The changing nitrogen landscape of United States streams: Declining deposition and increasing organic nitrogen.

Air quality regulations have led to decreased nitrogen (N) and sulfur deposition across the conterminous United States (CONUS) during the last several decades, particularly in the eastern parts. But it is unclear if declining deposition has altered stream N at large scales. We compared watershed N inputs with N chemistry from over 2,000 CONUS streams where deposition was the largest N input to the watershed. Weighted change analysis showed that deposition declined across most watersheds, especially in the Eastern CONUS. Nationally, declining N deposition was not associated with significant large-scale declines in stream nitrate concentration. Instead, significant increases in stream dissolved organic carbon (DOC) and total organic N (TON) were widespread across regions. Possible mechanisms behind these increases include declines in acidity and/or ionic strength drivers, changes in carbon availability, and/or climate variables. Our results also reveal a declining trend of DOC/TON ratio over the entire study period, primarily influenced by the trend in the Eastern region, suggesting the rate of increase in stream TON exceeded the rate of increase in DOC concentration during this period. Our results illustrate the complexity of nutrient cycling that links long-term atmospheric deposition to water quality. More research is needed to understand how increased dissolved organic N could affect aquatic ecosystems and downstream riverine nutrient export.

Our national nutrient reduction needs: Applying a conservation prioritization framework to US agricultural lands.

Targeted conservation approaches seek to focus resources on areas where they can deliver the greatest benefits and are recognized as key to reducing nonpoint source nutrients from agricultural landscapes into sensitive receiving waters. Moreover, there is growing recognition of the importance and complementarity of in-field and edge-of-field conservation for reaching nutrient reduction goals. Here we provide a generic prioritization that can help with spatial targeting and applied it across the conterminous US (CONUS). The prioritization begins with identifying areas with high agricultural nutrient surplus, i.e., where the most nitrogen (N) and/or phosphorus (P) inputs are left on the landscape after crop harvest. Subwatersheds with high surplus included 52% and 50% of CONUS subwatersheds for N and P, respectively, and were located predominantly in the Midwest for N, in the South for P, and in California for both N and P. Then we identified the most suitable conservation strategies using a hierarchy of metrics including nutrient use efficiency (proportion of new nutrient inputs removed by crop harvest), tile drainage, existing buffers for agricultural run-off, and wetland restoration potential. In-field nutrient input reduction emerged as a priority because nutrient use efficiency fell below a high but achievable goal of 0.7 (30% of nutrients applied are not utilized) in 45% and 44% of CONUS subwatersheds for N and P, respectively. In many parts of the southern and western US, in-field conservation (i.e., reducing inputs + preventing nutrients from leaving fields) alone was likely the optimal strategy as agriculture was already well-buffered. However, stacking in-field conservation with additional edge-of-field buffering would be important to conservation strategies in 35% and 29% of CONUS subwatersheds for N and P, respectively. Nutrient use efficiencies were often high enough in the Midwest that proposed strategies focused more on preventing nutrients from leaving fields, managing tile effluent, and buffering agricultural fields. Almost all major river basins would benefit from a variety of nutrient reduction conservation strategies, underscoring the potential of targeted approaches to help limit excess nutrients in surface and ground waters.

Wetland Flowpaths Mediate Nitrogen and Phosphorus Concentrations across the Upper Mississippi River Basin.

Eutrophication, harmful algal blooms, and human health impacts are critical environmental challenges resulting from excess nitrogen and phosphorus in surface waters. Yet we have limited information regarding how wetland characteristics mediate water quality across watershed scales. We developed a large, novel set of spatial variables characterizing hydrological flowpaths from wetlands to streams, that is, "wetland hydrological transport variables," to explore how wetlands statistically explain the variability in total nitrogen (TN) and total phosphorus (TP) concentrations across the Upper Mississippi River Basin (UMRB) in the United States. We found that wetland flowpath variables improved landscape-to-aquatic nutrient multilinear regression models (from R2 = 0.89 to 0.91 for TN; R2 = 0.53 to 0.84 for TP) and provided insights into potential processes governing how wetlands influence watershed-scale TN and TP concentrations. Specifically, flowpath variables describing flow-attenuating environments, for example, subsurface transport compared to overland flowpaths, were related to lower TN and TP concentrations. Frequent hydrological connections from wetlands to streams were also linked to low TP concentrations, which likely suggests a nutrient source limitation in some areas of the UMRB. Consideration of wetland flowpaths could inform management and conservation activities designed to reduce nutrient export to downstream waters.

National hydrologic connectivity classification links wetlands with stream water quality.

Wetland hydrologic connections to downstream waters influence stream water quality. However, no systematic approach for characterizing this connectivity exists. Here using physical principles, we categorized conterminous US freshwater wetlands into four hydrologic connectivity classes based on stream contact and flowpath depth to the nearest stream: riparian, non-riparian shallow, non-riparian mid-depth and non-riparian deep. These classes were heterogeneously distributed over the conterminous United States; for example, riparian dominated the south-eastern and Gulf coasts, while non-riparian deep dominated the Upper Midwest and High Plains. Analysis of a national stream dataset indicated acidification and organic matter brownification increased with connectivity. Eutrophication and sedimentation decreased with wetland area but did not respond to connectivity. This classification advances our mechanistic understanding of wetland influences on water quality nationally and could be applied globally.

Shifts in the composition of nitrogen deposition in the conterminous United States are discernable in stream chemistry.

Across the conterminous United States (U.S.), the composition of atmospheric nitrogen (N) deposition is changing spatially and temporally. Previously, deposition was dominated by oxidized N, but now reduced N (ammonia [NH3] + ammonium [NH4+]) is equivalent to oxidized N when deposition is averaged across the entire nation and, in some areas, reduced N dominates deposition. To evaluate if there are effects of this change on stream chemistry at the national scale, estimates of N deposition form (oxidized or reduced) from the National Atmospheric Deposition Program Total Deposition data were coupled with stream measurements from the U.S. Environmental Protection Agency (EPA) National Rivers and Streams Assessments (three stream surveys between 2000 and 2014). A recent fine-scaled N input inventory was used to identify watersheds (<1000 km2) where atmospheric deposition is the largest N source (n = 1906). Within these more atmospherically-influenced watersheds there was a clear temporal shift from a greater proportion of sites dominated by oxidized N deposition to a greater proportion of sites dominated by reduced forms of N deposition. We found a significant positive correlation between oxidized N deposition and stream NO3- concentrations, whereas the correlation between reduced N deposition and stream NO3- concentrations were significant but weaker. Sites dominated by atmospheric inputs of reduced N forms had higher stream total organic N and total N despite lower total N deposition on average. This higher stream concentration of total N is mainly driven by the higher concentration of total organic N, suggesting an interaction between elevated reduced N in deposition and living components of the ecosystem or soil organic matter dynamics. Regardless of the proportion of reduced to oxidized N forms in deposition, stream NH4+ concentrations were generally low, suggesting that N deposited in a reduced form is rapidly immobilized, nitrified and/or assimilated by watershed processes.

Identifying lakes at risk of toxic cyanobacterial blooms using satellite imagery and field surveys across the United States.

Harmful algal blooms caused by cyanobacteria are a threat to global water resources and human health. Satellite remote sensing has vastly expanded spatial and temporal data on lake cyanobacteria, yet there is still acute need for tools that identify which waterbodies are at-risk for toxic cyanobacterial blooms. Algal toxins cannot be directly detected through imagery but monitoring toxins associated with cyanobacterial blooms is critical for assessing risk to the environment, animals, and people. The objective of this study is to address this need by developing an approach relating satellite imagery on cyanobacteria with field surveys to model the risk of toxic blooms among lakes. The Medium Resolution Imaging Spectrometer (MERIS) and United States (US) National Lakes Assessments are leveraged to model the probability among lakes of exceeding lower and higher demonstration thresholds for microcystin toxin, cyanobacteria, and chlorophyll a. By leveraging the large spatial variation among lakes using two national-scale data sources, rather than focusing on temporal variability, this approach avoids many of the previous challenges in relating satellite imagery to cyanotoxins. For every satellite-derived lake-level Cyanobacteria Index (CI_cyano) increase of 0.01 CI_cyano/km2, the odds of exceeding six bloom thresholds increased by 23-54 %. When the models were applied to the 2192 satellite monitored lakes in the US, the number of lakes identified with ≥75 % probability of exceeding the thresholds included as many as 335 lakes for the lower thresholds and 70 lakes for the higher thresholds, respectively. For microcystin, the models identified 162 and 70 lakes with ≥75 % probability of exceeding the lower (0.2 µg/L) and higher (1.0 µg/L) thresholds, respectively. This approach represents a critical advancement in using satellite imagery and field data to identify lakes at risk for developing toxic cyanobacteria blooms. Such models can help translate satellite data to aid water quality monitoring and management.

Deep soil nitrogen storage slows nitrate leaching through the vadose zone.

Nitrogen (N) fertilizer applications are important for agricultural yield, yet not all the applied N is taken up by crops, leading to surplus N storage in soil or leaching to groundwater and surface water. Leaching loss of fertilizer N represents a cost for farmers and has consequences for human health and the environment, especially in the southern Willamette Valley, Oregon, USA, where groundwater nitrate contamination is prevalent. While improved nutrient management and conservation practices have been implemented to minimize leaching, nitrate levels in groundwater continue to increase in many long-term monitoring wells. To elucidate controls on leaching rates and N dynamics in agricultural soils across soil depths, and in response to seasonal and annual variation in management (e.g., fertilizer input amount and summer irrigation), we intensively monitored the transport of water and nitrate every two weeks for four years through the vadose zone at three depths (0.8, 1.5, and 3.0 m) in a sweet corn (maize) field. Though nitrate leaching was highly variable among lysimeters at the same depth and across years, a strong pattern emerged: annual nitrate leaching significantly decreased with depth across the study, averaging ~104 kg N ha-1 yr-1 near the surface (0.8 m) versus ~56 kg N ha-1 yr-1 in the deep soil (3.0 m), a 54% reduction in leaching between the soil layers. Even though crops were irrigated in summer, most leaching (~72% below 3.0 m) occurred during the wet fall and winter. Based on steady state assumptions, a net equivalent of ~29% of surface N inputs leached below 3.0 m into the deeper soil and groundwater, while ~44% was removed in crop harvest, indicating considerable N retention in the soil (~27% of inputs or approximately 58 kg N ha-1 yr-1). The accumulation and long-term dynamics of deep soil N is a legacy of agricultural management that should be further studied to better manage and reduce nitrate loss to groundwater.

Wildfires can increase regulated nitrate, arsenic, and disinfection byproduct violations and concentrations in public drinking water supplies.

Wildfires are a concern for water quality in the United States, particularly in the wildland-urban interface of populous areas. Wildfires combust vegetation and surface soil organic matter, reduce plant nutrient uptake, and can alter the composition of runoff and receiving waters. At the wildland-urban interface, fires can also introduce contaminants from the combustion of man-made structures. We examine post-wildfire effects on drinking water quality by evaluating concentrations and maximum contaminant level (MCL) violations of selected contaminants regulated in the U.S. at public drinking water systems (PWSs) located downstream from wildfire events. Among contaminants regulated under the U.S. Safe Drinking Water Act, nitrate, arsenic, disinfection byproducts, and volatile organic compounds (VOCs) were analyzed in watersheds that experienced major wildfires. Surface water sourced drinking water (SWDW) nitrate violations increased by an average of 0.56 violations per PWS and concentrations increased by 0.044 mg-N/L post-wildfire. Groundwater sourced drinking water (GWDW) nitrate violations increased by 0.069 violations per PWS and concentrations increased by 0.12 mg-N/L post-wildfire. SWDW total trihalomethane (TTHM) violations increased by 0.58 violations per PWS and concentrations increased by 10.4 µg/L. SWDW total haloacetic acid (HAA5) violations increased by 0.82 violations per PWS and concentrations increased by 8.5 µg/L. Arsenic violations increased by 1.08 violations per PWS and concentrations increased by 0.92 µg/L. There was no significant effect of wildfires on average VOC violations. Nitrate violations increased in 75% of SWDW sites and 34% of GWDW sites post-wildfire, while about 71% and 50% of SWDW sites showed an increase in TTHM and HAA5 violations. Violations also increased for 35% of arsenic and 44% of VOC sites post-wildfire. These findings support the need for increased awareness about the impact of wildfires on drinking water treatment to help PWS operators adapt to the consequences of wildfires on source water quality, particularly in wildfire-prone regions.

δ15N of Chironomidae: An index of nitrogen sources and processing within watersheds for national aquatic monitoring programs.

Nitrogen (N) removal along flowpaths to aquatic ecosystems is an important regulating ecosystem service that can help reduce N pollution in the nation's waterways, but can be challenging to measure at large spatial scales. Measurements that integrate N processing within watersheds would be particularly useful for assessing the magnitude of this vital service. Because most N removal processes cause isotopic fractionation, δ15N from basal food-chain organisms in aquatic ecosystems can provide information on both N sources and the degree of watershed N processing. As part of EPA's National Aquatic Resource Surveys (NARS), we measured δ15N of Chironomidae collected from over 2000 lakes, rivers and streams across the continental USA. Using information on N inputs to watersheds and summer total N concentrations ([TN]) in the water column, we assessed where elevated chironomid δ15N would indicate N removal rather than possible enriched sources of N. Chironomid δ15N values ranged from -4 to +20‰, and were higher in rivers and streams than in lakes, indicating that N in rivers and streams underwent more processing and cycling that preferentially removes 14N than N in lakes. Chironomid δ15N increased with watershed size, N inputs, and water chemical components, and decreased as precipitation increased. In rivers and streams with high watershed N inputs, we found lower [TN] in streams with higher chironomid δ15N values, suggesting high rates of gaseous N loss such as denitrification. At low watershed N inputs, the pattern reversed; streams with elevated chironomid δ15N had higher [TN] than streams with lower chironomid δ15N, possibly indicating unknown sources elevated in δ15N such as legacy N, or waste from animals or humans. Chironomid δ15N values can be a valuable tool to assess integrated watershed-level N sources, input rates, and processing for water quality monitoring and assessment at large scales.

Context is Everything: Interacting Inputs and Landscape Characteristics Control Stream Nitrogen.

To understand the environmental and anthropogenic drivers of stream nitrogen (N) concentrations across the conterminous US, we combined summer low-flow data from 4997 streams with watershed information across three survey periods (2000-2014) of the US EPA's National Rivers and Streams Assessment. Watershed N inputs explained 51% of the variation in log-transformed stream total N (TN) concentrations. Both N source and input rates influenced stream NO3/TN ratios and N concentrations. Streams dominated by oxidized N forms (NO3/TN ratio > 0.50) were more strongly responsive to the N input rate compared to streams dominated by other N forms. NO3 proportional contribution increased with N inputs, supporting N saturation-enhanced NO3 export to aquatic ecosystems. By combining information about N inputs with climatic and landscape factors, random forest models of stream N concentrations explained 70, 58, and 60% of the spatial variation in stream concentrations of TN, dissolved inorganic N, and total organic N, respectively. The strength and direction of relationships between watershed drivers and stream N concentrations and forms varied with N input intensity. Model results for high N input watersheds not only indicated potential contributions from contaminated groundwater to high stream N concentrations but also the mitigating role of wetlands.

Coupling the dual isotopes of water (δ2H and δ18O) and nitrate (δ15N and δ18O): A new framework for classifying current and legacy groundwater pollution.

Nitrate contamination of groundwater is a concern globally, particularly in agricultural regions where decades of fertilizer nitrogen (N) use has led to a legacy of N accumulation in soils and groundwater. Linkages between current management practices and groundwater nitrate dynamics are often confounded by the legacy effect, and other processes unrelated to management. A coupled analysis of dual stable isotopes of water (δH2O = δ2H and δ18O) and nitrate (δNO3 - = δ15N and δ18O) can be a powerful approach to identify sources and processes responsible for groundwater pollution. To assess how management practices impact groundwater nitrate, we interpreted behavior of δH2O and δNO3 -, together with nitrate concentrations, in water samples collected from long-term monitoring wells in the Southern Willamette Valley (SWV), Oregon. The source(s) of nitrate and water varied among wells, suggesting that the nitrate concentration patterns were not uniform across the shallow aquifer of the valley. Analyzing the stability versus variability of a well's corresponding δH2O and δNO3 - values over time revealed the mechanisms controlling nitrate concentrations. Wells with stable δH2O and δNO3 - values and nitrate concentrations were influenced by one water source with a long residence time and one nitrate source. Variable nitrate concentrations of other wells were attributed to dilution with an alternate water source, mixing of two nitrate sources, or variances in the release of legacy N from overlying soils. Denitrification was not an important process influencing well nitrate dynamics. Understanding the drivers of nitrate dynamics and interaction with legacy N is crucial for managing water quality improvement. This case study illustrates when and where such coupled stable isotope approaches might provide key insights to management on groundwater nitrate contamination issues.

Considerations when using nutrient inventories to prioritize water quality improvement efforts across the US.

Ongoing water quality degradation tied to nitrogen and phosphorus pollution results in significant economic damages by diminishing the recreational value of surface water and compromising fisheries. Progress in decreasing nitrogen and phosphorus pollution to surface water over the past two decades has been slow. Limited resources need to be leveraged efficiently and effectively to prioritize watersheds for restoration. Leveraging recent nitrogen and phosphorus inventories for the years 2002, 2007, and 2012, we extracted relevant flux and demand terms to help identify US subbasins that are likely contributing a disproportionate amount of point and non-point source nutrient pollution to surface water by exploring the mean spatial distribution of terrestrial anthropogenic surplus, agricultural surplus, agricultural nutrient use efficiency, and point source loads. A small proportion of the landscape, <25% of subbasin area of the United States, contains 50% of anthropogenic and agriculture nitrogen and phosphorus surplus while only 2% of landscape contributes >50% of point source loads into surface water. Point source loads are mainly concentrated in urban areas across the country with point source loading rates often exceeding >10.0 kg N ha-1 yr-1 and >1.0 kg P ha-1 yr-1. However, the ability for future upgrades to wastewater treatment plant infrastructure alone is unlikely to drive further improvement in water quality, outside of local water ways, since point source loads only account for ~4% of anthropogenic N and P surplus. As such, further progress in boosting nutrient use efficiency in agricultural production, usually lowest in areas of intensive livestock production, would likely contribute to the biggest gains to water quality restoration goals. This analysis and the corresponding database integrate multiple streams of information to highlight areas where N and P are being managed inefficiently to give decision makers a succinct platform to identify likely areas and sources of water quality degradation.

Phosphorus Inventory for the Conterminous United States (2002-2012).

Published reports suggest efforts designed to prevent the occurrence of harmful algal blooms and hypoxia by reducing non-point and point source phosphorus (P) pollution are not delivering water quality improvements in many areas. Part of the uncertainty in evaluating watershed responses to management practices is the lack of standardized estimates of phosphorus inputs and outputs. To assess P trends across the conterminous United States, we compiled an inventory using publicly available datasets of agricultural P fluxes, atmospheric P deposition, human P demand and waste, and point source discharges for 2002, 2007, and 2012 at the scale of the 8-digit Hydrologic Unit Code subbasin (~1,800 km2). Estimates of agricultural legacy P surplus accumulated from 1945 to 2001 were also developed. Fertilizer and manure inputs were found to exceed crop removal rates by up to 50% in many agricultural regions. This excess in inputs has led to the continued accumulation of legacy P in agricultural lands. Atmospheric P deposition increased throughout the Rockies, potentially contributing to reported increases in surface water P concentrations in undisturbed watersheds. In some urban areas, P fluxes associated with human waste and non-farm fertilizer use has declined despite population growth, likely due, in part, to various sales bans on P-containing detergents and fertilizers. Although regions and individual subbasins have different contemporary and legacy P sources, a standardized method of accounting for large and small fluxes and ready to use inventory numbers provide essential infromation to coordinate targeted interventions to reduce P concentrations in the nation's waters.

Nitrogen futures in the shared socioeconomic pathways 4.

Humanity's transformation of the nitrogen cycle has major consequences for ecosystems, climate and human health, making it one of the key environmental issues of our time. Understanding how trends could evolve over the course of the 21st century is crucial for scientists and decision-makers from local to global scales. Scenario analysis is the primary tool for doing so, and has been applied across all major environmental issues, including nitrogen pollution. However, to date most scenario efforts addressing nitrogen flows have either taken a narrow approach, focusing on a singular impact or sector, or have not been integrated within a broader scenario framework - a missed opportunity given the multiple environmental and socio-economic impacts that nitrogen pollution exacerbates. Capitalizing on our expanding knowledge of nitrogen flows, this study introduces a framework for new nitrogen-focused narratives based on the widely used Shared Socioeconomic Pathways that include all the major nitrogen-polluting sectors (agriculture, industry, transport and wastewater). These new narratives are the first to integrate the influence of climate and other environmental pollution control policies, while also incorporating explicit nitrogen-control measures. The next step is for them to be used as model inputs to evaluate the impact of different nitrogen production, consumption and loss trajectories, and thus advance understanding of how to address environmental impacts while simultaneously meeting key development goals. This effort is an important step in assessing how humanity can return to the planetary boundary of this essential element over the coming century.

Seasonal disconnect between streamflow and retention shapes riverine nitrogen export in the Willamette River Basin, Oregon.

Watershed nutrient balance studies traditionally focus on annual fluxes. In areas with strongly seasonal, Mediterranean-type climate regimes, riverine nutrient export may be greater during wet seasons when hydrologic forcing overwhelms or bypasses retention mechanisms. By combining data on riverine export with spatially detailed nutrient inputs, we examine how nitrogen (N) supply, retention, and streamflow shape annual and seasonal riverine N export in Oregon's Willamette River Basin (WRB). The WRB has pronounced dry summers and wet winters, and the distribution of farmland, cities and forests create significant spatial variations in N inputs. Local data on N inputs were coupled with streamflow and chemistry to calculate fractional N export for 22 WRB sub-watersheds in the mid-2000s. For the entire WRB, 78% of the N inputs came from agricultural activities, mainly as synthetic fertilizer (69%); the next largest inputs were deposition (10%), alder fixation (5%) and point sources (5%). Crop-specific estimates of fertilizer agreed with county fertilizer sales rates at the high end of extension recommendations. Fractional riverine N export (annual riverine N export / net watershed N input) averaged 38% of net inputs in WRB tributaries, greater than other regions of North America. Fall and winter together accounted for 60-90% of the riverine N export across all watersheds. Summer export was small but was greatest in the watersheds that receive seasonal snowmelt. Large wet season losses, when biotic sinks are less active, result in a relatively high proportion of N inputs exported in this region with a Mediterranean climate and high runoff.

Patterns and predictions of drinking water nitrate violations across the conterminous United States.

Excess nitrate in drinking water is a human health concern, especially for young children. Public drinking water systems in violation of the 10 mg nitrate-N/L maximum contaminant level (MCL) must be reported in EPA's Safe Drinking Water Information System (SDWIS). We used SDWIS data with random forest modeling to examine the drivers of nitrate violations across the conterminous U.S. and to predict where public water systems are at risk of exceeding the nitrate MCL. As explanatory variables, we used land cover, nitrogen inputs, soil/hydrogeology, and climate variables. While we looked at the role of nitrate treatment in separate analyses, we did not include treatment as a factor in the final models, due to incomplete information in SDWIS. For groundwater (GW) systems, a classification model correctly classified 79% of catchments in violation and a regression model explained 43% of the variation in nitrate concentrations above the MCL. The most important variables in the GW classification model were % cropland, agricultural drainage, irrigation-to-precipitation ratio, nitrogen surplus, and surplus precipitation. Regions predicted to have risk for nitrate violations in GW were the Central California Valley, parts of Washington, Idaho, the Great Plains, Piedmont of Pennsylvania and Coastal Plains of Delaware, and regions of Wisconsin, Iowa, and Minnesota. For surface water (SW) systems, a classification model correctly classified 90% of catchments and a regression model explained 52% of the variation in nitrate concentration. The variables most important for the SW classification model were largely hydroclimatic variables including surplus precipitation, irrigation-to-precipitation ratio, and % shrubland. Areas at greatest risk for SW nitrate violations were generally in the non-mountainous west and southwest. Identifying the areas with possible risk for future violations and potential drivers of nitrate violations across U.S. can inform decisions on how source water protection and other management options could best protect drinking water.

Where Have All the Nutrients Gone? Long-Term Decoupling of Inputs and Outputs in the Willamette River Watershed, Oregon, United States.

Better documentation and understanding of long-term temporal dynamics of nitrogen (N) and phosphorus (P) in watersheds is necessary to support effective water quality management, in part because studies have identified time lags between terrestrial nutrient balances and water quality. We present annual time series data from 1969 to 2012 for terrestrial N and P sources and monthly data from 1972 to 2013 for river N and P for the Willamette River Basin, Oregon, United States. Inputs to the watershed increased by factors of 3 for N and 1.2 for P. Synthetic fertilizer inputs increased in total and relative importance over time, while sewage inputs decreased. For N, increased fertilizer application was not matched by a proportionate increase in crop harvest; N use efficiency decreased from 69% to 38%. P use efficiency increased from 52% to 67%. As nutrient inputs to terrestrial systems increased, river concentrations and loads of total N, total P, and dissolved inorganic P decreased, and annual nutrient loads were strongly related to discharge. The N:P ratio of both sewage and fertilizer doubled over time but there was no similar trend in riverine export; river N:P concentrations declined dramatically during storms. River nutrient export over time was related to hydrology and waste discharge, with relatively little influence of watershed balances, suggesting that accumulation within soils or groundwater over time is mediating watershed export. Simply managing yearly nutrient balances is unlikely to improve water quality; rather, many factors must be considered, including soil and groundwater storage capacity, and gaseous loss pathways.

The U.S. consumer phosphorus footprint: where do nitrogen and phosphorus diverge?

Phosphorus (P) and nitrogen (N) are essential nutrients for food production but their excess use in agriculture can have major social costs, particularly related to water quality degradation. Nutrient footprint approaches estimate N and P release to the environment through food production and waste management and enable linking these emissions to particular consumption patterns. Following an established method for quantifying a consumer-oriented N footprint for the United States (U.S.), we calculate an analogous P footprint and assess the N:P ratio across different stages of food production and consumption. Circa 2012, the average consumer's P footprint was 4.4 kg P capita-1 yr-1 compared to 22.4 kg N capita-1 yr-1 for the food portion of the N footprint. Animal products have the largest contribution to both footprints, comprising >70% of the average per capita N and P footprints. The N:P ratio of environmental release based on virtual nutrient factors (kilograms N or P per kilogram of food consumed) varies considerably across food groups and stages. The overall N:P ratio of the footprints was lower (5.2 by mass) than for that of U.S. food consumption (8.6), reinforcing our finding that P is managed less efficiently than N in food production systems but more efficiently removed from wastewater. While strategies like reducing meat consumption will effectively reduce both N and P footprints by decreasing overall synthetic fertilizer nutrient demands, consideration of how food production and waste treatment differentially affect N and P releases to the environment can also inform eutrophication management.

Key components and contrasts in the nitrogen budget across a US-Canadian transboundary watershed.

Watershed nitrogen (N) budgets provide insights into drivers and solutions for groundwater and surface water N contamination. We constructed a comprehensive N budget for the transboundary Nooksack River Watershed (British Columbia, Canada and Washington, US) using locally-derived data, national statistics and standard parameters. Feed imports for dairy (mainly in the US) and poultry (mainly in Canada) accounted for 30 and 29% of the total N input to the watershed, respectively. Synthetic fertilizer was the next largest source contributing 21% of inputs. Food imports for humans and pets together accounted for 9% of total inputs, lower than atmospheric deposition (10%). N imported by returning salmon representing marine derived nutrients accounted for <0.06 % of total N input. Quantified N export was 80% of total N input, driven by ammonia emission (32% of exports). Animal product export was the second largest output of N (31%) as milk and cattle in the US and poultry products in Canada. Riverine export of N was estimated at 28% of total N export. The commonly used crop nitrogen use efficiency (NUE) metric alone did not provide sufficient information on farming activities but in combination with other criteria such as farm-gate NUE may better represent management efficiency. Agriculture was the primary driver of N inputs to the environment as a result of its regional importance; the N budget information can inform management to minimize N losses. The N budget provides key information for stakeholders across sectors and borders to create environmentally and economically viable and effective solutions.

Arsenic Drinking Water Violations Decreased across the United States Following Revision of the Maximum Contaminant Level.

Arsenic poses a threat to public health due to widespread environmental prevalence and known carcinogenic effects. In 2001, the US EPA published the Final Arsenic Rule (FAR) for public drinking water, reducing the maximum contaminant level (MCL) from 50 to 10 µg/L. We investigated impacts of the FAR on drinking water violations temporally and geographically using the Safe Drinking Water Information System. Violations exceeding the MCL and the population served by violating systems were analyzed across the conterminous US from 2006 (onset of FAR enforcement) to 2017. The percentage of public water system violations declined from 1.3% in 2008 to 0.55% in 2017 (p < 0.001, slope = -0.070), and the population served decreased by over 1 million (p < 0.001, slope = -106 886). Geographical analysis demonstrated higher mean violations and populations served in certain counties rather than evenly distributed across states. The decline in violations is likely due to the adoption of documented and undocumented treatment methods and possibly from reduced environmental releases. Considering other studies that have shown decreased urinary arsenic levels in the population served by public water systems since the new standard, it may be inferred that the FAR is facilitating the reduction of arsenic exposure in the US.