Stéphane Sauvage, Eric van der Swaluw, Oksana Tarasova, Esperanza Perdrix, Hartmut Herrmann, Xavier Querol, Véronique Riffault, Olivier Favez, D. Mooibroek, Dominik van Pinxteren, Andrés Alastuey, Christoph Hüglin, Augustin Colette, Philip K. Hopke, Marco Pandolfi, Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Generalitat de Catalunya, Ministère de l'Écologie, du Développement durable et de l'Énergie (France), Agence Nationale de la Recherche (France), European Commission, Lower Saxony State Government, Institute of Environmental Assessment and Water Research (IDAEA), Consejo Superior de Investigaciones Científicas [Madrid] (CSIC), National Institute for Public Health and the Environment [Bilthoven] (RIVM), Clarkson University, Leibniz Institute for Tropospheric Research (TROPOS), Institut National de l'Environnement Industriel et des Risques (INERIS), Swiss Federal Laboratories for Materials Science and Technology [Dübendorf] (EMPA), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), Centre for Energy and Environment (CERI EE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), World Meteorological Organization (WMO), and ANR-11-LABX-0005,Cappa,Physiques et Chimie de l'Environnement Atmosphérique(2011)
Here we report results of a detailed analysis of the urban and non-urban contributions to particulate matter (PM) concentrations and source contributions in five European cities, namely Schiedam (the Netherlands, NL), Lens (France, FR), Leipzig (Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM chemically speciated data from 12 European paired monitoring sites (one traffic, five urban, five regional and one continental background) were analysed by positive matrix factorisation (PMF) and Lenschow's approach to assign measured PM and source contributions to the different spatial levels. Five common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols, road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM mass at urban low-traffic-impact sites (UB) depending on the country. Three additional common sources were identified at a subset of sites/countries, namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %-13 % of PM mass, and residual oil combustion (V-Ni) and primary industrial (IND) (NL and ES), together explaining an additional 11 %-15 % of PM mass. In all countries, the majority of PM measured at UB sites was of a regional+continental (R+C) nature (64 %-74 %). The R+C PM increments due to anthropogenic emissions in DE, NL, CH, ES and FR represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively, of UB PM mass. Overall, the R+C PM increments due to natural and anthropogenic sources showed opposite seasonal profiles with the former increasing in summer and the latter increasing in winter, even if exceptions were observed. In ES, the anthropogenic R+C PM increment was higher in summer due to high contributions from regional SSA and V-Ni sources, both being mostly related to maritime shipping emissions at the Spanish sites. Conversely, in the other countries, higher anthropogenic R+C PM increments in winter were mostly due to high contributions from NSA and BB regional sources during the cold season. On annual average, the sources showing higher R+C increments were SSA (77 %-91 % of SSA source contribution at the urban level), NSA (51 %-94 %), MM (58 %-80 %), BB (42 %-78 %) and IND (91 % in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %-99 %; identified only in DE). The highest regional SSA increment was observed in ES, especially in summer, and was related to ship emissions, enhanced photochemistry and peculiar meteorological patterns of the Western Mediterranean. The highest R+C and urban NSA increments were observed in NL and associated with high availability of precursors such as NOx and NH3. Conversely, on average, the sources showing higher local increments were RT (62 %-90 % at all sites) and V-Ni (65 %-80 % in ES and NL). The relationship between SSA and V-Ni indicated that the contribution of ship emissions to the local sulfate concentrations in NL has strongly decreased since 2007 thanks to the shift from high-sulfur-to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities included here could be achieved by further reducing local (urban) emissions of PM, NOx and NH3 (from both traffic and non-traffic sources) but also SO2 and PM (from maritime ships and ports) and giving high relevance to non-urban contributions by further reducing emissions of SO2 (maritime shipping) and NH3 (agriculture) and those from industry, regional BB sources and coal combustion., Measurements were funded by the Spanish Ministry of Economy, Industry and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R) and by the Generalitat de Catalunya (AGAUR 2014 SGR33, AGAUR 2017 SGR41 and the DGQA), by the French Ministry of Environment (Bureau de l'Air du Ministère de l'Ecologie, du Développement durable, et de l’Energie), by the French National Research Agency (ANR) and by the Regional Council “Hauts-de-France” and the European Regional Development Fund (ERDF), and by the Saxon State Office for Environment, Agriculture and Geology (LfULG).