•For moderate reductions, emission and PM concentration changes are linearly linked.•Reducing SO2 emissions where abundant is always efficient.•Reducing NH3 emissions is more efficient where it is ...less abundant.•Reducing NOx emissions where NOx are abundant can be counter-productive.•Both NOx and NH3 regimes occur in some regions, calling for combined reductions
Given the remaining air quality issues in many European regions, smart air quality strategies are necessary to reduce the burden of poor air quality. While designing effective strategies for non-reactive primary pollutants is straightforward, this is not the case for secondary pollutants for which the relationship between emission changes and the resulting concentration changes can be nonlinear. Under such conditions, strategies targeting the largest emitting sources might not be the most effective. In this work, we provide elements to better understand the role of the main emission precursors (SO2, NOx, NH3) on the formation of secondary inorganic aerosols. By quantifying the PM2.5 sensitivity to emission reductions for each of these three precursors, we define and quantify the intensity of PM2.5 formation chemical regimes across Europe. We find that for emission reductions limited to 25%, the relation between emission and PM concentration changes remain mostly linear, with the exception of the Po Valley where non-linearities reach more than 30% in winter. When emission reductions increase to 50%, non-linearity reaches more than 60% in the Po Valley but stay below 30% in the rest of Europe. In terms of implications on abatement strategies, our findings can be summarized in the following key messages: (1) reducing SO2 emissions where abundant is always efficient (e.g. eastern Europe and Balkans); (2) reducing NH3 emissions is more efficient where it is less abundant (e.g. the Po basin) than where it is abundant, given the limiting role of NH3 in the PM formation; (3) reducing NOx emissions where NOx are abundant can be counter-productive with potential increases of PM due to the increased oxidant capacity of the atmosphere (e.g. Po valley); (4) because regions with both NH3 and NOx sensitive chemical regimes are mixed within countries, both need to be reduced together, as pollution reduction policies need at least to be defined at a country level; (6) while for NH3 the focus is clearly on wintertime, it is the whole year for NOx. The simulations proposed in this work could be used as benchmark for other models as they constitute the type of scenarios required to support air quality strategies. In addition, the straight and systematic emission reductions imposed for the scenarios in this work are well suited for a better understanding of the behavior of the model, in terms of responses to emission reductions.
Tropospheric trace gas and aerosol pollutants have adverse effects on health, environment and climate. In order to quantify and mitigate such effects, a wide range of processes leading to the ...formation and transport of pollutants must be considered, understood and represented in numerical models. Regional scale pollution episodes result from the combination of several factors: high emissions (from anthropogenic or natural sources), stagnant meteorological conditions, kinetics and efficiency of the chemistry and the deposition. All these processes are highly variable in time and space, and their relative contribution to the pollutants budgets can be quantified with chemistry-transport models. The CHIMERE chemistry-transport model is dedicated to regional atmospheric pollution event studies. Since it has now reached a certain level a maturity, the new stable version, CHIMERE 2013, is described to provide a reference model paper. The successive developments of the model are reviewed on the basis of published investigations that are referenced in order to discuss the scientific choices and to provide an overview of the main results.
This paper describes the pre-operational analysis and forecasting system developed during MACC (Monitoring Atmospheric Composition and Climate) and continued in the MACC-II (Monitoring Atmospheric ...Composition and Climate: Interim Implementation) European projects to provide air quality services for the European continent. This system is based on seven state-of-the art models developed and run in Europe (CHIMERE, EMEP, EURAD-IM, LOTOS-EUROS, MATCH, MOCAGE and SILAM). These models are used to calculate multi-model ensemble products. The paper gives an overall picture of its status at the end of MACC-II (summer 2014) and analyses the performance of the multi-model ensemble. The MACC-II system provides daily 96 h forecasts with hourly outputs of 10 chemical species/aerosols (O3, NO2, SO2, CO, PM10, PM2.5, NO, NH3, total NMVOCs (non-methane volatile organic compounds) and PAN+PAN precursors) over eight vertical levels from the surface to 5 km height. The hourly analysis at the surface is done a posteriori for the past day using a selection of representative air quality data from European monitoring stations. The performance of the system is assessed daily, weekly and every 3 months (seasonally) through statistical indicators calculated using the available representative air quality data from European monitoring stations. Results for a case study show the ability of the ensemble median to forecast regional ozone pollution events. The seasonal performances of the individual models and of the multi-model ensemble have been monitored since September 2009 for ozone, NO2 and PM10. The statistical indicators for ozone in summer 2014 show that the ensemble median gives on average the best performances compared to the seven models. There is very little degradation of the scores with the forecast day but there is a marked diurnal cycle, similarly to the individual models, that can be related partly to the prescribed diurnal variations of anthropogenic emissions in the models. During summer 2014, the diurnal ozone maximum is underestimated by the ensemble median by about 4 μg m−3 on average. Locally, during the studied ozone episodes, the maxima from the ensemble median are often lower than observations by 30–50 μg m−3. Overall, ozone scores are generally good with average values for the normalised indicators of 0.14 for the modified normalised mean bias and of 0.30 for the fractional gross error. Tests have also shown that the ensemble median is robust to reduction of ensemble size by one, that is, if predictions are unavailable from one model. Scores are also discussed for PM10 for winter 2013–1014. There is an underestimation of most models leading the ensemble median to a mean bias of −4.5 μg m−3. The ensemble median fractional gross error is larger for PM10 (~ 0.52) than for ozone and the correlation is lower (~ 0.35 for PM10 and ~ 0.54 for ozone). This is related to a larger spread of the seven model scores for PM10 than for ozone linked to different levels of complexity of aerosol representation in the individual models. In parallel, a scientific analysis of the results of the seven models and of the ensemble is also done over the Mediterranean area because of the specificity of its meteorology and emissions. The system is robust in terms of the production availability. Major efforts have been done in MACC-II towards the operationalisation of all its components. Foreseen developments and research for improving its performances are discussed in the conclusion.
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