Prediction of source contributions to urban background PM10 concentrations in European cities: a case study for an episode in December 2016 using EMEP/MSC-W rv4.15 and LOTOS-EUROS v2.0 – Part 1: The country contributions

A large fraction of the urban population in Europe is exposed to particulate matter levels above the WHO guideline value. To make more effective mitigation strategies, it is important to understand the influence on particulate matter (PM) from pollutants emitted in different European nations. In this study, we evaluate a country source contribution forecasting system aimed at assessing the domestic and transboundary contributions to PM in major European cities for an episode in December 2016. The system is composed of two models (EMEP/MSC-W rv4.15 and LOTOS-EUROS v2.0), which allows the consideration of differences in the source attribution. We also compared the PM10 concentrations, and both models present satisfactory agreement in the 4 d forecasts of the surface concentrations, since the hourly concentrations can be highly correlated with in situ observations. The correlation coefficients reach values of up to 0.58 for LOTOS-EUROS and 0.50 for EMEP for the urban stations; the values are 0.58 for LOTOS-EUROS and 0.72 for EMEP for the rural stations. However, the models underpredict the highest hourly concentrations measured by the urban stations (mean underestimation of 36 %), which is to be expected given the relatively coarse model resolution used (0.25∘ longitude × 0.125∘ latitude). For the source attribution calculations, LOTOS-EUROS uses a labelling technique, while the EMEP/MSC-W model uses a scenario having reduced anthropogenic emissions, and then it is compared to a reference run where no changes are applied. Different percentages (5 %, 15 %, and 50 %) for the reduced emissions in the EMEP/MSC-W model were used to test the robustness of the methodology. The impact of the different ways to define the urban area for the studied cities was also investigated (i.e. one model grid cell, nine grid cells, and grid cells covering the definition given by the Global Administrative Areas – GADM). We found that the combination of a 15 % emission reduction and a larger domain (nine grid cells or GADM) helps to preserve the linearity between emission and concentrations changes. The nonlinearity, related to the emission reduction scenario used, is suggested by the nature of the mismatch between the total concentration and the sum of the concentrations from different calculated sources. Even limited, this nonlinearity is observed in the NO3-, NH4+, and H2O concentrations, which is related to gas–aerosol partitioning of the species. The use of a 15 % emission reduction and of a larger city domain also causes better agreement on the determination of the main country contributors between both country source calculations. Over the 34 European cities investigated, PM10 was dominated by domestic emissions for the studied episode (1–9 December 2016). The two models generally agree on the dominant external country contributor (68 % on an hourly basis) to PM10 concentrations. Overall, 75 % of the hourly predicted PM10 concentrations of both models have the same top five main country contributors. Better agreement on the dominant country contributor for primary (emitted) species (70 % is found for primary organic matter (POM) and 80 % for elemental carbon – EC) than for the inorganic secondary component of the aerosol (50 %), which is predictable due to the conceptual differences in the source attribution used by both models. The country contribution calculated by the scenario approach depends on the chemical regime, which largely impacts the secondary components, unlike the calculation using the labelling approach.