Single-particle analysis of industrial emissions brings new insights for health risk assessment of PM
Introduction
In developed countries, the concentration of particulate matter (PM) of industrial origin in the atmosphere has considerably decreased thanks to regulation policy (EU Directive, 2008). However, an increase of respiratory diseases has been noticed and reported to be linked to fine and ultrafine particles, especially in large cities (Donaldson and MacNee, 2001, Garcia-Chevesich et al., 2014, Jorquera and Barraza, 2012, Mehta et al., 2013, Tao et al., 2014). The recycling activity of metal-containing materials is one of the significant industrial particle sources which impact the air quality of highly populated urban areas (Johnson et al., 2007). The regulation of industrial emissions and the improvement of the filter efficiencies have reduced the total amount and the average size of the metal-rich particles emitted into the atmosphere (Nair et al., 2010), but significant levels of fine and ultrafine metal-rich particles are still observed in industrial and urban areas (Bu-Olayan and Thomas, 2009, Harrison and Yin, 2010, Kumar et al., 2013, Moreno et al., 2010, Pöschl, 2010, Sanderson et al., 2014, Zhang et al., 2005). It is now well established that the finest fraction of particulate matter, with an aerodynamic diameter smaller than 1 μm (PM1), is more hazardous for human health than PM10 and PM2.5 (Brook et al., 2002, Nel et al., 2006, Perrone et al., 2010, Polichetti et al., 2009, Sammut et al., 2008, Sammut et al., 2010). For humans, beside the risk related to the ingestion of particles, inhalation of particles is an important exposure pathway of metal contamination (Perrone et al., 2010, Polichetti et al., 2009, Sammut et al., 2010). Inhalation of metal-containing PM in ambient air is associated with adverse health effects, even at concentrations near or not much higher than current ambient levels (Kelly and Fussell, 2012, Kelly and Fussell, 2015). Risk assessment simulations provided by the health protection agencies consider only the particle mass level (i.e. PM10, PM2.5 or PM1) and bulk metal contents within the samples, but not the solubility, the speciation, size and chemical heterogeneity of particles, although it is now well established that these parameters control the toxicity of the particles (Charrier and Anastasio, 2011, Ettler et al., 2005, Ruby et al., 1996, Sammut et al., 2010, Sauvain et al., 2011, Uzu et al., 2011a, Wang et al., 2013). For example, Adamson et al. (2000) demonstrated that less soluble forms of Zn-rich particles (e.g. zinc sulfate) are less toxic than more soluble forms (e.g. zinc chloride). However, the relevance of water-soluble versus insoluble species of metals within PM remains unclear (Kelly and Fussell, 2012, Kelly and Fussell, 2015). Therefore, metal speciation of particles contributes much more to the understanding of the health risk of PM than bulk concentration (Fernandez et al., 2000, Lock and Janssen, 2001, Popescu et al., 2013, Sammut et al., 2010, Schreck et al., 2011). As an example, we have previously investigated the composition and the toxicity of particles collected within a lead-acid battery recycling facility located in a French urban area (Uzu et al., 2009, Uzu et al., 2011b). Since 2009, the Pb level in the atmosphere measured near this plant has been lower than the regulated value of 0.25 μg m−3 (ORAMIP, 2011). However, these particles have a significant inherent oxidant potential and can induce inflammatory effects, especially the PM1 emitted from furnace and refining emissions (Uzu et al., 2011a). The particles collected inside the working places of the facility and in channeled emission have been characterized in detail, whereby it was suggested that the species and compositions of individual particles would explain the adverse health effects (Uzu et al., 2011b).
Single-particle analysis employing scanning electron microscopy coupled with energy dispersive X-ray spectrometer (SEM-EDX), Raman microspectrometry (RMS) and/or FTIR microscopy is a powerful analytical methodology for PM characterization which provides information on morphology, elemental and molecular compositions of single particles, and thus more detailed information on chemical compositions of the samples, as widely demonstrated in the literature (Eom et al., 2013, Geng et al., 2011, Jung et al., 2014, Kim et al., 2009, Maskey and Ro, 2011, Sobanska et al., 2006, Sobanska et al., 2014, Ault and Axson, 2017).
In the present work, multiple single particle analytical techniques were utilized to characterize both PM10-1 and PM1-0.1 particles collected in the courtyard of a lead battery recycling facility, so as to provide a better understanding of the oxidant potential and inflammatory effects of these particles. Individual particles were investigated using SEM-EDX and RMS. The surface composition of particles is of high concern as it may govern the particle solubility linked to the metal toxicity, and thus the surface characterization of particles was performed with time-of-flight secondary ion mass spectrometry (ToF-SIMS). Molecular composition is discussed in the context of exposure risk assessment. This last point aims at evidencing that environmental policies need to be improved.
Section snippets
Particle sampling
The sampling was performed in the courtyard of a lead batteries recycling facility in the urban area of Toulouse, France (43°38′12,139″N, 1°25′36,516″E). Three units working at different stages of the recycling process are identified in the plant: (i) the battery grinding unit where battery components are separated under wet conditions, (ii) the smelter where lead pastes are processed in rotary furnaces at 1200 °C and finally (iii) the refinery where lead is purified from unwanted metals or
Variability in the abundances and size distributions of the particles in ambient air
The average number size distributions of the particles derived from particle number concentration (PNC) and lead-containing particle number concentration (PNC-Pb) (see experimental section) is shown in Fig. 1a. A quasi-unimodal size distribution of the overall particles was observed at an average diameter of 0.9 μm and 75 ± 4% of the particles are encountered between 0.3 and 2.5 μm. The result is consistent with the previous work showing that 90% of the particles from channeled (chimney stacks)
Short time chemical evolution of the particles
Although collected at different periods, the characterization results for particles collected at the courtyard agreed well with those for particles collected at the working places of the lead battery recycling facility (Uzu et al., 2009, Uzu et al., 2011b). This reflects a good representativeness of the particle compositions over the time. In this work, the size segregation of lead-containing particles with ball and needle shape morphologies was clearly evidenced in PM1-0.1 when particles were
Conclusions
The present study evidences the Pb enrichment in the finest fraction of the particles (PM1-0.1) collected in the ambient air at the courtyard of a lead recycling plant. The particle compositions differed from the PM compositions at the emission sources, i.e., inside the working places and in the channeled emissions. The collected particles were mainly composed of lead sulfates mixed with iron oxides and sodium sulfates, and were coated with Cl-rich species. These Cl-rich species are more
Acknowledgements
This work is a part of the IRENI program, supported by the Nord Pas-de-Calais Regional Council and by the European Regional Development Fund. This work was also supported by the PHC STAR program (N°29934K) and by Basic Science Research Programs through the National Research Foundation of Korea (NRF) funded by the Ministry of Education, Science and Technology (NRF-2015R1A2A1A09003573). The LASIR and PC2A are included in the Labex CaPPA (ANR-11-LABX-0005-01). The authors thank P. Recourt for
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