Bioturbation frequency alters methane emissions from reservoir sediments.

Inland aquatic systems are major global contributors to the atmospheric carbon budget through greenhouse gas (GHG) emissions, although the amount and form of carbon released varies widely across and within systems. Bioturbation of aquatic sediments can impact biogeochemical conditions and physically release sediment-bound bubbles containing GHGs, but variation in the frequency of such disturbance may modify the rate and composition of resulting GHG emissions. We hypothesized that an intermediate bioturbation frequency would result in the greatest methane (CH4) releases due to mechanical release of trapped bubbles, while frequent disturbance would result in greater diffusive carbon dioxide (CO2) releases relative to CH4, due to increased aeration of the sediment. We tested this bioturbation frequency hypothesis using laboratory mesocosms containing homogenized reservoir sediment. We used mechanical disturbance to simulate bioturbation at 3, 7, 14, or 21-day intervals; a control treatment was undisturbed for the duration of the experiment. We measured GHG emission (ebullition and diffusion) rates. An intermediate frequency of disturbance (7 days) produced the highest total GHG emission rate, while the most frequent disturbance interval (3 days) and least frequent interval (0 days) reduced overall GHG emissions relative to weekly disturbance by 24% and 15%, respectively. These patterns were primarily driven by differences in CH4 ebullition. Contrary to our hypothesis, there was no relationship between disturbance frequency and diffusive CO2 emissions. For all disturbance treatments, the majority of ebullition occurred during disturbance events, suggesting mechanical release of entrapped bubbles is an important emission mechanism. The frequency of disturbance has variable effects on GHG emissions and may explain conflicting results in prior studies of bioturbation. Our study provides insight into bioturbation as a driver of within-system variation in GHG emissions and highlights that variable bioturbation frequency results in non-linear responses in CH4 emissions, a globally important GHG, from reservoir sediments.

Increasingly severe cyanobacterial blooms and deep water hypoxia coincide with warming water temperatures in reservoirs.

Cyanobacterial blooms are expected to intensify and become more widespread with climate change and sustained nutrient pollution, subsequently increasing threats to lentic ecosystems, water quality, and human health. However, little is known about their rates of change because long-term monitoring data are rare, except for some well-studied individual lakes, which typically are large and broadly dispersed geographically. Using monitoring data spanning 1987-2018 for 20 temperate reservoirs located in the USA, we found that cyanobacteria cell densities mostly posed low-to-moderate human health risks until 2003-2005, after which cell densities rapidly increased. Increases were greatest in reservoirs with extensive agriculture in their watersheds, but even those with mostly forested watersheds experienced increases. Since 2009, cell densities posing high human health risks have become frequent with 75% of yearly observations exceeding 100,000 cells ml-1 , including 53% of observations from reservoirs with mostly forested watersheds. These increases coincided with progressively earlier and longer summer warming of surface waters, evidence of earlier onset of stratification, lengthening durations of deep-water hypoxia, and warming deep waters in non-stratifying reservoirs. Among years, higher cell densities in stratifying reservoirs were associated with greater summer precipitation, warmer June surface water temperatures, and higher total Kjeldahl nitrogen concentrations. These trends are evidence that expected increases in cyanobacterial blooms already are occurring as changing climate conditions in some regions increasingly favor their proliferation. Consequently, their negative effects on ecosystems, human health, and socioeconomic wellbeing could increase and expand if warming trends and nutrient pollution continue.

Temporal trends in methane emissions from a small eutrophic reservoir: the key role of a spring burst.

Waters impounded behind dams (i.e., reservoirs) are important sources of greenhouses gases (GHGs), especially methane (CH4), but emission estimates are not well constrained due to high spatial and temporal variability, limitations in monitoring methods to characterize hot spot and hot moment emissions, and the limited number of studies that investigate diurnal, seasonal, and interannual patterns in emissions. In this study, we investigate the temporal patterns and biophysical drivers of CH4 emissions from Acton Lake, a small eutrophic reservoir, using a combination of methods: eddy covariance monitoring, continuous warm-season ebullition measurements, spatial emission surveys, and measurements of key drivers of CH4 production and emission. We used an artificial neural network to gap fill the eddy covariance time series and to explore the relative importance of biophysical drivers on the interannual timescale. We combined spatial and temporal monitoring information to estimate annual whole-reservoir emissions. Acton Lake had cumulative areal emission rates of 45.6 ± 8.3 and 51.4 ± 4.3 g CH4 m-2 in 2017 and 2018, respectively, or 109 ± 14 and 123 ± 10 Mg CH4 in 2017 and 2018 across the whole 2.4 km2 area of the lake. The main difference between years was a period of elevated emissions lasting less than 2 weeks in the spring of 2018, which contributed 17 % of the annual emissions in the shallow region of the reservoir. The spring burst coincided with a phytoplankton bloom, which was likely driven by favorable precipitation and temperature conditions in 2018 compared to 2017. Combining spatially extensive measurements with temporally continuous monitoring enabled us to quantify aspects of the spatial and temporal variability in CH4 emission. We found that the relationships between CH4 emissions and sediment temperature depended on location within the reservoir, and we observed a clear spatiotemporal offset in maximum CH4 emissions as a function of reservoir depth. These findings suggest a strong spatial pattern in CH4 biogeochemistry within this relatively small (2.4 km2) reservoir. In addressing the need for a better understanding of GHG emissions from reservoirs, there is a trade-off in intensive measurements of one water body vs. short-term and/or spatially limited measurements in many water bodies. The insights from multi-year, continuous, spatially extensive studies like this one can be used to inform both the study design and emission upscaling from spatially or temporally limited results, specifically the importance of trophic status and intra-reservoir variability in assumptions about upscaling CH4 emissions.

Spatial variability of sediment methane production and methanogen communities within a eutrophic reservoir: Importance of organic matter source and quantity.

Freshwater reservoirs are an important source of the greenhouse gas methane (CH4) to the atmosphere, but global emission estimates are poorly constrained (13.3-52.5 Tg C yr-1), partially due to extreme spatial variability in emission rates within and among reservoirs. Spatial heterogeneity in the availability of organic matter (OM) for biological CH4 production by methanogenic archaea may be an important contributor to this variation. To investigate this, we measured sediment CH4 potential production rates, OM source and quantity, and methanogen community composition at 15 sites within a eutrophic reservoir in Ohio, USA. CH4 production rates were highest in the shallow riverine inlet zone of the reservoir, even when rates were normalized to OM quantity, indicating that OM was more readily utilized by methanogens in the riverine zone than in the transitional or lacustrine zones. Sediment stable isotopes and C:N indicated a greater proportion of terrestrial OM in the particulate sediment of this zone. Methanogens were present at all sites, but the riverine zone contained a higher relative abundance of methanogens capable of acetoclastic and methylotrophic methanogenesis, likely reflecting differences in decomposition processes or OM quality. While we found that methane potential production rates were negatively correlated with autochthonous carbon in particulate sediment OM, rates were positively correlated with indicators of autochthonous carbon in the porewater dissolved OM. It is likely that both dissolved and particulate sediment OM affect CH4 production rates, and that both terrestrial and aquatic OM sources are important in the riverine methane production hot spot.

Methane and Carbon Dioxide Emissions From Reservoirs: Controls and Upscaling.

Estimating carbon dioxide (CO2) and methane (CH4) emission rates from reservoirs is important for regional and national greenhouse gas inventories. A lack of methodologically consistent data sets for many parts of the world, including agriculturally intensive areas of the United States, poses a major challenge to the development of models for predicting emission rates. In this study, we used a systematic approach to measure CO2 and CH4 diffusive and ebullitive emission rates from 32 reservoirs distributed across an agricultural to forested land use gradient in the United States. We found that all reservoirs were a source of CH4 to the atmosphere, with ebullition being the dominant emission pathway in 75% of the systems. Ebullition was a negligible emission pathway for CO2, and 65% of sampled reservoirs were a net CO2 sink. Boosted regression trees (BRTs), a type of machine learning algorithm, identified reservoir morphology and watershed agricultural land use as important predictors of emission rates. We used the BRT to predict CH4 emission rates for reservoirs in the U.S. state of Ohio and estimate they are the fourth largest anthropogenic CH4 source in the state. Our work demonstrates that CH4 emission rates for reservoirs in our study region can be predicted from information in readily available national geodatabases. Expanded sampling campaigns could generate the data needed to train models for upscaling in other U.S. regions or nationally.

Eutrophication will increase methane emissions from lakes and impoundments during the 21st century.

Lakes and impoundments are an important source of methane (CH4), a potent greenhouse gas, to the atmosphere. A recent analysis shows aquatic productivity (i.e., eutrophication) is an important driver of CH4 emissions from lentic waters. Considering that aquatic productivity will increase over the next century due to climate change and a growing human population, a concomitant increase in aquatic CH4 emissions may occur. We simulate the eutrophication of lentic waters under scenarios of future nutrient loading to inland waters and show that enhanced eutrophication of lakes and impoundments will substantially increase CH4 emissions from these systems (+30-90%) over the next century. This increased CH4 emission has an atmospheric impact of 1.7-2.6 Pg C-CO2-eq y-1, which is equivalent to 18-33% of annual CO2 emissions from burning fossil fuels. Thus, it is not only important to limit eutrophication to preserve fragile water supplies, but also to avoid acceleration of climate change.

Effects of an Experimental Water-level Drawdown on Methane Emissions from a Eutrophic Reservoir.

Reservoirs are a globally significant source of methane (CH4) to the atmosphere. However, emission rate estimates may be biased low due to inadequate monitoring during brief periods of elevated emission rates (that is, hot moments). Here we investigate CH4 bubbling (that is, ebullition) during periods of falling water levels in a eutrophic reservoir in the Midwestern USA. We hypothesized that periods of water-level decline trigger the release of CH4-rich bubbles from the sediments and that these emissions constitute a substantial fraction of the annual CH4 flux. We explored this hypothesis by monitoring CH4 ebullition in a eutrophic reservoir over a 7-month period, which included an experimental water-level drawdown. We found that the ebullitive CH4 flux rate was among the highest ever reported for a reservoir (mean = 32.3 mg CH4 m-2 h-1). The already high ebullitive flux rates increased by factors of 1.4-77 across the nine monitoring sites during the 24-h experimental water-level drawdown, but these emissions constituted only 3% of the CH4 flux during the 7-month monitoring period due to the naturally high ebullitive CH4 flux rates that persist throughout the warm weather season. Although drawdown emissions were found to be a minor component of annual CH4 emissions in this reservoir, our findings demonstrate a link between water-level change and CH4 ebullition, suggesting that CH4 emissions may be mitigated through water-level management in some reservoirs.

Watershed Land Use and Seasonal Variation Constrain the Influence of Riparian Canopy Cover on Stream Ecosystem Metabolism.

Ecosystem metabolism is an important determinant of trophic structure, nutrient cycling, and other critical ecosystem processes in streams. Whereas watershed- and local-scale controls on stream metabolism have been independently investigated, little is known about how controls exerted at different scales interact to determine stream metabolic rates, particularly in urban streams and across seasons. To address this knowledge gap, we measured ecosystem metabolism in four urban and four reference streams in northern Kentucky, USA, with paired closed and open riparian canopies, during each of the four seasons. Gross primary production (GPP), ecosystem respiration, and net ecosystem production (NEP) were all best predicted by models with season as a main effect, but interactions between season, canopy, and watershed varied for each response. Urban streams exhibited higher GPP during most seasons, likely due to elevated nutrient loads. Open canopy reaches in both urban and forested streams, supported higher rates of GPP than the closed canopy which reaches during the summer and fall, when the overhead vegetation shaded the closed reaches. The effect of canopy cover on GPP was similar among urban and forested streams. The combination of watershed and local-scale controls resulted in urban streams that alternated between net heterotrophy (NEP <0) and net autotrophy (NEP >0) at the reach-scale during seasons with dense canopy cover. This finding has management relevance because net production can lead to accumulation of algal biomass and associated issues like nighttime hypoxia. Our study suggests that although watershed urbanization fundamentally alters ecosystem function, the preservation and restoration of canopied riparian zones can provide an important management tool at the local scale, with the strongest impacts on stream metabolism during summer.

Influence of infrastructure on water quality and greenhouse gas dynamics in urban streams.

Streams and rivers are significant sources of nitrous oxide (N2O), carbon dioxide (CO2), and methane (CH4) globally, and watershed management can alter greenhouse gas (GHG) emissions from streams. We hypothesized that urban infrastructure significantly alters downstream water quality and contributes to variability in GHG saturation and emissions. We measured gas saturation and estimated emission rates in headwaters of two urban stream networks (Red Run and Dead Run) of the Baltimore Ecosystem Study Long-Term Ecological Research project. We identified four combinations of stormwater and sanitary infrastructure present in these watersheds, including: (1) stream burial, (2) inline stormwater wetlands, (3) riparian/floodplain preservation, and (4) septic systems. We selected two first order catchments in each of these categories and measured GHG concentrations, emissions, and dissolved inorganic and organic carbon (DIC and DOC) and nutrient concentrations biweekly for 1 year. From a water quality perspective, the DOC : NO3 - ratio of streamwater was significantly different across infrastructure categories. Multiple linear regressions including DOC : NO3 - and other variables (dissolved oxygen, DO; total dissolved nitrogen, TDN; and temperature) explained much of the statistical variation in nitrous oxide (N2O, r2 = 0.78), carbon dioxide (CO2, r2 = 0.78) and methane (CH4, r 2 = 0.50) saturation in stream water. We measured N2O saturation ratios, which were among the highest reported in the literature for streams, ranging from 1.1 to 47 across all sites and dates. N2O saturation ratios were highest in streams draining watersheds with septic systems and strongly correlated with TDN. The CO2 saturation ratio was highly correlated with the N2O saturation ratio across all sites and dates, and the CO2 saturation ratio ranged from 1.1 to 73. CH4 was always supersaturated, with saturation ratios ranging from 3.0 to 2157. Longitudinal surveys extending form headwaters to third-order outlets of Red Run and Dead Run took place in spring and fall. Linear regressions of these data yielded significant negative relationships between each gas with increasing watershed size as well as consistent relationships between solutes (TDN or DOC, and DOC : TDN ratio) and gas saturation. Despite a decline in gas saturation between the headwaters and stream outlet, streams remained saturated with GHGs throughout the drainage network, suggesting that urban streams are continuous sources of CO2, CH4, and N2O. Our results suggest that infrastructure decisions can have significant effects on downstream water quality and greenhouse gases, and watershed management strategies may need to consider coupled impacts on urban water and air quality.

Urban infrastructure influences dissolved organic matter quality and bacterial metabolism in an urban stream network.

1. Urban streams are degraded by a suite of factors, including burial beneath urban infrastructure, such as roads or parking lots, which eliminates light and reduces direct organic matter inputs to streams from riparian zones. These changes to stream metabolism and terrestrial carbon contribution will likely have consequences for organic matter metabolism by microbes and dissolved organic matter (DOM) use patterns in streams. Respiration by heterotrophic biofilms drives the nitrogen and phosphorus cycles, but we lack a clear understanding of how stream burial and seasonality affect microbial carbon use. 2. We studied seasonal changes (autumn, spring, and summer) in organic matter metabolism by microbial communities in open and buried reaches of three urban streams in Cincinnati, OH. We characterised DOM quality using fluorescence spectroscopy and extracellular enzyme profiles, and we measured the respiration response to carbon supplements in nutrient diffusing substrata (NDS). We hypothesised: (1) that algal production would lead to higher quality DOM in spring compared to other seasons and in open compared to buried reaches, (2) lower reliance of microbial respiration on recalcitrant carbon sources in spring and in open reaches, and (3) that microbial respiration would increase in response to added carbon in autumn and in buried reaches. 3. Several fluorescence metrics showed higher quality DOM in spring than autumn, but only the metric of recalcitrant humic compounds varied by reach, with more humic DOM in open compared to buried reaches. This likely reflected open reaches as an avenue for direct terrestrial inputs from the riparian zone. 4. Extracellular enzyme assays showed that microbes in buried reaches allocated more effort to degrade recalcitrant carbon sources, consistent with a lack of labile carbon compounds due to limited photosynthesis. Nitrogen acquisition enzymes were highest in autumn coincident with riparian leaf inputs to the streams. Buried and open reaches both responded more strongly to added carbon in autumn when terrestrial leaf inputs dominated compared to the spring when vernal algal blooms were pronounced. 5. Our data show that stream burial affects the quality of the DOM pool with consequences for how microbes use those carbon sources, and that heterotrophic respiration increased on carbon-supplemented NDS in buried and open stream reaches in both seasons. Different carbon quality and use patterns suggest that urban stream infrastructure affects spatiotemporal patterns of bacterial respiration, with likely consequences for nitrogen and/or phosphorus cycling given that carbon use drives other biogeochemical cycles. Management actions that increase light to buried streams could shift the balance between allochthonous and autochthonous DOM in urban streams with consequences for spatiotemporal patterns in bacterial metabolism.

Greenhouse Gas Emissions from Reservoir Water Surfaces: A New Global Synthesis.

Collectively, reservoirs created by dams are thought to be an important source of greenhouse gases (GHGs) to the atmosphere. So far, efforts to quantify, model, and manage these emissions have been limited by data availability and inconsistencies in methodological approach. Here, we synthesize reservoir CH4, CO2, and N2O emission data with three main objectives: (1) to generate a global estimate of GHG emissions from reservoirs, (2) to identify the best predictors of these emissions, and (3) to consider the effect of methodology on emission estimates. We estimate that GHG emissions from reservoir water surfaces account for 0.8 (0.5-1.2) Pg CO2 equivalents per year, with the majority of this forcing due to CH4. We then discuss the potential for several alternative pathways such as dam degassing and downstream emissions to contribute significantly to overall emissions. Although prior studies have linked reservoir GHG emissions to reservoir age and latitude, we find that factors related to reservoir productivity are better predictors of emission.

Urban Stream Burial Increases Watershed-Scale Nitrate Export.

Nitrogen (N) uptake in streams is an important ecosystem service that reduces nutrient loading to downstream ecosystems. Here we synthesize studies that investigated the effects of urban stream burial on N-uptake in two metropolitan areas and use simulation modeling to scale our measurements to the broader watershed scale. We report that nitrate travels on average 18 times farther downstream in buried than in open streams before being removed from the water column, indicating that burial substantially reduces N uptake in streams. Simulation modeling suggests that as burial expands throughout a river network, N uptake rates increase in the remaining open reaches which somewhat offsets reduced N uptake in buried reaches. This is particularly true at low levels of stream burial. At higher levels of stream burial, however, open reaches become rare and cumulative N uptake across all open reaches in the watershed rapidly declines. As a result, watershed-scale N export increases slowly at low levels of stream burial, after which increases in export become more pronounced. Stream burial in the lower, more urbanized portions of the watershed had a greater effect on N export than an equivalent amount of stream burial in the upper watershed. We suggest that stream daylighting (i.e., uncovering buried streams) can increase watershed-scale N retention.

High methane emissions from a midlatitude reservoir draining an agricultural watershed.

Reservoirs are a globally significant source of methane (CH4), although most measurements have been made in tropical and boreal systems draining undeveloped watersheds. To assess the magnitude of CH4 emissions from reservoirs in midlatitude agricultural regions, we measured CH4 and carbon dioxide (CO2) emission rates from William H. Harsha Lake (Ohio, U.S.A.), an agricultural impacted reservoir, over a 13 month period. The reservoir was a strong source of CH4 throughout the year, emitting on average 176 ± 36 mg C m(-2) d(-1), the highest reservoir CH4 emissions profile documented in the United States to date. Contrary to our initial hypothesis, the largest CH4 emissions were during summer stratified conditions, not during fall turnover. The river-reservoir transition zone emitted CH4 at rates an order of magnitude higher than the rest of the reservoir, and total carbon emissions (i.e., CH4 + CO2) were also greater at the transition zone, indicating that the river delta supported greater carbon mineralization rates than elsewhere. Midlatitude agricultural impacted reservoirs may be a larger source of CH4 to the atmosphere than currently recognized, particularly if river deltas are consistent CH4 hot spots. We estimate that CH4 emissions from agricultural reservoirs could be a significant component of anthropogenic CH4 emissions in the U.S.A.

How much is enough? Minimal responses of water quality and stream biota to partial retrofit stormwater management in a suburban neighborhood.

Decentralized stormwater management approaches (e.g., biofiltration swales, pervious pavement, green roofs, rain gardens) that capture, detain, infiltrate, and filter runoff are now commonly used to minimize the impacts of stormwater runoff from impervious surfaces on aquatic ecosystems. However, there is little research on the effectiveness of retrofit, parcel-scale stormwater management practices for improving downstream aquatic ecosystem health. A reverse auction was used to encourage homeowners to mitigate stormwater on their property within the suburban, 1.8 km(2) Shepherd Creek catchment in Cincinnati, Ohio (USA). In 2007-2008, 165 rain barrels and 81 rain gardens were installed on 30% of the properties in four experimental (treatment) subcatchments, and two additional subcatchments were maintained as controls. At the base of the subcatchments, we sampled monthly baseflow water quality, and seasonal (5×/year) physical habitat, periphyton assemblages, and macroinvertebrate assemblages in the streams for the three years before and after treatment implementation. Given the minor reductions in directly connected impervious area from the rain barrel installations (11.6% to 10.4% in the most impaired subcatchment) and high total impervious levels (13.1% to 19.9% in experimental subcatchments), we expected minor or no responses of water quality and biota to stormwater management. There were trends of increased conductivity, iron, and sulfate for control sites, but no such contemporaneous trends for experimental sites. The minor effects of treatment on streamflow volume and water quality did not translate into changes in biotic health, and the few periphyton and macroinvertebrate responses could be explained by factors not associated with the treatment (e.g., vegetation clearing, drought conditions). Improvement of overall stream health is unlikely without additional treatment of major impervious surfaces (including roads, apartment buildings, and parking lots). Further research is needed to define the minimum effect threshold and restoration trajectories for retrofitting catchments to improve the health of stream ecosystems.

Direct gas injection method: a simple modification to an elemental analyzer/isotope ratio mass spectrometer for stable isotope analysis of N and C from N2O and CO2 gases in nanomolar concentrations.

RATIONALE: Stable isotope analyses of trace amounts of nitrous oxide gas require special instrumentation and laborious sample preparation methods that have hindered many laboratories from measuring this potent greenhouse gas. A simple modification to an Elemental Analyzer (EA) coupled to an Isotope Ratio Mass Spectrometry (IRMS) setup that allows users to measure the N and C isotopic ratios of nitrous oxide (N(2)O) and carbon dioxide (CO(2)) by injecting the gases directly into the EA is described. METHODS: The standard EA was fitted with a gas injection port and a home-made packed column filled with Hayesep Q polymer. A gas mixture of 3.1% N(2)O in helium (He) was injected directly into the EA. This method allowed large volumes of sample to be injected without saturating the column. RESULTS: The use of the home-made column resulted in better resolution of sample peaks and allowed smaller concentrations of the analyte to be injected. This study showed that this method produced accurate and reproducible stable isotope measurements with sample injection volumes ranging from 100 to 5000 µL, containing between 20 and 1000 nmol of analyte. CONCLUSIONS: This simple, inexpensive method can be useful for the laboratories that do not have access to more advanced and expensive interfaces to analyze nanomolar quantities of N(2)O and CO(2) from microbiological and ecological studies and offers a simple alternative for in-house measurements of these trace gases.

Floodplain restoration enhances denitrification and reach-scale nitrogen removal in an agricultural stream.

Streams of the agricultural Midwest, USA, export large quantities of nitrogen, which impairs downstream water quality, most notably in the Gulf of Mexico. The two-stage ditch is a novel restoration practice, in which floodplains are constructed alongside channelized ditches. During high flows, water flows across the floodplains, increasing benthic surface area and stream water residence time, as well as the potential for nitrogen removal via denitrification. To determine two-stage ditch nitrogen removal efficacy, we measured denitrification rates in the channel and on the floodplains of a two-stage ditch in north-central Indiana for one year before and two years after restoration. We found that instream rates were similar before and after the restoration, and they were influenced by surface water NO3- concentration and sediment organic matter content. Denitrification rates were lower on the constructed floodplains and were predicted by soil exchangeable NO3- concentration. Using storm flow simulations, we found that two-stage ditch restoration contributed significantly to NO3- removal during storm events, but because of the high NO3- loads at our study site, < 10% of the NO3- load was removed under all storm flow scenarios. The highest percentage of NO3- removal occurred at the lowest loads; therefore, the two-stage ditch's effectiveness at reducing downstream N loading will be maximized when the practice is coupled with efforts to reduce N inputs from adjacent fields.

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.

Stream denitrification across biomes and its response to anthropogenic nitrate loading.

Anthropogenic addition of bioavailable nitrogen to the biosphere is increasing and terrestrial ecosystems are becoming increasingly nitrogen-saturated, causing more bioavailable nitrogen to enter groundwater and surface waters. Large-scale nitrogen budgets show that an average of about 20-25 per cent of the nitrogen added to the biosphere is exported from rivers to the ocean or inland basins, indicating that substantial sinks for nitrogen must exist in the landscape. Streams and rivers may themselves be important sinks for bioavailable nitrogen owing to their hydrological connections with terrestrial systems, high rates of biological activity, and streambed sediment environments that favour microbial denitrification. Here we present data from nitrogen stable isotope tracer experiments across 72 streams and 8 regions representing several biomes. We show that total biotic uptake and denitrification of nitrate increase with stream nitrate concentration, but that the efficiency of biotic uptake and denitrification declines as concentration increases, reducing the proportion of in-stream nitrate that is removed from transport. Our data suggest that the total uptake of nitrate is related to ecosystem photosynthesis and that denitrification is related to ecosystem respiration. In addition, we use a stream network model to demonstrate that excess nitrate in streams elicits a disproportionate increase in the fraction of nitrate that is exported to receiving waters and reduces the relative role of small versus large streams as nitrate sinks.