A one-year comprehensive chemical characterisation of fine aerosol (PM2.5) at urban, suburban and rural background sites in the region of Paris (France)

摘要

Studies describing the chemical composition of fine aerosol (PM_(2.5)) in urban areas are often conducted for a few weeks only and at one sole site, giving thus a narrow view of their temporal and spatial characteristics. This paper presents a one-year (11 September 2009-10 September 2010) survey of the daily chemical composition of PM_(2.5) in the region of Paris, which is the second most populated "Larger Urban Zone" in Europe. Five sampling sites representative of suburban (SUB), urban (URB), northeast (NER), northwest (NWR) and south (SOR) rural backgrounds were implemented. The major chemical components of PM_(2.5) were determined including elemental carbon (EC), organic carbon (OC), and the major ions. OC was converted to organic matter (OM) using the chemical mass closure methodology, which leads to conversion factors of 1.95 for the SUB and URB sites, and 2.05 for the three rural ones. On average, gravimetrically determined PM_(2.5) annual mass concentrations are 15.2, 14.8, 12.6, 11.7 and 10.8 μg m~(-3) for SUB, URB, NER, NWR and SOR sites, respectively. The chemical composition of fine aerosol is very homogeneous at the five sites and is composed of OM (38-47%), nitrate (17-22%), non-sea-salt sulfate (13-16%), ammonium (10-12%), EC (4-10%), mineral dust (2-5%) and sea salt (3-4%). This chemical composition is in agreement with those reported in the literature for most European environments. On an annual scale, Paris (URB and SUB sites) exhibits its highest PM_(2.5) concentrations during late autumn, winter and early spring (higher than 15 μg m~(-3) on average, from December to April), intermediates during late spring and early autumn (between 10 and 15 μg m~(-3) during May, June, September, October, and November) and the lowest during summer (below 10 μg m~(-3) during July and August). PM levels are mostly homogeneous on a regional scale, during the whole project (e.g. for URB plotted against NER sites: slope 1.06, r 2=0.84, n=330), suggesting the importance of mid-or long-range transport, and regional instead of local scale phenomena. During this one-year project, two thirds of the days exceeding the PM_(2.5) 2015 EU annual limit value of 25 μg m~(-3) were due to continental import from countries located northeast, east of France. This result questions the efficiency of local, regional and even national abatement strategies during pollution episodes, pointing to the need for a wider collaborative work with the neighbouring countries on these topics. Nevertheless, emissions of local anthropogenic sources lead to higher levels at the URB and SUB sites compared to the others (e.g. 26% higher on average at the URB than at the NWR site for PM_(2.5), during the whole campaign), which can even be emphasised by specific meteorological conditions such as low boundary layer heights. OM and secondary inorganic species (nitrate, non-sea-salt sulfate and ammonium, noted SIA) are mainly imported by mid-or long-range transport (e.g. for NWR plotted against URB sites: slope 0.79,r~2=0.72, n=335 for OM, and slope 0.91,r~2=0.89, n=335 for SIA) whereas EC is primarily locally emitted (e.g. for SOR plotted against URB sites: slope 0.27;r~2=0.03; n=335). This database will serve as a basis for investigating carbonaceous aerosols, metals as well as the main sources and geographical origins of PM in the region of Paris.