Ammonia emissions from a grazed field estimated by miniDOAS measurements and inverse dispersion modelling

Ammonia (NH3) fluxes were estimated from a field being grazed by dairy cattle during spring by applying a backward Lagrangian stochastic model (bLS) model combined with horizontal concentration gradients measured across the field. Continuous concentration measurements at field boundaries were made by open-path miniDOAS (differential optical absorption spectroscopy) instruments while the cattle were present and for 6 subsequent days. The deposition of emitted NH3 to "clean" patches on the field was also simulated, allowing both "net" and "gross" emission estimates, where the dry deposition velocity (vd) was predicted by a canopy resistance (Rc) model developed from local NH3 flux and meteorological measurements. Estimated emissions peaked during grazing and decreased after the cattle had left the field, while control on emissions was observed from covariance with temperature, wind speed and humidity and wetness measurements made on the field, revealing a diurnal emission profile. Large concentration differences were observed between downwind receptors, due to spatially heterogeneous emission patterns. This was likely caused by uneven cattle distribution and a low grazing density, where "hotspots" of emissions would arise as the cattle grouped in certain areas, such as around the water trough. The spatial complexity was accounted for by separating the model source area into sub-sections and optimising individual source area coefficients to measured concentrations. The background concentration was the greatest source of uncertainty, and based on a sensitivity/uncertainty analysis the overall uncertainty associated with derived emission factors from this study is at least 30–40 %

Pan-European rural monitoring network shows dominance of NH3 gas and NH4NO3 aerosol in inorganic atmospheric pollution load

A comprehensive European dataset on monthly atmospheric NH3, acid gases (HNO3, SO2, HCl), and aerosols (NH4+, NO3-, SO42-, Cl−, Na+, Ca2+, Mg2+) is presented and analysed. Speciated measurements were made with a low-volume denuder and filter pack method (DEnuder for Long-Term Atmospheric sampling, DELTA®) as part of the EU NitroEurope (NEU) integrated project. Altogether, there were 64 sites in 20 countries (2006–2010), coordinated between seven European laboratories. Bulk wet-deposition measurements were carried out at 16 co-located sites (2008–2010). Inter-comparisons of chemical analysis and DELTA® measurements allowed an assessment of comparability between laboratories. The form and concentrations of the different gas and aerosol components measured varied between individual sites and grouped sites according to country, European regions, and four main ecosystem types (crops, grassland, forests, and semi-natural). The smallest concentrations (with the exception of SO42- and Na+) were in northern Europe (Scandinavia), with broad elevations of all components across other regions. SO2 concentrations were highest in central and eastern Europe, with larger SO2 emissions, but particulate SO42- concentrations were more homogeneous between regions. Gas-phase NH3 was the most abundant single measured component at the majority of sites, with the largest variability in concentrations across the network. The largest concentrations of NH3, NH4+ and NO-3 were at cropland sites in intensively managed agricultural areas (e.g. Borgo Cioffi in Italy), and the smallest were at remote semi-natural and forest sites (e.g. Lompolojänkkä, Finland), highlighting the potential for NH3 to drive the formation of both NH4+ and NO3- aerosol. In the aerosol phase, NH4+ was highly correlated with both NO3- and SO42-, with a near-1:1 relationship between the equivalent concentrations of NH4+ and sum(NO3- + SO42-) of which around 60 % was as NH4NO3. Distinct seasonality was also observed in the data, influenced by changes in emissions, chemical interactions, and the influence of meteorology on partitioning between the main inorganic gases and aerosol species. Springtime maxima in NH3 were attributed to the main period of manure spreading, while the peak in summer and trough in winter were linked to the influence of temperature and rainfall on emissions, deposition, and gas–aerosol-phase equilibrium. Seasonality in SO2 was mainly driven by emissions (combustion), with concentrations peaking in winter, except in southern Europe, where the peak occurred in summer. Particulate SO42− showed large peaks in concentrations in summer in southern and eastern Europe, contrasting with much smaller peaks occurring in early spring in other regions. The peaks in particulate SO42- coincided with peaks in NH3 concentrations, attributed to the formation of the stable (NH4)2SO4. HNO3 concentrations were more complex, related to traffic and industrial emissions, photochemistry, and HNO3:NH4NO3 partitioning. While HNO3 concentrations were seen to peak in the summer in eastern and southern Europe (increased photochemistry), the absence of a spring peak in HNO3 in all regions may be explained by the depletion of HNO3 through reaction with surplus NH3 to form the semi-volatile aerosol NH4NO3. Cooler, wetter conditions in early spring favour the formation and persistence of NH4NO3 in the aerosol phase, consistent with the higher springtime concentrations of NH4+ and NO3−. The seasonal profile of NO3- was mirrored by NH4+, illustrating the influence of gas–aerosol partitioning of NH4NO3 in the seasonality of these components. Gas-phase NH3 and aerosol NH4NO3 were the dominant species in the total inorganic gas and aerosol species measured in the NEU network. With the current and projected trends in SO2, NOx , and NH3 emissions, concentrations of NH3 and NH4NO3 can be expected to continue to dominate the inorganic pollution load over the next decades, especially NH3, which is linked to substantial exceedances of ecological thresholds across Europe. The shift from (NH4)2SO4 to an atmosphere more abundant in NH4NO3 is expected to maintain a larger fraction of reactive N in the gas phase by partitioning to NH3 and HNO3 in warm weather, while NH4NO3 continues to contribute to exceedances of air quality limits for PM2.5

Meteorological measurements at Auchencorth Moss from 1995 to 2016

The Auchencorth Moss atmospheric observatory has being measuring meteorological parameters since 1995. The site was originally set‐up to measure the deposition of sulphur dioxide at a site that represented the vegetation and climate typical of NW Europe, in relatively clean background air. It is one of the longest running flux monitoring sites in the region, over semi‐natural vegetation, providing infrastructure and support for many measurement campaigns and continuous monitoring of air pollutants and greenhouse gases. The meteorological sensors that are used, data processing and quality reviewing procedures are described for a set of core measurements up to 2016. These core measurements are essential for the interpretation of the other atmospheric variables

ECLAIRE: Effects of Climate Change on Air Pollution Impacts and Response Strategies for European Ecosystems. Project final report

The central goal of ECLAIRE is to assess how climate change will alter the extent to which air pollutants threaten terrestrial ecosystems. Particular attention has been given to nitrogen compounds, especially nitrogen oxides (NOx) and ammonia (NH3), as well as Biogenic Volatile Organic Compounds (BVOCs) in relation to tropospheric ozone (O3) formation, including their interactions with aerosol components. ECLAIRE has combined a broad program of field and laboratory experimentation and modelling of pollution fluxes and ecosystem impacts, advancing both mechanistic understanding and providing support to European policy makers. The central finding of ECLAIRE is that future climate change is expected to worsen the threat of air pollutants on Europe’s ecosystems. Firstly, climate warming is expected to increase the emissions of many trace gases, such as agricultural NH3, the soil component of NOx emissions and key BVOCs. Experimental data and numerical models show how these effects will tend to increase atmospheric N deposition in future. By contrast, the net effect on tropospheric O3 is less clear. This is because parallel increases in atmospheric CO2 concentrations will offset the temperature-driven increase for some BVOCs, such as isoprene. By contrast, there is currently insufficient evidence to be confident that CO2 will offset anticipated climate increases in monoterpene emissions. Secondly, climate warming is found to be likely to increase the vulnerability of ecosystems towards air pollutant exposure or atmospheric deposition. Such effects may occur as a consequence of combined perturbation, as well as through specific interactions, such as between drought, O3, N and aerosol exposure. These combined effects of climate change are expected to offset part of the benefit of current emissions control policies. Unless decisive mitigation actions are taken, it is anticipated that ongoing climate warming will increase agricultural and other biogenic emissions, posing a challenge for national emissions ceilings and air quality objectives related to nitrogen and ozone pollution. The O3 effects will be further worsened if progress is not made to curb increases in methane (CH4) emissions in the northern hemisphere. Other key findings of ECLAIRE are that: 1) N deposition and O3 have adverse synergistic effects. Exposure to ambient O3 concentrations was shown to reduce the Nitrogen Use Efficiency of plants, both decreasing agricultural production and posing an increased risk of other forms of nitrogen pollution, such as nitrate leaching (NO3-) and the greenhouse gas nitrous oxide (N2O); 2) within-canopy dynamics for volatile aerosol can increase dry deposition and shorten atmospheric lifetimes; 3) ambient aerosol levels reduce the ability of plants to conserve water under drought conditions; 4) low-resolution mapping studies tend to underestimate the extent of local critical loads exceedance; 5) new dose-response functions can be used to improve the assessment of costs, including estimation of the value of damage due to air pollution effects on ecosystems, 6) scenarios can be constructed that combine technical mitigation measures with dietary change options (reducing livestock products in food down to recommended levels for health criteria), with the balance between the two strategies being a matter for future societal discussion. ECLAIRE has supported the revision process for the National Emissions Ceilings Directive and will continue to deliver scientific underpinning into the future for the UNECE Convention on Long-range Transboundary Air Pollution

ECLAIRE third periodic report

The ÉCLAIRE project (Effects of Climate Change on Air Pollution Impacts and Response Strategies for European Ecosystems) is a four year (2011-2015) project funded by the EU's Seventh Framework Programme for Research and Technological Development (FP7)

Effects of changing temperature on leaf surface water-film chemistry and trace gas exchange processes over terrestrial vegetation. A contribution to ACCENT CCAQ Topic 2

The effects of an increase of air temperature on the stomatal conductance of beech, a widespread tree specie in Europe, have been examined by using a Jarvisian model of stomatal conductance calibrated on a sixth months long field experiment in northern Italy. An increase of few degrees centigrade in air temperature resulted in very little changes in the mean stomatal conductance of the trees, but the diurnal course of this important parameter underwent an evident change, consisting in increased stomatal conductance values in the first hours of the day and decreased values in the rest of the day, and particularly in the afternoon

The atmospheric budget of oxidized nitrogen and its role in ozone formation and deposition

Emissions of reactive oxidized nitrogen (NO and NO2), collectively known as NOx, from human activities are c. 21 Tg N annually, or 70% of global total emissions. They occur predominantly in industrialized regions, largely from fossil fuel combustion, but also from increased use of N fertilizers. Soil emissions of NO not only make an important contribution to global totals, but also play a part in regulating the dry deposition of NO and NO2 (NOx) to plant canopies. Soil microbial production of NO leads to a soil 'compensation point' for NO deposition or emission, which depends on soil temperature, N and water status. In warm conditions, the net emission of NOx from plant canopies contributes to the photochemical formation of ozone. Moreover, the effect of NOx emissions from soil is to reduce net rates of NO2 deposition to terrestrial surfaces over large areas. Increasing anthropogenic emissions of NOx have led to an approximate doubling in surface O3 concentrations since the last century. NOx acts as a catalyst for the production of O3 from volatile organic compounds (VOCs). Paradoxically, emission controls on motor vehicles might lead to increases in O3 concentrations in urban areas. Removal of NO and NO2 by dry deposition is regulated to some extent by soil production of NO; the major sink for NO2 is stomatal uptake. Long-term flux measurements over moorland in Scotland show very small deposition rates for NO2 at night and before mid-day of 1–4 ng NO2-N m−2 s−1, and similar emission rates during afternoon. The bi-directional flux gives 24-h average deposition velocities of only 1–2 mm s−1, and implies a long life-time for NOx due to removal by dry deposition. Rates of removal of O3 at the ground are also influenced by stomatal uptake, but significant non-stomatal uptake occurs at night and in winter. Measurements above moorland showed 40% of total annual flux was stomatal, with 60% non-stomatal, giving nocturnal and winter deposition velocities of 2–3 mm s−1 and daytime summer values of 10 mm s−1. The stomatal uptake is responsible for adverse effects on vegetation. The critical level for O3 exposure (AOT40) is used to derive a threshold O3 stomatal flux for wheat of 0·5 μg m−2 s−1. Use of modelled stomatal fluxes rather than exposure might give more reliable estimates of yield loss; preliminary calculations suggest that the relative grain yield reduction (%) can be estimated as 38 times the stomatal ozone flux (g m−2) above the threshold, summed over the growing season