Sciare J.,French Climate and Environment Sciences Laboratory |
D'Argouges O.,French Climate and Environment Sciences Laboratory |
Zhang Q.J.,University Paris Diderot |
Sarda-Esteve R.,French Climate and Environment Sciences Laboratory |
And 4 more authors.
Atmospheric Chemistry and Physics | Year: 2010
Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM2.5). This time-resolved dataset allowed investigating the factors controlling the levels of PM2.5 in Paris and showed that polluted periods with PM2.5 > 15 μg mg-3 were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM2.5 concentrations (typically of about 10 μg mg-3); carbonaceous aerosols contributing for most of this mass (typically 75%). In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM2.5 over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM2.5 and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols. © 2010 Author(s).
Lopez M.,French Climate and Environment Sciences Laboratory |
Schmidt M.,French Climate and Environment Sciences Laboratory |
Delmotte M.,French Climate and Environment Sciences Laboratory |
Colomb A.,French National Center for Scientific Research |
And 9 more authors.
Atmospheric Chemistry and Physics | Year: 2013
Measurements of the mole fraction of the CO2 and its isotopes were performed in Paris during the MEGAPOLI winter campaign (January-February 2010). Radiocarbon (14CO2) measurements were used to identify the relative contributions of 77% CO2 from fossil fuel consumption (CO2ff from liquid and gas combustion) and 23% from biospheric CO2 (CO2 from the use of biofuels and from human and plant respiration: CO2bio). These percentages correspond to average mole fractions of 26.4 ppm and 8.2 ppm for CO2ff and CO2bio, respectively. The 13CO2 analysis indicated that gas and liquid fuel contributed 70% and 30%, respectively, of the CO2 emission from fossil fuel use. Continuous measurements of CO and NOx and the ratios CO/CO2ff and NOx/CO2ff derived from radiocarbon measurements during four days make it possible to estimate the fossil fuel CO2 contribution over the entire campaign. The ratios CO/CO2ff and NOx/CO2ff are functions of air mass origin and exhibited daily ranges of 7.9 to 14.5 ppb ppm-1 and 1.1 to 4.3 ppb ppm-1, respectively. These ratios are consistent with different emission inventories given the uncertainties of the different approaches. By using both tracers to derive the fossil fuel CO2, we observed similar diurnal cycles with two maxima during rush hour traffic. © 2013 Author(s).
Ammoura L.,CEA Saclay Nuclear Research Center |
Xueref-Remy I.,CEA Saclay Nuclear Research Center |
Gros V.,CEA Saclay Nuclear Research Center |
Baudic A.,CEA Saclay Nuclear Research Center |
And 7 more authors.
Atmospheric Chemistry and Physics | Year: 2014
Measurements of CO2, CO, NOx and selected Volatile Organic Compounds (VOCs) mole fractions were performed continuously during a 10-day period in the Guy Môquet tunnel in Thiais, a peri-urban area about 15 km south of the centre of Paris, between 28 September and 8 October 2012. This data set is used here to identify the characteristics of traffic-emitted CO2 by evaluating its ratios to co-emitted species for the first time in the Paris region. High coefficients of determination (r2> 0.7) are observed between CO2 and certain compounds that are characteristic of the traffic source (CO, NOx, benzene, xylenes and acetylene). Weak correlations (2 0.2) are found with species such as propane, n-butane and i-butane that are associated with fuel evaporation, an insignificant source for CO2. To better characterise the traffic signal we focus only on species that are well-correlated with CO2 and on rush-hour periods characterised by the highest traffic-related mole fractions. From those mole fractions we remove the nighttime-average weekday mole fraction obtained for each species that we infer to be the most appropriate background signal for our study. Then we calculate observed δspecies δCO2 ratios, which we compare with the ones provided by the 2010 bottom-up high-resolved regional emission inventory from Airparif (the association in charge of monitoring the air quality in Île-de-France), focusing on local emission data for the specific road of the tunnel. We find an excellent agreement (2%) between the local inventory emission CO2 ratio and our observed CO2 ratio. Former tunnel experiments carried out elsewhere in the world provided observed CO2 ratios that differ from 49 to 592% to ours. This variability can be related to technological improvement of vehicles, differences in driving conditions, and fleet composition. We also find a satisfactory agreement with the Airparif inventory for n-propylbenzene, n-pentane and xylenes to CO2 ratios. For most of the other species, the ratios obtained from the local emission inventory overestimate the observed ratios to CO2 by 34 to more than 300%. However, the emission ratios of NOx, o-xylene and i-pentane are underestimated by 30 to 79%. One main cause of such high differences between the inventory and our observations is likely the obsolete feature of the VOCs speciation matrix of the inventory that has not been updated since 1998, although law regulations on some VOCs have occurred since that time. Our study bears important consequences, discussed in the conclusion, for the characterisation of the urban CO2 plume and for atmospheric inverse modelling of urban CO2 emissions. © Author(s) 2014.
Poulakis E.,University of Crete |
Theodosi C.,University of Crete |
Bressi M.,CEA Saclay Nuclear Research Center |
Sciare J.,CEA Saclay Nuclear Research Center |
And 3 more authors.
Environmental Science and Pollution Research | Year: 2015
A variety of mineral components (Al, Fe) and trace metals (V, Cr, Mn, Ni, Cu, Zn, Cd, Pb) were simultaneously measured in PM2.5 and PM10 fractions at three different locations (traffic, urban, and suburban) in the Greater Paris Area (GPA) on a daily basis throughout a year. Mineral species and trace metal levels measured in both fractions are in agreement with those reported in the literature and below the thresholds defined by the European guidelines for toxic metals (Cd, Ni, Pb). Size distribution between PM2.5 and PM10 fractions revealed that mineral components prevail in the coarse mode, while trace metals are mainly confined in the fine one. Enrichment factor analysis, statistical analysis, and seasonal variability suggest that elements such as Mn, Cr, Zn, Fe, and Cu are attributed to traffic, V and Ni to oil combustion while Cd and Pb to industrial activities with regional origin. Meteorological parameters such as rain, boundary layer height (BLH), and air mass origin were found to significantly influence element concentrations. Periods with high frequency of northern and eastern air masses (from high populated and industrialized areas) are characterized by high metal concentrations. Finally, inner city and traffic emissions were also evaluated in PM2.5 fraction. Significant contributions (>50 %) were measured in the traffic site for Mn, Fe, Cr, Zn, and Cu, confirming that vehicle emissions contribute significantly to their levels, while in the urban site, the lower contributions (18 to 33 %) for all measured metals highlight the influence of regional sources on their levels. © 2015, Springer-Verlag Berlin Heidelberg.
Petetin H.,University Paris Est Creteil |
Beekmann M.,University Paris Est Creteil |
Colomb A.,University Paris Est Creteil |
Colomb A.,CNRS Laboratory of Physics and Meteorology |
And 11 more authors.
Atmospheric Chemistry and Physics | Year: 2015
High uncertainties affect black carbon (BC) emissions, and, despite its important impact on air pollution and climate, very few BC emissions evaluations are found in the literature. This paper presents a novel approach, based on airborne measurements across the Paris, France, plume, developed in order to evaluate BC and NOx emissions at the scale of a whole agglomeration. The methodology consists in integrating, for each transect, across the plume observed and simulated concentrations above background. This allows for several error sources (e.g., representativeness, chemistry, plume lateral dispersion) to be minimized in the model used. The procedure is applied with the CHIMERE chemistry-transport model to three inventories - the EMEP inventory and the so-called TNO and TNO-MP inventories - over the month of July 2009. Various systematic uncertainty sources both in the model (e.g., boundary layer height, vertical mixing, deposition) and in observations (e.g., BC nature) are discussed and quantified, notably through sensitivity tests. Large uncertainty values are determined in our results, which limits the usefulness of the method to rather strongly erroneous emission inventories. A statistically significant (but moderate) overestimation is obtained for the TNO BC emissions and the EMEP and TNO-MP NOx emissions, as well as for the BC / NOx emission ratio in TNO-MP. The benefit of the airborne approach is discussed through a comparison with the BC / NOx ratio at a ground site in Paris, which additionally suggests a spatially heterogeneous error in BC emissions over the agglomeration. © Author(s) 2015.