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Over the past century, ammonia (NH3) emissions have increased with the growth of livestock and fertilizer usage. The abundant NH3 emissions lead to secondary fine particulate matter (PM2.5) pollution, climate change, and a reduction in biodiversity, and they affect human health. Up-to-date and spatially and temporally resolved information on NH3 emissions is essential to better quantify their impact. In this study we applied the existing Daily Emissions Constrained by Satellite Observations (DECSO) algorithm to NH3 observations from the Cross-track Infrared Sounder (CrIS) to estimate NH3 emissions. Because NH3 in the atmosphere is influenced by nitrogen oxides (NOx), we implemented DECSO to estimate NOx and NH3 emissions simultaneously. The emissions are derived over Europe for 2020 on a spatial resolution of 0.2°×0.2° using daily observations from both CrIS and the TROPOspheric Monitoring Instrument (TROPOMI; on the Sentinel-5 Precursor (S5P) satellite). Due to the limited number of daily satellite observations of NH3, monthly emissions of NH3 are reported. The total NH3 emissions derived from observations are about 8 Tg yr−1, with a precision of about 5 %–17 % per grid cell per year over the European domain (35–55° N, 10° W–30° E). The comparison of the satellite-derived NH3 emissions from DECSO with independent bottom-up inventories and in situ observations indicates a consistency in terms of magnitude on the country totals, with the results also being comparable regarding the temporal and spatial distributions. The validation of DECSO over Europe implies that we can use DECSO to quickly derive fairly accurate monthly emissions of NH3 over regions with limited local information on NH3 emissions.

European emission trends of nitrogen oxides since 1880 and up to present are presented here and are linked to the evolution of road transport emissions. Road transport has been the dominating source of NOx emissions since 1970, and contributes with 40% to the total emissions in 2005. Five trend regimes have been identified between 1880 and 2005. The first regime (1880–1950) is determined by a slow increase in fuel consumption all over Europe. The second regime (1950–1980) is characterized by a continued steep upward trend in liquid fuel use and by the introduction of the first regulations on road traffic emissions. Reduction in fuel consumption determines the emission trends in the third regime (1980–1990) that is also characterized by important differences between Eastern and Western Europe. Emissions from road traffic continue to grow in Western Europe in this period, and it is argued here that the reason for this continued NOx emission increase is related to early inefficient regulations for NOx in the transport sector. The fourth regime (1990–2000) involves a turning point for road traffic emissions, with a general decrease of emissions in Europe during that decade. It is in this period that we can identify the first emission reductions due to technological abatement in Western Europe. In the fifth regime (2000–2005), the economic recovery in Eastern Europe imposes increased emission from road traffic in this area. Western European emissions are on the other hand decoupled from the fuel consumption, and continue to decrease. The implementation of strict measures to control NOx emissions is demonstrated here to be a main reason for the continued Western European emission reductions. The results indicate that even though the effectiveness of European standards is hampered by a slow vehicle turnover, loopholes in the type-approval testing, and an increase in diesel consumption, the effect of such technical abatement measures is traceable in the evolution of European road traffic emissions over the last 15 years.

While the burden caused by air pollution in urban areas is well documented, the origin of this pollution and therefore the responsibility of the urban areas in generating this pollution are still a subject of scientific discussion. Source apportionment represents a useful technique to quantify the city's responsibility, but the approaches and applications are not harmonized and therefore not comparable, resulting in confusing and sometimes contradicting interpretations. In this work, we analyse how different source apportionment approaches apply to the urban scale and how their building elements and parameters are defined and set. We discuss in particular the options available in terms of indicator, receptor, source, and methodology. We show that different choices for these options lead to very large differences in terms of outcome. For the 150 large EU cities selected in our study, different choices made for the indicator, the receptor, and the source each lead to an average difference of a factor of 2 in terms of city contribution. We also show that temporal- and spatial-averaging processes applied to the air quality indicator, especially when diverging source apportionments are aggregated into a single number, lead to the favouring of strategies that target background sources while occulting actions that would be efficient in the city centre. We stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility, with important implications. Indeed, if cities are seen as a minor actor, plans will target the background as a priority at the expense of potentially effective local actions.

Information on the origin of pollution constitutes an essential step of air quality management as it helps identifying measures to control air pollution. In this work, we review the most widely used source-apportionment methods for air quality management. Using theoretical and real-case datasets we study the differences among these methods and explain why they result in very different conclusions to support air quality planning. These differences are a consequence of the intrinsic assumptions that underpin the different methodologies and determine/limit their range of applicability. We show that ignoring their underlying assumptions is a risk for efficient/successful air quality management as these methods are sometimes used beyond their scope and range of applicability. The simplest approach based on increments (incremental approach) is often not suitable to support air quality planning. Contributions obtained through mass-transfer methods (receptor models or tagging approaches built in air quality models) are appropriate to support planning but only for specific pollutants. Impacts obtained via “brute-force” methods are the best suited but it is important to assess carefully their application range to make sure they reproduce correctly the prevailing chemical regimes. Keywords: Urban air pollution, Source allocation, Source apportionment, Increment, Contribution, Impact, Air quality planning, Brute force, Mitigation strategy

The expedited near-real-time Level 1.5 Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) version 3 products were evaluated against data from the ground-based European Aerosol Research Lidar Network (EARLINET). The statistical framework and results of the three-year evaluation of 48 CALIOP overpasses with ground tracks within a 100 km distance from operating EARLINET stations are presented and include analysis for the following CALIOP classifications of aerosol type: dust, polluted dust, clean marine, clean continental, polluted continental, mixed and/or smoke/biomass burning. For the complete data set comprising both the planetary boundary layer (PBL) and the free troposphere (FT) data, the correlation coefficient (R) was 0.86. When the analysis was conducted separately for the PBL and FT, the correlation coefficients were R = 0.6 and R = 0.85, respectively. From analysis of selected specific cases, it was initially thought that the presence of FT layers, with high attenuated backscatter, led to poor agreement of the PBL backscatter profiles between the CALIOP and EARLINET and prompted a further analysis to filter out such cases; however, removal of these layers did not improve the agreement as R reduced marginally from R = 0.86 to R = 0.84 for the combined PBL and FT analysis, increased marginally from R = 0.6 up to R = 0.65 for the PBL on its own, and decreased marginally from R = 0.85 to R = 0.79 for the FT analysis on its own. This suggests considerable variability, across the data set, in the spatial distribution of the aerosol over spatial scales of 100 km or less around some EARLINET stations rather than influence from elevated FT layers. For specific aerosol types, the correlation coefficient between CALIOP backscatter profiles and the EARLINET data ranged from R = 0.37 for polluted continental aerosol in the PBL to R = 0.57 for dust in the FT.

The EMEP4UK modelling system is a high resolution (5×5 km2) application of the EMEP chemistry-transport model, designed for scientific and policy studies in the UK. We demonstrate the use and performance of the EMEP4UK system through the study of ground-level ozone (O3) during the extreme August 2003 heat-wave. Meteorology is generated by the Weather Research and Forecast (WRF) model, nudged every six hours with reanalysis data. We focus on SE England, where hourly average O3 reached up to 140 ppb during the heat-wave. EMEP4UK accurately reproduces elevated O3 and much of its day-to-day variability during the heat-wave. Key O3 precursors, nitrogen dioxide and isoprene, are less well simulated, but show generally accurate diurnal cycles and concentrations to within a factor of ~2–3 of observations. The modelled surface O3 distribution has an intricate spatio-temporal structure, governed by a combination of meteorology, emissions and photochemistry. A series of sensitivity runs with the model are used to explore the factors that influenced O3 levels during the heat-wave. Various factors appear to be important on different days and at different sites. Ozone imported from outside the model domain, especially the south, is very important on several days during the heat-wave, contributing up to 85 ppb. The effect of dry deposition is also important on several days. Modelled isoprene concentrations are generally best simulated if isoprene emissions are changed from the base emissions: typically doubled, but elevated by up to a factor of five on one hot day. We found that accurate modelling of the exact positions of nitrogen oxide and volatile organic compound plumes is crucial for the successful simulation of O3 at a particular time and location. Variations in temperature of ±5 K were found to have impacts on O3 of typically less than ±10 ppb.

During the last twenty-five years European emission data have been compiled and reported under the Cooperative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe (EMEP) as part of the work under the UNECE Convention on Long-range Transboundary Air Pollution (LRTAP). This paper presents emission trends of SO2 reported to EMEP and validated within the programme for the period 1980–2004. These European anthropogenic sulphur emissions have been steadily decreasing over the last twenty-five years, amounting from about 55 Tg SO2 in 1980 to 15 Tg SO2 in 2004. The uncertainty in sulphur emission estimates for individual countries and years are documented to range between 3% and 25%. The relative contribution of European emissions to global anthropogenic sulphur emissions has been halved during this period. Based on annual emission reports from European countries, three emission reduction regimes have been identified. The period 1980–1989 is characterized by low annual emission reductions (below 5% reduction per year and 20% for the whole period) and is dominated by emission reductions in Western Europe. The period 1990–1999 is characterised by high annual emission reductions (up to 11% reduction per year and 54% for the whole period), most pronounced in Central and Eastern Europe. The annual emission reductions in the period 2000–2004 are medium to low (below 6% reduction per year and 17% for the whole period) and reflect the unified Europe, with equally large reductions in both East and West. The sulphur emission reduction has been largest in the sector Combustion in energy and transformation industries, but substantial decreases are also seen in the Non-industrial combustion plants together with the sectors Industrial combustion and Industrial production processes. The majority of European countries have reduced their emissions by more than 60% between 1990 and 2004, and one quarter have already achieved sulphur emission reductions higher than 80%. At European level, the total sulphur target for 2010 set in the Gothenburg Protocol (16 Tg) has apparently already been met by 2004. However, still half of the Parties to the Gothenburg Protocol have to reduce further their sulphur emissions in order to attain their individual country total emission targets for 2010. It is also noteworthy that, contrasting the Gothenburg Protocol requirements, a growing number of countries have recently been reporting increasing sulphur emissions, while others report only minor further decreases. The emission trends presented here are supported by different studies of air concentrations and depositions carried out within and outside the framework of the LRTAP Convention.

This paper presents the first outcomes of the "FAIRMODE pilot" activity, aiming at improving the way in which air quality models are used in the frame of the European "Air Quality Directive". Member States may use modelling, combined with measurements, to "assess" current levels of air quality and estimate future air quality under different scenarios. In case of current and potential exceedances of the Directive limit values, it is also requested that they "plan" and implement emission reductions measures to avoid future exceedances. In both "assessment" and "planning", air quality models can and should be used; but to do so, the used modelling chain has to be fit-for-purpose and properly checked and verified. FAIRMODE has developed in the recent years a suite of methodologies and tools to check if emission inventories, model performance, source apportionment techniques and planning activities are fit-for-purpose. Within the "FAIRMODE pilot", these tools are used and tested by regional/local authorities, with the two-fold objective of improving management practices at regional/local scale, and providing valuable feedback to the FAIRMODE community. Results and lessons learnt from this activity are presented in this paper, as a showcase that can potentially benefit other authorities in charge of air quality assessment and planning., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Information on the origin of pollution constitutes an essential step of air quality management as it helps identifying measures to control air pollution. In this work, we review the most widely used source-apportionment methods for air quality management. Using theoretical and real-case datasets we study the differences among these methods and explain why they result in very different conclusions to support air quality planning. These differences are a consequence of the intrinsic assumptions that underpin the different methodologies and determine/limit their range of applicability. We show that ignoring their underlying assumptions is a risk for efficient/successful air quality management as these methods are sometimes used beyond their scope and range of applicability. The simplest approach based on increments (incremental approach) is often not suitable to support air quality planning. Contributions obtained through mass-transfer methods (receptor models or tagging approaches built in air quality models) are appropriate to support planning but only for specific pollutants. Impacts obtained via "brute-force" methods are the best suited but it is important to assess carefully their application range to make sure they reproduce correctly the prevailing chemical regimes., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

A methodology is proposed to support the evaluation and comparison of different types of emission inventories. The strengths and weaknesses of the methodology are presented and discussed based on an example. The approach results in a "diamond" diagram useful to flag out anomalous behaviors in the emission inventories and to get insight in possible explanations. In particular, the "diamond" diagram is shown to provide meaningful information in terms of: discrepancies between the total emissions reported by macro-sector and pollutant, contribution of each macro-sector to the total amount of emissions released by pollutant, and the identification and quantification of the different factors causing the discrepancies between total emissions. A practical example in Barcelona is used for testing and to provide relevant information for the analyzed emission datasets. The tests show the capability of the proposed methodology to flag inconsistencies in the existing inventories. The proposed methodology system may be useful for regional and urban inventory developers as an initial evaluation of the consistency of their inventories.