority of stream length within a drainage network and have high ratios of bioreactive benthic surface area to water volume ( 12 ).

Proceedings of the National Academy of Sciences of↗