International audienceExisting descriptions of bi-directional ammonia (NH3) land-atmosphere exchange incorporate temperature and moisture controls, and are beginning to be used in regional chemical transport models. However, such models have typically applied simpler emission factors to upscale the main NH3 emission terms. While this approach has successfully simulated the main spatial patterns on local to global scales, it fails to address the environment- and climate-dependence of emissions. To handle these issues, we outline the basis for a new modelling paradigm where both NH3 emissions and deposition are calculated online according to diurnal, seasonal and spatial differences in meteorology. We show how measurements reveal a strong, but complex pattern of climatic dependence, which is increasingly being characterized using ground-based NH3 monitoring and satellite observations, while advances in process-based modelling are illustrated for agricultural and natural sources, including a global application for seabird colonies. A future architecture for NH3 emission-deposition modelling is proposed that integrates the spatio-temporal interactions, and provides the necessary foundation to assess the consequences of climate change. Based on available measurements, a first empirical estimate suggests that 5°C warming would increase emissions by 42 per cent (28-67%). Together with increased anthropogenic activity, global NH3 emissions may increase from 65 (45-85) Tg N in 2008 to reach 132 (89-179) Tg by 2100

Atmospheric Environment, 55. 319-327. 10.1016Environment, 55. 319-327. 10. /j.atmosenv.2012 Contact CEH NORA team at noraceh@ceh.ac.ukThe NERC and CEH trademarks and logos ('the Trademarks') are registered trademarks of NERC in the UK and other countries, and may not be used without the prior written consent of the Trademark owner. AbstractSeabird colonies represent a significant source of atmospheric ammonia (NH 3 ) in remote maritime systems, producing a source of nitrogen that may encourage plant growth, alter terrestrial plant community composition and affect the surrounding marine ecosystem. To investigate seabird NH 3 emissions on a global scale, we developed a contemporary seabird database including a total seabird population of 261 million breeding pairs. We used this in conjunction with a bioenergetics model to estimate the mass of nitrogen excreted by all seabirds at each breeding colony. The results combined with the findings of mid-latitude field studies of volatilization rates estimate the global distribution of NH 3 emissions from seabird colonies on an annual basis. The largest uncertainty in our emission estimate concerns the potential temperature dependence of NH 3 emission. To investigate this we calculated and compared temperature independent emission estimates with a maximum feasible temperature dependent emission, based on the thermodynamic dissociation and solubility equilibria. Using the temperature independent approach, we estimate global NH 3 emissions from seabird colonies at 404 Gg NH 3 per year. By comparison, since most seabirds are located in relatively cold circumpolar locations, the thermodynamically dependent estimate is 136 Gg NH 3 per year. Actual global emissions are expected to be within these bounds, as other factors, such as non-linear interactions with water availability and surface infiltration, moderate the theoretical temperature response. Combining sources of error from temperature (± 49 %), seabird population estimates (± 36 %), variation in diet composition (± 23 %) and nonbreeder attendance (± 13 %), gives a mid estimate with an overall uncertainty range of NH 3 emission from seabird colonies of 270 [97 to 442] Gg NH 3 per year. These emissions are environmentally relevant as they primarily occur as "hot-spots" in otherwise pristine environments with low anthropogenic emissions.2

Abstract. Nitrogen applied to the surface of the land for agricultural purposes represents a significant source of reactive nitrogen (Nr) that can be emitted as a gaseous Nr species, be denitrified to atmospheric nitrogen (N2), run off during rain events or form plant-useable nitrogen in the soil. To investigate the magnitude, temporal variability and spatial heterogeneity of nitrogen pathways on a global scale from sources of animal manure and synthetic fertilizer, we developed a mechanistic parameterization of these pathways within a global terrestrial land model, the Community Land Model (CLM). In this first model version the parameterization emphasizes an explicit climate-dependent approach while using highly simplified representations of agricultural practices, including manure management and fertilizer application. The climate-dependent approach explicitly simulates the relationship between meteorological variables and biogeochemical processes to calculate the volatilization of ammonia (NH3), nitrification and runoff of Nr following manure or synthetic fertilizer application. For the year 2000, approximately 125 Tg N yr−1 is applied as manure and 62 Tg N yr−1 is applied as synthetic fertilizer. We estimate the resulting global NH3 emissions are 21 Tg N yr−1 from manure (17 % of manure production) and 12 Tg N yr−1 from fertilizer (19 % of fertilizer application); reactive nitrogen runoff during rain events is calculated as 11 Tg N yr−1 from manure and 5 Tg N yr−1 from fertilizer. The remaining nitrogen from manure (93 Tg N yr−1) and synthetic fertilizer (45 Tg N yr−1) is captured by the canopy or transferred to the soil nitrogen pools. The parameterization was implemented in the CLM from 1850 to 2000 using a transient simulation which predicted that, even though absolute values of all nitrogen pathways are increasing with increased manure and synthetic fertilizer application, partitioning of nitrogen to NH3 emissions from manure is increasing on a percentage basis, from 14 % of nitrogen applied in 1850 (3 Tg NH3 yr−1) to 17 % of nitrogen applied in 2000 (21 Tg NH3 yr−1). Under current manure and synthetic fertilizer application rates we find a global sensitivity of an additional 1 Tg NH3 (approximately 3 % of manure and fertilizer) emitted per year per °C of warming. While the model confirms earlier estimates of nitrogen fluxes made in a range of studies, its key purpose is to provide a theoretical framework that can be employed within a biogeochemical model, that can explicitly respond to climate and that can evolve and improve with further observation.

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Abstract. Nitrogen applied to the surface of the land for agricultural purposes represents a significant source of reactive nitrogen (Nr) that can be emitted as a gaseous Nr species, be denitrified to atmospheric nitrogen (N2), run-off during rain events or form plant useable nitrogen in the soil. To investigate the magnitude, temporal variability and spatial heterogeneity of nitrogen pathways on a global scale from sources of animal manure and synthetic fertilizer, we developed a mechanistic parameterization of these pathways within a global terrestrial model. The parameterization uses a climate dependent approach whereby the relationships between meteorological variables and biogeochemical processes are used to calculate the volatilization of ammonia (NH3), nitrification and run-off of Nr following manure or fertilizer application. For the year 2000, we estimate global NH3 emission and Nr dissolved during rain events from manure at 21 and 11 Tg N yr−1, respectively; for synthetic fertilizer we estimate the NH3 emission and Nr run-off during rain events at 12 and 5 Tg N yr−1, respectively. The parameterization was implemented in the Community Land Model from 1850 to 2000 using a transient simulation which predicted that, even though absolute values of all nitrogen pathways are increasing with increased manure and synthetic fertilizer application, partitioning of nitrogen to NH3 emissions from manure is increasing on a percentage basis, from 14 % of nitrogen applied (3 Tg NH3 yr−1) in 1850 to 18 % of nitrogen applied in 2000 (22 Tg NH3 yr−1). While the model confirms earlier estimates of nitrogen fluxes made in a range of studies, its key purpose is to provide a theoretical framework that can be employed within a biogeochemical model, that can explicitly respond to climate and that can evolve and improve with further observation.

Abstract. Since 1850 the concentration of atmospheric methane (CH4), a potent greenhouse gas, has more than doubled. Recent studies suggest that emission inventories may be missing sources and underestimating emissions. To investigate whether offshore oil and gas platforms leak CH4 during normal operation, we measured CH4 mole fractions around eight oil and gas production platforms in the North Sea which were neither flaring gas nor offloading oil. We use the measurements from summer 2017, along with meteorological data, in a Gaussian plume model to estimate CH4 emissions from each platform. We find CH4 mole fractions of between 11 and 370 ppb above background concentrations downwind of the platforms measured, corresponding to a median CH4 emission of 6.8 g CH4 s−1 for each platform, with a range of 2.9 to 22.3 g CH4 s−1. When matched to production records, during our measurements individual platforms lost between 0.04 % and 1.4 % of gas produced with a median loss of 0.23 %. When the measured platforms are considered collectively (i.e. the sum of platforms' emission fluxes weighted by the sum of the platforms' production), we estimate the CH4 loss to be 0.19 % of gas production. These estimates are substantially higher than the emissions most recently reported to the National Atmospheric Emission Inventory (NAEI) for total CH4 loss from United Kingdom platforms in the North Sea. The NAEI reports CH4 losses from the offshore oil and gas platforms we measured to be 0.13 % of gas production, with most of their emissions coming from gas flaring and offshore oil loading, neither of which was taking place at the time of our measurements. All oil and gas platforms we observed were found to leak CH4 during normal operation, and much of this leakage has not been included in UK emission inventories. Further research is required to accurately determine total CH4 leakage from all offshore oil and gas operations and to properly include the leakage in national and international emission inventories.

River nitrogen export is simulated within the Community Earth System Model (CESM) by coupling nitrogen leaching and runoff fluxes from the Community Land Model (CLM) to the River Transport Model (RTM). The coupled CLM-RTM prognostically simulates the downstream impact of human N cycle perturbation on coastal areas. It also provides a framework for estimating denitrification fluxes of N 2 and associated trace gases like N 2 O in soils and river sediments. An important limitation of the current model is that it only simulates dissolved inorganic nitrogen (DIN) river export, due to the lack of dissolved organic nitrogen (DON) and particulate nitrogen (PN) leaching fluxes in CLM. In addition, the partitioning of soil N loss in CLM between the primary loss pathways of denitrification and N leaching/runoff appears heavily skewed toward denitrification compared to other literature estimates, especially in nonagricultural regions, and also varies considerably among the four model configurations presented here. River N export is generally well predicted in the model configurations that include midlatitude crops, but tends to be underpredicted in rivers that are less perturbed by human agriculture. This is especially true in the tropics, where CLM likely underestimates leaching and runoff of all forms of nitrogen. River export of DIN is overpredicted in some relatively unperturbed Arctic rivers, which may result from excessive N inputs to those regions in CLM. Better representation of N loss in CLM can improve confidence in model results with respect to the core model objective of simulating nitrogen limitation of the carbon cycle.

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