Abstract

Abstract. The present study aims at identifying and apportioning fine aerosols to their major sources in Paris (France) – the second most populated "larger urban zone" in Europe – and determining their geographical origins. It is based on the daily chemical composition of PM2.5 examined over 1 year at an urban background site of Paris (Bressi et al., 2013). Positive matrix factorization (EPA PMF3.0) was used to identify and apportion fine aerosols to their sources; bootstrapping was performed to determine the adequate number of PMF factors, and statistics (root mean square error, coefficient of determination, etc.) were examined to better model PM2.5 mass and chemical components. Potential source contribution function (PSCF) and conditional probability function (CPF) allowed the geographical origins of the sources to be assessed; special attention was paid to implement suitable weighting functions. Seven factors, namely ammonium sulfate (A.S.)-rich factor, ammonium nitrate (A.N.)-rich factor, heavy oil combustion, road traffic, biomass burning, marine aerosols and metal industry, were identified; a detailed discussion of their chemical characteristics is reported. They contribute 27, 24, 17, 14, 12, 6 and 1% of PM2.5 mass (14.7 μg m−3) respectively on the annual average; their seasonal variability is discussed. The A.S.- and A.N.-rich factors have undergone mid- or long-range transport from continental Europe; heavy oil combustion mainly stems from northern France and the English Channel, whereas road traffic and biomass burning are primarily locally emitted. Therefore, on average more than half of PM2.5 mass measured in the city of Paris is due to mid- or long-range transport of secondary aerosols stemming from continental Europe, whereas local sources only contribute a quarter of the annual averaged mass. These results imply that fine-aerosol abatement policies conducted at the local scale may not be sufficient to notably reduce PM2.5 levels at urban background sites in Paris, suggesting instead more coordinated strategies amongst neighbouring countries. Similar conclusions might be drawn in other continental urban background sites given the transboundary nature of PM2.5 pollution.

Highlights

  • Aerosols are airborne solid or liquid particles arising from various natural and anthropogenic sources (IPCC, 2007)

  • Too few factors will result in a mixing of different sources in the same factor as well as high residuals, whereas too many factors will lead to meaningless sources made up of a sole chemical species

  • Based on 1-year PM2.5 sampling at an urban site located in Paris (France), and on the use of statistical tools (EPA PMF3.0, conditional probability function (CPF), Potential source contribution function (PSCF)), this study allowed for (i) the identification of seven positive matrix factorization (PMF) factors that were related to real aerosol sources, (ii) the identification of the geographical origins of each factor, and (iii) the apportionment of each factor to PM2.5 mass discussed on yearly and seasonal bases

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Summary

Introduction

Aerosols are airborne solid or liquid particles arising from various natural and anthropogenic sources (IPCC, 2007) They are directly emitted into the atmosphere as particles (primary aerosols) or result from gas-to-particle conversions (secondary aerosols, Raes et al, 2000). Aerosols are subjects of concern for sanitary (Bernstein et al, 2004; Pope and Dockery, 2006), climatic (Forster et al, 2007; Isaksen et al, 2009) and economic reasons (Aphekom, 2012; US EPA, 2012), to name a few (see US EPA, 2011 for further details) Due to their enhanced adverse health effects in particular, fine particles (PM2.5, i.e. particles with an aerodynamic diameter less than or equal to 2.5 μm). Bressi et al.: Sources and geographical origins of fine aerosols in Paris have been subject to a stringent legislative framework during recent years

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