Anthony J. Dore

Towards a climate-dependent paradigm of ammonia emission and deposition

Existing 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.

Agricultural ammonia emissions inventory and spatial distribution in the North China Plain.

An agricultural ammonia (NH(3)) emission inventory in the North China Plain (NCP) on a prefecture level for the year 2004, and a 5 x 5 km(2) resolution spatial distribution map, has been calculated for the first time. The census database from Chinas statistics datasets, and emission factors re-calculated by the RAINS model supported total emissions of 3071 kt NH(3)-N yr(-1) for the NCP, accounting for 27% of the total emissions in China. NH(3) emission from mineral fertilizer application contributed 1620 kt NH(3)-N yr(-1), 54% of the total emission, while livestock emissions accounted for the remaining 46% of the total emissions, including 7%, 27%, 7% and 5% from cattle, pigs, sheep and goats, and poultry, respectively. A high-resolution spatial NH(3) emissions map was developed based on 1 x 1 km land use database and aggregated to a 5 x 5 km grid resolution. The highest emission density value was 198 kg N ha(-1) yr(-1).

An improved wet deposition map of the United Kingdom incorporating the Seeder-Feeder effect over mountainous terrain

Data of the mean annual rainfall at 4000 sites across the United Kingdom during the period 1986–1988 have been used. These were combined with measurements of the concentrations of principal ions in rainfall at 59 rural lowland sites. The data have been modified to account for the higher concentrations of ions dissolved in rain water measured in mountainous areas. This occurs due to the scavenging of polluted hill caps clouds by less-polluted raindrops. It was assumd that scavenged cloudwater concentrations were double those of the local rainfall. The results show that the annual deposition by rainfall of pollutant ions over high ground is much higher than had previously been thought. Relative to the original scheme, which assumed ion concentrations were constant with height, the new scheme calculated increases in deposition of up to 76%. Rainfall was found to be more polluted near the east coast of Britain. However, the highest annual pollutant deposition by rainfall occurred in the mountainous regions near the west coast, such as the Lake District and Snowdonia, due to the high rainfall in these areas.

Modelling the spatial distribution of ammonia emissions in the UK

Ammonia emissions (NH3) are characterised by a high spatial variability at a local scale. When modelling the spatial distribution of NH3 emissions, it is important to provide robust emission estimates, since the model output is used to assess potential environmental impacts, e.g. exceedance of critical loads. The aim of this study was to provide a new, updated spatial NH3 emission inventory for the UK for the year 2000, based on an improved modelling approach and the use of updated input datasets. The AENEID model distributes NH3 emissions from a range of agricultural activities, such as grazing and housing of livestock, storage and spreading of manures, and fertilizer application, at a 1-km grid resolution over the most suitable landcover types. The results of the emission calculation for the year 2000 are analysed and the methodology is compared with a previous spatial emission inventory for 1996.

A Spatial Analysis of Atmospheric Ammonia and Ammonium in the U.K.

As measures are implemented internationally to reduce SO2 and NOx emissions, attention is falling on the contribution of NH3 emissions to acidification, nitrogen eutrophication, and aerosol formation. In the U.K., a monitoring network has been established to measure the spatial distribution and long-term trends in atmospheric gaseous NH3 and aerosol NH4. At the same time, an atmospheric chemistry and transport model, FRAME, has been developed with a focus on reduced nitrogen (NHx). The monitoring data are important to evaluate the model, while the model is essential for a more detailed spatial assessment. The national network is established with over 80 sampling locations. Measurements of NH3 and NH4 (at up to 50 sites) have been made using a new low-cost denuder-filterpack system. Additionally, improved passive sampling methods for NH3 have been applied to explore local variability. The measurements confirm the high spatial variability of NH3 (annual means 0.06 to 11 mg NH3 m), consistent with its nature as a primary pollutant emitted from ground-level sources, while NH4, being a slowly formed secondary product, shows much less spatial variability (0.14 to 2.4 mg NH4 m). These features are reproduced in the FRAME model, which provides estimates at a 5-km level. Analysis of the underlying NH3 emission inventory shows that sheep emissions may have been underestimated and nonagricultural sources overestimated relative to emissions from cattle. The combination of model and measurements is applied to estimate spatial patterns of dry deposition to different vegetation types. The combined approach provides the basis to assess NHx responses across the U.K. to international emission controls.

Orographic enhancement of snowfall.

Field studies have been conducted at a hill site in Scotland to measure the variation with altitude of wet deposition by snowfall. The results showed that, due to wind drift effects, snowflakes were captured very inefficiently by snow collectors. It was therefore not possible to measure an increase in precipitation with altitude. The average concentrations of principal ions dissolved in the snow water were calculated over a two-month period. The results showed that the concentrations increased by factors of between 1.4 and 1.9 with an altitude rise of 400 m. A model of the orographic enhancement of snowfall by the seeder-feeder effect showed that the orographic enhancements of precipitation and pollutant deposition were significantly greater for snowfall than for rainfall. The wind drift of snow crystals and the evaporation of precipitation in dry valley air were important in determining the patterns of deposition.

Modelling future impacts of air pollution using the multi-scale UK Integrated Assessment Model (UKIAM).

Integrated assessment modelling has evolved to support policy development in relation to air pollutants and greenhouse gases by providing integrated simulation tools able to produce quick and realistic representations of emission scenarios and their environmental impacts without the need to re-run complex atmospheric dispersion models. The UK Integrated Assessment Model (UKIAM) has been developed to investigate strategies for reducing UK emissions by bringing together information on projected UK emissions of SO2, NOx, NH3, PM10 and PM2.5, atmospheric dispersion, criteria for protection of ecosystems, urban air quality and human health, and data on potential abatement measures to reduce emissions, which may subsequently be linked to associated analyses of costs and benefits. We describe the multi-scale model structure ranging from continental to roadside, UK emission sources, atmospheric dispersion of emissions, implementation of abatement measures, integration with European-scale modelling, and environmental impacts. The model generates outputs from a national perspective which are used to evaluate alternative strategies in relation to emissions, deposition patterns, air quality metrics and ecosystem critical load exceedance. We present a selection of scenarios in relation to the 2020 Business-As-Usual projections and identify potential further reductions beyond those currently being planned.

The UK Integrated Assessment Model, UKIAM: A National Scale Approach to the Analysis of Strategies for Abatement of Atmospheric Pollutants Under the Convention on Long-Range Transboundary Air Pollution

Integrated assessment modelling aims to bring together information on emissions, atmospheric transport between sources and exposed areas or populations, criteria for environmental protection, and potential emission control measures and their costs, in order to explore effective abatement strategies. We describe the development of a new UK scale Integrated Assessment Model which can be used to investigate strategies for the attainment of national emission ceilings. The model optimises abatement strategies in relation to acidification, eutrophication, and/or human-exposure to particulate PM10, with reference to the deposition of sulphur and nitrogen (oxidised and reduced), and concentrations of primary and secondary particles. The model combines sector specific emissions, atmospheric transport and deposition, ecosystem specific critical load exceedances, and pollution abatement costs to determine optimised abatement strategies using benefit and, where applicable, recovery functions.

The importance of source configuration in quantifying footprints of regional atmospheric sulphur deposition

An atmospheric transport-chemistry model is applied to investigate the effects of source configuration in simulating regional sulphur deposition footprints from elevated point sources. Dry and wet depositions of sulphur are calculated for each of the 69 largest point sources in the UK. Deposition contributions for each point source are calculated for 2003, as well as for a 2010 emissions scenario. The 2010 emissions scenario has been chosen to simulate the Gothenburg protocol emission scenario. Point source location is found to be a major driver of the dry/wet deposition ratio for each deposition footprint, with increased precipitation scavenging of SO(x) in hill areas resulting in a larger fraction of the emitted sulphur being deposited within the UK for sources located near these areas. This reduces exported transboundary pollution, but, associated with the occurrence of sensitive soils in hill areas, increases the domestic threat of soil acidification. The simulation of plume rise using individual stack parameters for each point source demonstrates a high sensitivity of SO(2) surface concentration to effective source height. This emphasises the importance of using site-specific information for each major stack, which is rarely included in regional atmospheric pollution models, due to the difficulty in obtaining the required input data. The simulations quantify how the fraction of emitted SO(x) exported from the UK increases with source magnitude, effective source height and easterly location. The modelled reduction in SO(x) emissions, between 2003 and 2010 resulted in a smaller fraction being exported, with the result that the reductions in SO(x) deposition to the UK are less than proportionate to the emission reduction. This non-linearity is associated with a relatively larger fraction of the SO(2) being converted to sulphate aerosol for the 2010 scenario, in the presence of ammonia. The effect results in less-than-proportional UK benefits of reducing in SO(2) emissions, together with greater-than-proportional benefits in reducing export of UK SO(2) emissions.

The Effect of Emission from Coal Combustion in Nonindustrial Sources on Deposition of Sulfur and Oxidized Nitrogen in Poland

Abstract Poland has one of the largest sulfur and nitrogen emissions in Europe. This is mainly because coal is a main fuel in industrial and nonindustrial combustion. The aim of this paper is to assess the amount of sulfur and nitrogen deposited from SNAP sector 02 (nonindustrial sources) coal combustion. To assess this issue, the Fine Resolution Atmospheric Multipollutant Exchange (FRAME) model was used. The results suggest that industrial combustion has the largest impact on deposition of oxidized sulfur, whereas the oxidized nitrogen national deposition budget is dominated by transboundary transport. The total mass of pollutants deposited in Poland, originating from nonindustrial coal combustion, is 45 Gg of sulfur and 2.5 Gg of nitrogen, which is over 18% of oxidized sulfur and nearly 2% of oxidized nitrogen deposited. SNAP 02 is responsible for up to 80% of dry-deposited sulfur and 11% of nitrogen. The contribution to wet deposition is largest in central Poland in the case of sulfur and in some areas can exceed 11%. For oxidized nitrogen, nonindustrial emissions contribute less than 1% over the whole area of Poland. The switch from coal to gas fuel in this sector will result in benefits in sulfur and nitrogen deposition reduction.