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Indirect nitrous oxide (N2O) emissions from rivers are currently derived using poorly constrained default IPCC emission factors (EF5r) which yield unreliable flux estimates. Here, we demonstrate how hydrogeological conditions can be used to develop more refined regional-scale EF5r estimates required for compiling accurate national greenhouse gas inventories. Focusing on three UK river catchments with contrasting bedrock and superficial geologies, N2O and nitrate (NO3-) concentrations were analyzed in 651 river water samples collected from 2011 to 2013. Unconfined Cretaceous Chalk bedrock regions yielded the highest median N2O-N concentration (3.0 μg L-1), EF5r (0.00036) and N2O-N flux (10.8 kg ha-1 a-1). Conversely, regions of bedrock confined by glacial deposits yielded significantly lower median N2O-N concentration (0.8 μg L-1), EF5r (0.00016) and N2O-N flux (2.6 kg ha-1 a-1), regardless of bedrock type. Bedrock permeability is an important control in regions where groundwater is unconfined, with a high N2O yield from high permeability Chalk contrasting with significantly lower median N2O-N concentration (0.7 μg L-1), EF5r (0.00020) and N2O-N flux (2.0 kg ha-1 a-1) on lower permeability unconfined Jurassic mudstone. The evidence presented here demonstrates EF5r can be differentiated by hydrogeological conditions and thus provide a valuable proxy for generating improved regional-scale N2O emission estimates.

Indirect nitrous oxide (N2O) emissions produced by nitrogen (N) leaching into surface water and groundwater bodies are poorly understood in comparison to direct N2O emissions from soils. In this study, dissolved N2O concentrations were measured weekly in both lowland headwater streams and subsurface agricultural field drain discharges over a two-year period (2013–2015) in an intensive arable catchment, Norfolk, UK. All field drain and stream water samples were found to have dissolved N2O concentrations higher than the water–air equilibrium concentration, illustrating that all sites were acting as a net source of N2O emissions to the atmosphere. Soil texture was found to significantly influence field drain N2O dynamics, with mean concentrations from drains in clay loam soils (5.3 µg N L-1) being greater than drains in sandy loam soils (4.0 µg N L-1). Soil texture also impacted upon the relationships between field drain N2O concentrations and other water quality parameters (pH, flow rate, and nitrate (NO3) and nitrite (NO2) concentrations), highlighting possible differences in N2O production mechanisms in different soil types. Catchment antecedent moisture conditions influenced the storm event mobilisation of N2O in both field drains and streams, with the greatest concentration increases recorded during precipitation events preceded by prolonged wet conditions. N2O concentrations also varied seasonally, with the lowest mean concentrations typically occurring during the summer months (JJA). Nitrogen fertiliser application rates and different soil inversion regimes were found to have no effect on dissolved N2O concentrations, whereas higher N2O concentrations recorded in field drains under a winter cover crop compared to fallow fields revealed cover crops are an ineffective greenhouse gas emission mitigation strategy. Overall, this study highlights the complex interactions governing the dynamics of dissolved N2O concentrations in field drains and headwater streams in a lowland intensive agricultural catchment.

We hypothesise that climate change, together with intensive agricultural systems, will increase the transfer of pollutants from land to water and impact on stream health. This study builds, for the first time, an integrated assessment of nutrient transfers, bringing together a) high-frequency data from the outlets of two surface water-dominated, headwater (~ 10 km²) agricultural catchments, b) event-by-event analysis of nutrient transfers, c) concentration duration curves for comparison with EU Water Framework Directive water quality targets, d) event analysis of location-specific, sub-daily rainfall projections (UKCP, 2009), and e) a linear model relating storm rainfall to phosphorus load. These components, in combination, bring innovation and new insight into the estimation of future phosphorus transfers, which was not available from individual components. The data demonstrated two features of particular concern for climate change impacts. Firstly, the bulk of the suspended sediment and total phosphorus (TP) load (greater than 90% and 80% respectively) was transferred during the highest discharge events. The linear model of rainfall-driven TP transfers estimated that, with the projected increase in winter rainfall (+ 8% to + 17% in the catchments by 2050s), annual event loads might increase by around 9% on average, if agricultural practices remain unchanged. Secondly, events following dry periods of several weeks, particularly in summer, were responsible for high concentrations of phosphorus, but relatively low loads. The high concentrations, associated with low flow, could become more frequent or last longer in the future, with a corresponding increase in the length of time that threshold concentrations (e.g. for water quality status) are exceeded. The results suggest that in order to build resilience in stream health and help mitigate potential increases in diffuse agricultural water pollution due to climate change, land management practices should target controllable risk factors, such as soil nutrient status, soil condition and crop cover.