The quality of the urban environment is of growing concern as its human population continues to dramatically increase. X-ray absorption spectroscopy (XAS) and SEM have been used to study the solid-phase speciation of Pb in urban road dust sediments (RDS) in Manchester, UK. XANES analysis and linear combination modeling indicate that PbCrO(4) and Pb-sorbed goethite occur in 1000-500 microm, 250-125 microm, 63-38 microm, and <38 microm size fractions, collectively representing between 51-67% of the contributing Pb-phases. XANES analysis suggests that PbO, PbCl2, and Pb carbonates are also present. EXAFS modeling for all grain size fractions gives best fit models with a first shell of two oxygen atoms at 2.29-2.32 A, which corroborate the possible presence of Pb-sorbed goethite, and also suggest the presence of Pb phosphates and Pb oxides. Second shell Pb-Fe and second and third shell Pb-Pb scattering distances confirm Pb-sorbed to Fe oxide, and PbCl2 and PbCrO4, respectively. Many of the XAS models are corroborated by SEM observations. The Pb-phases may pose a risk to human health if inhaled or ingested, with insoluble phases such as PbCrO4 potentially causing inflammation in the lungs, and soluble phases such as PbO potentially being the most bioaccessible in the digestive tract.
Whilst vehicular and industrial contributions to the airborne particulate budget are well explored, the input due to building demolition is relatively unknown. Air quality is of importance to human health, and it is well known that composition of airborne particles can have a significant influence on both chronic and acute health effects. Road dust (RD) was collected before and after the demolition of a large building to elucidate changes in elemental profile. Rainfall and PM10 mass concentration data aided interpretation of the elemental data. Quantification of Al, As, Ba, Ca, Cd, Cr, Cu, Fe, K, Mg, Mn, Na, Ni, Pb, Rh, S, Si, Sn, Ti, V and Zn was carried out. It was found that only Al, K, Mg, Si and S increased in concentration across all size fractions after the building demolition. Risk assessment was then carried out on elements with applicable reference dose values to assess the potential health risks due to the demolition. Significant risk to children was observed for chromium and aluminium exposure. PM10, monitored 40 metres from the demolition site, indicated no abnormal concentrations during the demolition; however, rainfall data were shown to affect the concentration of PM10. The elemental data observed in this study could possibly indicate the role of increased sulphur concentrations (in this case as a result of the demolition) on the buffer capacity of RD, hence leaching metals into rainwater.
ABSTR ACT X-ray absorption spectroscopy, scanning electron microscopy (SEM) and X-ray diffractometry (XRD) have been used to study the solid-phase speciation of Zn in urban road dust sediments (RDS) in Manchester, UK. X-ray absorption near-edge structure (XANES) analysis using linear combination modelling suggest that the soluble species Zn(NO 3 ) 2 ·6H 2 O and ZnCl 2 represent 70À83%, and Zn-sorbed goethite 17À30%, of the Zn species present. The presence of goethite is not corroborated by extended X-ray absorption fine structure (EXAFS) modelled first shell scattering ZnÀO distances of 2.01À2.03 Å , but this may be due to distortion of the Zn octahedra on the goethite surface, or the existence of Zn-sorbed species with other metal hydrous oxides, as inferred by the EXAFS-modelled second shell Fe and Al scatterers. Analysis by EXAFS also suggests that metallic Zn-Cu-Sn-Pb and Zn-silicate phases are present in the RDS, and this is corroborated by SEM and XRD. Other phases suggested by EXAFS include ZnO, franklinite, Zn-sorbed birnessite and zinc formate. Differences between the XANES and other results suggest that model compounds such as Zn-bearing phyllosilicates and metallic Zn phases may have been missing from the XANES fitting. Long-term low-level exposure to the RDS Zn phases identified may lead to an increased risk of cardiovascular or pulmonary diseases.
It is well documented that a large portion of urban particulate matters is derived from road dust. Isolating particles of RD which are small enough to be inhaled, however, is a difficult process. In this study, it is shown for the first time that the\ 38 lm fraction of road dust particles can be used as a proxy for road dust particles \ 10 lm in bioaccessibility studies. This study probed similarities between the \ 10 and \ 38 lm fractions of urban road dust to show that the larger of the two can be used for analysis for which larger sample masses are required, as is the case with in vitro analysis. Road dust, initially segregated to size \ 38 lm using sieves, was again size segregated to \ 10 lm using water deposition. Both the original \ 38 lm and the separated \ 10 lm fractions were then subject to single particle analysis by SEM-EDX and bulk analysis by ICP-OES for its elemental composition. Dissolution tests in artificial lysosomal fluid, representative of lung fluid, were carried out on both samples to determine % bioaccessibility of selected potentially harmful elements and thus probe similarities/differences in in vitro behaviour between the two fractions. The separation technique achieved 94.3% of particles \ 10 lm in terms of number of particles (the original sample contained 90.4% as determined by SEM-EDX). Acid-soluble metal concentration results indicated differences between the samples. However, when manipulated to negate the input of Si, SEM-EDX data showed general similarities in metal concentrations. Dissolution testing results indicated similar behaviour between the two samples in a simulated biological fluid.
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