In this work, the source of ambient particulate matter (PM10) collected over a one-year period at an urban background site in Lens (France) was determined and investigated using a positive matrix factorization receptor model (US EPA PMF v3.0). In addition, a potential source contribution function (PSCF) was performed by means of the Hybrid Single-Particle Lagrangian Integrated Trajectory (Hysplit) v4.9 model to assess prevailing geographical origins of the identified sources. A selective iteration process was followed for the qualification of the more robust and meaningful PMF solution. Components measured and used in the PMF included inorganic and organic species: soluble ionic species, trace elements, elemental carbon (EC), sugar alcohols, sugar anhydride, and organic carbon (OC). The mean PM10 concentration measured from March 2011 to March 2012 was about 21 μg m−3 with typically OM, nitrate and sulfate contributing to most of the mass and accounting respectively for 5.8, 4.5 and 2.3 μg m−3 on a yearly basis. Accordingly, PMF outputs showed that the main emission sources were (in decreasing order of contribution) secondary inorganic aerosols (28% of the total PM10 mass), aged marine emissions (19%), with probably predominant contribution of shipping activities, biomass burning (13%), mineral dust (13%), primary biogenic emissions (9%), fresh sea salts (8%), primary traffic emissions (6%) and heavy oil combustion (4%). Significant temporal variations were observed for most of the identified sources. In particular, biomass burning emissions were negligible in summer but responsible for about 25% of total PM10 and 50% of total OC in wintertime. Conversely, primary biogenic emissions were found to be negligible in winter but to represent about 20% of total PM10 and 40% of total OC in summer. The latter result calls for more investigations of primary biogenic aerosols using source apportionment studies, which quite usually disregard this type of source. This study further underlines the major influence of secondary processes during daily threshold exceedances. Finally, apparent discrepancies that could be generally observed between filter-based studies (such as the present one) and aerosol mass spectrometer-based PMF analyses (organic fractions) are also discussed.

Precise Si isotopic fractionation in silica (quartz), opal (diatomite, sponges) and standards have been determined employing a Nu Instruments Plasma multicollector inductively coupled plasma mass spectrometer (MC-ICP-MS) in dry plasma mode, using a Cetac Aridus desolvating nebulization system. Variations in sample ²⁸Si/²⁹Si ratios are expressed as δ²⁹Si units, which represent deviations in ‰ from the same ratio of the NBS28 standard measured using the standard-sample bracketing technique. We measured Mg isotopes in dynamic mode for adequate correction of instrumental mass bias, applying the fractionation exponential law and external normalisation. The repeatability and the internal precision on the δ²⁹Si measurements of a 1 ppm Si solution in diluted HF/HCl is better than ±0.1‰ (±2 σ). The accuracy has been assessed by cross analyses of an in-house standard with the laser fluorination-isotope ratio mass spectrometry (IRMS). The dry plasma methodology improves the sensitivity more than ten times compared to wet plasma MC-ICP-MS and hence is of great relevance regarding environmental, biogeochemical and geological sciences where Si isotopes open up a range of new studies.

The research presented here was initiated to improve the current knowledge on easily released metals from atmospheric particles. The objectives of this paper were to develop an in vitro method to estimate lung bioaccessibility and to provide quantitative data on metals bioaccessibility. A large set of metals has been investigated (Ba, Cd, Ce, Co, Cu, La, Mn, Mo, Ni, Pb, Rb, Sb and Zn) using two distinct fluids (water and Gamble solution) on four reference materials representing different types of particle sources. Through this study, different parameters such as extraction-time, composition of the leaching solution and solid-to-liquid (S/L) ratios were investigated. The findings obtained for four SRMs suggest that the bioaccessibility is maximized after a 24 h extraction for a range of S/L ratios varying from 1/500 to 1/50 000. We clearly demonstrate that the higher bioaccessibility of metals is obtained with the Gamble solution. Moreover, our results imply that bioaccessibility is speciation and element dependent with percentages varying from 3.3% for Pb to 92.5% for Zn. An estimation of uncertainties of 11% to 30% was obtained for metals bioaccessibility in the four reference materials. In addition, the extraction procedure was validated by performing a mass balance on both soluble and insoluble fractions. This developed method may be used to evaluate the pulmonary bioaccessibility of trace elements present in the atmospheric particles without major artefacts.