Regional lead isotope study of a polluted river catchment: River Wear, Northern England, UK

High precision, lead isotope analyses of archived stream sediments from the River Wear catchment, northeast England (1986-88), provide evidence for three main sources of anthropogenic lead pollution; lead mining, industrial lead emissions and leaded petrol. In the upper catchment, pollution is totally controlled and dominated by large lead discharges from historic mining centres in the North Pennine Orefield (²⁰⁸Pb/²⁰⁶Pb, ²⁰⁷Pb/²⁰⁶Pb ratios range from 2.0744-2.0954 and 0.8413-0.8554 respectively). In the lower catchment, co-extensive with the Durham Coalfield and areas of high population density, pollution levels are lower and regionally more uniform. Isotope ratios are systematically higher than in the upper catchment (²⁰⁸Pb/²⁰⁶Pb, ²⁰⁷Pb/²⁰⁶Pb ratios range from 2.0856-2.1397 and 0.8554-0.8896 respectively) and far exceed values determined for the geogenic regional background. Here, the pollution is characterised by the atmospheric deposition of industrial lead and petrol lead. Lead derived from the combustion of coal, although present, is masked by the other two sources. Recent sediments from the main channel of the River Wear are isotopically indistinguishable from older, low order stream sediments of the North Pennine Orefield, indicating that contamination of the river by lead mining waste (up to several 1000 mg/kg Pb at some locations) continues to pose an environmental problem; a pattern that can be traced all the way to the tidal reach. Using within-catchment isotope variation and sediment lead concentrations, estimates can be made of the discharges from discrete mines or groups of mines to the overall level of lead pollution in the River Wear. As well as providing information pertinent to source apportionment and on-going catchment remediation measures, the database is a valuable resource for epidemiologists concerned with the health risks posed by environmental lead.     

Source apportionment of heavy metals and ionic contaminants in rainwater tanks in a subtropical urban area in Australia

Due to prolonged droughts in recent years, the use of rainwater tanks in urban areas has increased in Australia. In order to apportion sources of contribution to heavy metal and ionic contaminants in rainwater tanks in Brisbane, a subtropical urban area in Australia, monthly tank water samples (24 sites, 31 tanks) and concurrent bulk deposition samples (18 sites) were collected during mainly April 2007-March 2008. The samples were analysed for acid-soluble metals, soluble anions, total inorganic carbon and total organic carbon, and characteristics such as total solid and pH. The Positive Matrix Factorisation model, EPA PMF 3.0, was used to apportion sources of contribution to the contaminants. Four source factors were identified for the bulk deposition samples, including ‘crustal matter/sea salt’, ‘car exhausts/road side dust’, ‘industrial dust’ and ‘aged sea salt/secondary aerosols’. For the tank water samples, apart from these atmospheric deposition related factors which contributed in total to 65% of the total contaminant concentration on average, another six rainwater collection system related factors were identified, including ‘plumbing’, ‘building material’, ‘galvanizing’, ‘roofing’, ‘steel’ and ‘lead flashing/paint’ (contributing in total to 35% of the total concentration on average). The Australian Drinking Water Guideline for lead was exceeded in 15% of the tank water samples. The collection system related factors, in particular the ‘lead flashing/paint’ factor, contributed to 79% of the lead in the tank water samples on average. The concentration of lead in tank water was found to vary with various environmental and collection system factors, in particular the presence of lead flashing on the roof. The results also indicated the important role of sludge dynamics inside the tank on the quality of tank water.     

PM10 source apportionment in Milan (Italy) using time-resolved data

In this work Positive Matrix Factorization (PMF) was applied to 4-hour resolved PM10 data collected in Milan (Italy) during summer and winter 2006. PM10 characterisation included elements (Mg-Pb), main inorganic ions (NH₄⁺, NO₃⁻, SO₄²⁻), levoglucosan and its isomers (mannosan and galactosan), and organic and elemental carbon (OC and EC).PMF resolved seven factors that were assigned to construction works, re-suspended dust, secondary sulphate, traffic, industry, secondary nitrate, and wood burning. Multi Linear Regression was applied to obtain the PM10 source apportionment. The 4-hour temporal resolution allowed the estimation of the factor contributions during peculiar episodes, which would have not been detected with the traditional 24-hour sampling strategy.     

Evaluation of chemical indicators for tracking and apportionment of phosphorus sources to Table Rock Lake in Southwest Missouri, USA

This work evaluated the suitability of selected chemical species as indicators for tracking and apportionment of point and non-point phosphorus sources within the Table Rock Lake watershed in Southwest Missouri, USA. The species were evaluated with respect to their uniqueness to specific source types, their ability to be detected in both sources and receiving waters, and the consistency of their concentration ratios to phosphorus. Four sampling events were conducted at 15 sample locations in one year to collect water samples for measuring the concentrations of total and dissolved phosphorus, seven anions, and 19 major and trace elements. Current analytical methods were sensitive enough for quantification of most of the chemical species in both sources and the receiving waterbody. Due to the high seasonal variation of phosphorus concentrations in source samples, no chemical species had consistent concentration ratios to phosphorus across source types. However, several chemicals were found to be unique to specific sources; bromide ion can be used as a unique indicator for the effluent of the largest wastewater treatment plant in the watershed.     

Size distribution and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in aerosol particle samples from the atmospheric environment of Delhi, India

Ambient aerosol particles were collected using a five-stage impactor at six different sites in Delhi. The impactor segregates the TSPM into five different sizes (viz. > 10.9, 10.9-5.4, 5.4-1.6, 1.6-0.7, and < 0.7 μm). Samples collected were chemically analyzed for all the five size ranges, for the estimation of 16 different PAHs. The particle size distribution of PAHs was observed to be unimodal in nature with the highest peak towards the smallest size aerosol particle (< 0.7 μm). The five size ranges were categorized into two broad categories viz. coarse (> 10.9 + 10.9 to 5.4 + 5.4 to 1.6 μm) and fine (1.6 to 0.7 + < 0.7 μm). It was observed that the dominant PAHs found were pyrene, benzo(a)pyrene, benzo(ghi)perylene and benzo(b)fluoranthene for both the coarse and fine fractions. Source apportionment of polycyclic aromatic hydrocarbons (PAHs) has been carried out using principal component analysis method (PCA) in both coarse and fine size modes. The major sources identified in this study, responsible for the elevated concentration of PAHs in Delhi, are vehicular emission and coal combustion. Some contribution from biomass burning was also observed.     

Source apportionment of volatile organic compounds in Hong Kong homes

Indoor volatile organic compound (VOC) data obtained in 100 Hong Kong homes were analyzed to investigate the nature of emission sources and their contributions to indoor concentrations. A principal component analysis (PCA) showed that off-gassing of building materials, household products, painted wood products, room freshener, mothballs and consumer products were the major sources of VOCs in Hong Kong homes. The source apportionments were then evaluated by using an absolute principal component scores (APCS) technique combined with multiple linear regressions. The results indicated that 76.5 ± 1% (average ± standard error) of the total VOC emissions in Hong Kong homes attributes to the off-gassing of building materials, followed by the room freshener (8 ± 4%), household products (6 ± 2%), mothballs (5 ± 3%) and painted wood products (4 ± 2%). Analysis on the source strength in the monitored homes revealed that although six indoor sources were identified and quantified in the Hong Kong homes, only some homes were responsible for the elevated concentrations of target VOCs emitted from these sources. The findings provide us the mechanism of reducing levels of indoor VOCs and ultimately lead to cost effective reduction in population exposures.     

Organic compound characterization and source apportionment of indoor and outdoor quasi-ultrafine particulate matter in retirement homes of the Los Angeles Basin

Abstract Quasi‐ultrafine (quasi‐UF) particulate matter (PM_0.25) and its components were measured in indoor and outdoor environments at four retirement communities in Los Angeles Basin, California, as part of the Cardiovascular Health and Air Pollution Study (CHAPS). The present paper focuses on the characterization of the sources, organic constituents and indoor and outdoor relationships of quasi‐UF PM. The average indoor/outdoor ratios of most of the measured polycyclic aromatic hydrocarbons (PAHs), hopanes, and steranes were close to or slightly lower than 1, and the corresponding indoor–outdoor correlation coefficients (R) were always positive and, for the most part, moderately strong (median R was 0.60 for PAHs and 0.74 for hopanes and steranes). This may reflect the possible impact of outdoor sources on indoor PAHs, hopanes, and steranes. Conversely, indoor n‐alkanes and n‐alkanoic acids were likely to be influenced by indoor sources. A chemical mass balance model was applied to both indoor and outdoor speciated chemical measurements of quasi‐UF PM. Among all apportioned sources of both indoor and outdoor particles, vehicular emissions was the one contributing the most to the PM_0.25 mass concentration measured at all sites (24–47% on average).

Practical Implications

Although people (particularly the elderly retirees of our study) generally spend most of their time indoors, a major portion of the PM_0.25 particles they are exposed to comes from outdoor mobile sources. This is important because, an earlier investigation, also conducted within the Cardiovascular Health and Air Pollution Study (CHAPS), showed that indoor‐infiltrated particles from mobile sources are more strongly correlated with adverse health effects observed in the elderly subjects living in the studied retirement communities compared with other particles found indoors ( Delfino et al., 2008 ).     

Stable lead isotopes in environmental health with emphasis on human investigations

There has been widespread use of stable lead isotopes in the earth sciences for more than 40 years focussed on the origin and age of rocks and minerals with lesser application in environmental investigations where the emphasis has been directed typically to the source of lead in environmental media such as air, water and soils.In contrast, the number of environmental health investigations focussed on humans (and primates) is limited in spite of the demonstrated utility of the approach in pioneering studies in the early 1970's. This paper reviews the status of lead isotopes in human investigations especially over the past 2 decades, the period over which most activity has taken place. Following a brief introduction to the method, examples are provided illustrating the use of lead isotopes in a wide spectrum of activities including sources and pathways of lead in diverse environments from urban to mining communities, various applications associated with pregnancy, the contribution of bone lead to blood lead including in the elderly, the half-life of lead in blood, and lead in bones and other media. A brief outline of critical research on non-human primates is also given. The lead isotope method is a powerful technique for tracing lead and could be employed more widely in human investigations.     

Source apportionment of PM2.5 in Beijing using principal component analysis/absolute principal component scores and UNMIX

Source apportionment of fine particulate matter (PM2.5, i.e., particles with an aerodynamic diameter of 2.5 microm or less) in Beijing, China, was determined using two eigenvector models, principal component analysis/absolute principal component scores (PCA/APCS) and UNMIX. The data used in this study were from the chemical analysis of 24-h samples, which were collected at 6-day intervals in January, April, July, and October 2000 in the Beijing metropolitan area. Both models identified five sources of PM2.5: secondary sulfate and secondary nitrate, a mixed source of coal combustion and biomass burning, industrial emission, motor vehicles exhaust, and road dust. On average, the PCA/APCS and UNMIX models resolved 73% and 85% of the PM2.5 mass concentrations, respectively. The results were comparable to previous estimate using the positive matrix factorization (PMF) and chemical mass balance (CMB) receptor models. Secondary products and the emissions from coal combustion and biomass burning dominated PM2.5. Such comparison among various receptor models, which contain different physical constraints, is important for better understanding PM2.5 sources.     

A lead isotopic study of the human bioaccessibility of lead in urban soils from Glasgow, Scotland

The human bioaccessibility of lead (Pb) in Pb-contaminated soils from the Glasgow area was determined by the Unified Bioaccessibility Research Group of Europe (BARGE) Method (UBM), an in vitro physiologically based extraction scheme that mimics the chemical environment of the human gastrointestinal system and contains both stomach and intestine compartments. For 27 soils ranging in total Pb concentration from 126 to 2160 mg kg^− 1 (median 539 mg kg^− 1), bioaccessibility as determined by the ‘stomach’ simulation (pH ~ 1.5) was 46-1580 mg kg^− 1, equivalent to 23-77% (mean 52%) of soil total Pb concentration. The corresponding bioaccessibility data for the ‘stomach + intestine’ simulation (pH ~ 6.3) were 6-623 mg kg^− 1 and 2-42% (mean 22%) of soil Pb concentration. The soil ²⁰⁶Pb/²⁰⁷Pb ratios ranged from 1.057 to 1.175. Three-isotope plots of ²⁰⁸Pb/²⁰⁶Pb against ²⁰⁶Pb/²⁰⁷Pb demonstrated that ²⁰⁶Pb/²⁰⁷Pb ratios were intermediate between values for source end-member extremes of imported Australian Pb ore (1.04) - used in the manufacture of alkyl Pb compounds (1.06-1.10) formerly added to petrol - and indigenous Pb ores/coal (1.17-1.19). The ²⁰⁶Pb/²⁰⁷Pb ratios of the UBM ‘stomach’ extracts were similar (< 0.01 difference) to those of the soil for 26 of the 27 samples (r = 0.993, p < 0.001) and lower in 24 of them. A slight preference for lower ²⁰⁶Pb/²⁰⁷Pb ratio was discernible in the UBM. However, the source of Pb appeared to be less important in determining the extent of UBM-bioaccessible Pb than the overall soil total Pb concentration and the soil phases with which the Pb was associated. The significant phases identified in a subset of samples were carbonates, manganese oxides, iron-aluminium oxyhydroxides and clays.     

Input characterization of perfluoroalkyl substances in wastewater treatment plants: source discrimination by exploratory data analysis

This paper presents a methodology based on multivariate data analysis for identifying input sources of perfluoroalkyl substances (PFASs) detected in 37 wastewater treatment plants (WWTPs) across more than 40 cities in the state of Minnesota (USA). Exploratory analysis of data points has been carried out by unsupervised pattern recognition (cluster analysis), correlation analysis, ANOVA and per capita discharges in an attempt to discriminate sources of PFASs in WWTPs. Robust cluster solutions grouped the database according to the different PFAS profiles in WWTP influent. Significantly elevated levels of perfluorohexanoic acid (PFHxA), perfluorooctanoic acid (PFOA) and/or perfluorooctane sulfonate (PFOS) in influent have been found in 18 out of 37 WWTPs (49%). A substantial increase in the concentrations of PFHxA and/or PFOA from influent to effluent was observed in 59% of the WWTPs surveyed, suggestive of high concentration inputs of precursors. The fate of one precursor (8:2 fluorotelomer alcohol) in WWTP was modeled based on fugacity analysis to understand the increasing effluent concentration. Furthermore, population-related emissions cannot wholly explain the occurrence and levels of PFASs in WWTPs. Unusually high influent levels of PFASs were observed in WWTPs located in specific industrial areas or where known contamination had taken place. Despite the restriction on the production/use of PFOA and PFOS, this paper demonstrates that wastewater from industrial activities is still a principal determinant of PFAS pollution in urban watersheds.     

Source apportionment of ambient volatile organic compounds in Hong Kong

Volatile organic compounds (VOCs) were measured at four stations with different environments in Hong Kong (HK) during two sampling campaigns. Positive matrix factorization was applied to characterize major VOC sources in HK. Nine sources were identified, and the spatial and seasonal variations of their contributions were derived. The most significant local VOC sources are vehicle and marine vessel exhausts or liquefied petroleum gas (LPG) at different stations. Vehicle- and marine vessel-related sources accounted for 2.9-12.7 ppbv in 2002-2003 and increased to 4.3-15.2 ppbv in 2006-2007. Different from the emission inventory, solvent-related sources only contributed 11- 19% at both sampling campaigns. Therefore, emission control from transport sector should be prioritized to alleviate ambient local VOC levels. Additionally, the contribution of aged VOC, which roughly represents contributions from regional and super-regional transport, also showed moderate increase during the four years, indicating cooperation with environmental authorities in the Pearl River Delta and beyond should be strengthened.All the anthropogenic sources contribute most to Yuen Long and least to Tap Mun. However, Tap Mun exhibited different trends in comparison with the other three stations, especially for sources of vehicle and marine vessel exhausts, LPG and paint solvents. When the local source contributions were incorporated with wind data to derive the directional dependences of sources, we may conclude that the rapid development of Yantian Container Terminal, the associated emissions from marine vessels around the Terminal and the on-site activities were likely responsible for the distinct VOC features at Tap Mun. The current impact from the Terminal is mainly concentrated in the northeastern corner of HK; however, it has the potential threat to other locations if the Terminal continues to expand in such a rapid speed in the coming years. More stringent VOC control measures on activities related to the operation of the Terminal is therefore highly recommended.     

Source apportionment of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of the Huangpu River, Shanghai, China

We applied cluster analysis and principal component analysis (PCA) with multivariate linear regression (MLR) to apportion sources of polycyclic aromatic hydrocarbons (PAHs) in surface sediments of the Huangpu River in Shanghai, China, based on the measured PAH concentrations of 32 samples collected at eight sites in four seasons in 2006. The results indicate that petrogenic and pyrogenic sources are the important sources of PAHs. Further analysis shows that the contributions of coal combustion, traffic-related pollution and spills of oil products (petrogenic) are 40%, 36% and 24% using PCA/MLR, respectively. Pyrogenic sources (coal combustion and traffic related pollution) contribute 76% of anthropogenic PAHs to sediments, which indicates that energy consumption is a predominant factor of PAH pollution in Shanghai. Rainfall, the monsoon and temperature play important roles in the distinct seasonal variation of PAH pollution, such that the contamination level of PAHs in spring is significantly higher than in the other seasons.

Brief

We apportion PAHs in surface sediments of the Huangpu River and show that coal combustion, traffic-related pollution, and petroleum spillage are the major sources.     

Childhood lead exposure and uptake in teeth in the Cleveland area during the era of leaded gasoline

Childhood uptake of lead from exposure to atmospheric leaded gasoline in the United States has been studied using mainly blood lead levels. Since reliable blood lead techniques were used only after the peak use of leaded gasoline, the prior exposure history is unclear. The well-documented decline in blood lead levels after the mid-1970s could represent the continuation of a historic steady decline in exposure from many sources. Alternatively, the post-1970s decline might represent the declining phase of a unimodal rise and fall corresponding closely to usage of leaded gasoline. To assess these possibilities, lead concentration and 207Pb/206Pb isotope ratios were measured in the enamel of permanent molar teeth formed between 1936 and 1993 in mainly African-American donors who grew up in the Cleveland area. Tooth enamel preserves the lead concentration and isotope ratio that prevails during tooth formation. Historical trends in enamel lead concentration were significantly correlated with surrogates of atmospheric lead exposure: lead in sediments of two dated Lake Erie cores, and lead consumed in gasoline. About two-thirds of the total lead uptake into enamel in this period was attributable to leaded gasoline, and the remainder to other sources (e.g. paint). Enamel 207Pb/206Pb isotope ratios were similar to those of one lake sediment. Multivariate analysis revealed significant correlation in neighborhoods with higher levels of traffic, and including lake sediment data, accounted for 53% of the variation in enamel lead levels. Enamel lead concentration was highly correlated with reported African-American childhood blood levels. The extrapolated peak level of 48 μg/dL (range 40 to 63) is associated with clinical and behavioral impairments, which may have implications for adults who were children during the peak gasoline lead exposure. In sum, leaded gasoline emission was the predominant source of lead exposure of African-American Cleveland children during the latter two-thirds of the 20th century.     

Comparison of lead isotopes with source apportionment models, including SOM, for air particulates

We have measured high precision lead isotopes in PM(2.5) particulates from a highly-trafficked site (Mascot) and rural site (Richmond) in the Sydney Basin, New South Wales, Australia to compare with isotopic data from total suspended particulates (TSP) from other sites in the Sydney Basin and evaluate relationships with source fingerprints obtained from multi-element PM(2.5) data. The isotopic data for the period 1998 to 2004 show seasonal peaks and troughs that are more pronounced in the rural site for the PM(2.5).samples but are consistent with the TSP. The Self Organising Map (SOM) method has been applied to the multi-element PM(2.5) data to evaluate its use in obtaining fingerprints for comparison with standard statistical procedures (ANSTO model). As seasonal effects are also significant for the multi-element data, the SOM modelling is reported as site and season dependent. At the Mascot site, the ANSTO model exhibits decreasing (206)Pb/(204)Pb ratios with increasing contributions of fingerprints for "secondary smoke" (industry), "soil", "smoke" and "seaspray". Similar patterns were shown by SOM winter fingerprints for both sites. At the rural site, there are large isotopic variations but for the majority of samples these are not associated with increased contributions from the main sources with the ANSTO model. For two winter sampling times, there are increased contributions from "secondary industry", "smoke", "soil" and seaspray with one time having a source or sources of Pb similar to that of Mascot. The only positive relationship between increasing (206)Pb/(204)Pb ratio and source contributions is found at the rural site using the SOM summer fingerprints, both of which show a significant contribution from sulphur. Several of the fingerprints using either model have significant contributions from black carbon (BC) and/or sulphur (S) that probably derive from diesel fuels and industrial sources. Increased contributions from sources with the SOM summer fingerprints could explain the summer-time peaks in isotopic ratio at both sites and, at the rural site, be associated with meteorological influences. Nevertheless, the SOM results indicate that there are multiple overlapping 'weak' sources.     

A comparison of the isotopic composition of lead in rainwater, surface vegetation and tree bark at the long-term monitoring site, Glensaugh, Scotland, in 2007

The lead concentrations and isotopic ratios (²⁰⁶Pb/²⁰⁷Pb, ²⁰⁸Pb/²⁰⁶Pb, ²⁰⁸Pb/²⁰⁷Pb) of 31 rainwater (September 2006-December 2007) and 11 surface vegetation (moss, lichen, heather) samples (October 2007) from the rural upland catchment of Glensaugh in northeast Scotland and of nine bark samples (October 2007) from trees, predominantly Scots pine, in or near Glensaugh were determined. The mean ²⁰⁶Pb/²⁰⁷Pb ratios for rainwater in 2006 and 2007 were similar to those previously determined for 2000 to 2003 at Glensaugh, yielding an average mean annual value of 1.151 ± 0.005 (± 1 SD) for the period from 2000, when an outright ban on leaded petrol came into force in the UK, to 2007. The mean ²⁰⁶Pb/²⁰⁷Pb ratio (1.146 ± 0.004; n = 7) for surface vegetation near the top (430-450 m) of the catchment was not significantly different (Student's t test) from that of rainwater (1.148 ± 0.017; n = 24) collected over the 12-month period prior to vegetation sampling, but both were significantly different, at the 0.1% (i.e. p < 0.001) and 1% (p < 0.01) level, respectively, from the corresponding mean value (1.134 ± 0.006; n = 9) for the outermost layer of tree bark. When considered in conjunction with similar direct evidence for 2002 and indirect evidence (e.g. grass, atmospheric particulates, dated peat) for recent decades in the Glensaugh area, these findings confirm that the lead isotopic composition of surface vegetation, including that of suitably located moss, reflects that of the atmosphere while that of the outermost layer of Scots pine bark is affected by non-contemporaneous lead. The nature and relative extent of the different contributory sources of lead to the current UK atmosphere in the era of unleaded petrol, however, are presently not well characterised on the basis of lead isotopic measurements.     

Bone lead levels and lead isotope ratios in red grouse from Scottish and Yorkshire moors

Leg and foot bones of adult and juvenile red grouse (Lagopus lagopus scoticus) were collected from hunter-shot birds on two Scottish estates (Glendye and Invermark) and one Yorkshire estate in September, 2003. The lead content of bones was measured by atomic absorption spectrophotometry, and corresponding stable lead isotopes (Pb^{204, 206, 207, 208}) by inductively coupled plasma mass spectrometry. At the Glendye (N = 111) and Invermark (N = 85) estates, relatively few birds (5.4% and 3.5%, respectively) had highly elevated bone lead concentrations (> 20 µg/g dry weight). In bones of these highly exposed birds, a combination of Pb²⁰⁶:Pb²⁰⁷ and Pb²⁰⁸:Pb²⁰⁷ratios was consistent with ingestion of lead gunshot available in Europe. By contrast, Yorkshire grouse experienced a high incidence (65.8%) of bone lead > 20 µg/g. The Pb²⁰⁶:Pb²⁰⁷ and Pb²⁰⁸:Pb²⁰⁷ratios in bones of these highly exposed birds were consistent with a combined exposure to ingested lead gunshot and lead from galena mining in the region. Lead isotope ratios also indicated that lead from UK gasoline combustion and fallout from atmospheric particles was not a likely source of elevated lead in bones of either Scottish or Yorkshire grouse. Suggested management options for the three moors include adopting nontoxic shot for all game shooting on the estates, allowing heather (Calluna vulgaris) vegetation to grow tall in lead shot fall-out zones to reduce physical access to high densities of lead shot already present, and provision of calcareous grit across moors to reduce lead assimilation from all ingested sources of lead.     

Potential source contributions and risk assessment of PAHs in sediments from Taihu Lake, China: comparison of three receptor models

In this work, three receptor models (Principal Component Analysis-Multiple Linear Regression (PCA-MLR) model, Unmix model and Positive Matrix Factorization (PMF) model) were employed to investigate potential source apportionment of PAHs in sediments from Taihu Lake, China. A total of 15 priority PAHs in 29 sediments from Taihu Lake were measured, with ∑PAHs (sum of 15 PAHs) concentrations ranging from 209 to 1003 ng g⁻¹ dw. Source apportionment results derived from three different models were similar, indicating that the highest contribution to ∑PAHs was from vehicular emission (53.6-54.3%), followed by coal combustion (23.8-28.8%) and wood combustion (11.9-16.0%). The contribution of mixed wood and coal combustion source identified by PCA-MLR was 41.3%. For the first time the risk assessment for each identified source category was quantitatively calculated by combining the BaP equivalents (BaPE) values with estimated source contributions. The results showed that vehicular emission posed the highest toxic risk, with BaPE values of 26.9-31.5 ng g⁻¹ dw, and the BaPE values for coal combustion and wood combustion were 6.56-15.6 ng g⁻¹ dw and 2.94-6.11 ng g⁻¹ dw, respectively. The distributions of contribution and BaPE for each identified source category were studied as well, and showed similar trends among the sampling sites, for each source category.     

The identification of lead ammunition as a source of lead exposure in First Nations: the use of lead isotope ratios

The use of lead shotshell to hunt water birds has been associated with lead-contamination in game meat. However, evidence illustrating that lead shotshell is a source of lead exposure in subsistence hunting groups cannot be deemed definitive. This study seeks to determine whether lead shotshell constitutes a source of lead exposure using lead isotope ratios. We examined stable lead isotope ratios for lichens, lead shotshell and bullets, and blood from residents of Fort Albany and Kashechewan First Nations, and the City of Hamilton, Ontario, Canada. Data were analyzed using ANOVA and regression analyses. ANOVA of isotope ratios for blood revealed significant differences with respect to location, but not sex. Hamilton differed from both Kashechewan and Fort Albany; however, the First Nations did not differ from each other. ANOVA of the isotope ratios for lead ammunition and lichens revealed no significant differences between lichen groups (north and south) and for the lead ammunition sources (pellets and bullets). A plot of (206)Pb/(204)Pb and (206)Pb/(207)Pb values illustrated that lichens and lead ammunition were distinct groupings and only the 95% confidence ellipse of the First Nations group overlapped that of lead ammunition. In addition, partial correlations between blood-lead levels (adjusted for age) and isotope ratios revealed significant (p<0.05) positive correlations for (206)Pb/(204)Pb and (206)Pb/(207)Pb, and a significant negative correlation for (208)Pb/(206)Pb, as predicted if leaded ammunition were the source of lead exposure. In conclusion, lead ammunition was identified as a source of lead exposure for First Nations people; however, the isotope ratios for lead shotshell pellets and bullets were indistinguishable. Thus, lead-contaminated meat from game harvested with lead bullets may also be contributing to the lead body burden.     

Temporal trend and source apportionment of water pollution in different functional zones of Qiantang River, China

The increasingly serious river water pollution in developing countries poses great threat to environmental health and human welfare. The assignment of river function to specific uses, known as zoning, is a useful tool to reveal variations of water environmental adaptability to human impact. Therefore, characterizing the temporal trend and identifying responsible pollution sources in different functional zones could greatly improve our knowledge about human impacts on the river water environment. The aim of this study is to obtain a deeper understanding of temporal trends and sources of water pollution in different functional zones with a case study of the Qiantang River, China. Measurement data were obtained and pretreated for 13 variables from 41 monitoring sites in four categories of functional zones during the period 1996-2004. An exploratory approach, which combines smoothing and non-parametric statistical tests, was applied to characterize trends of four significant parameters (permanganate index, ammonia nitrogen, total cadmium and fluoride) accounting for differences among different functional zones identified by discriminant analysis. Aided by GIS, yearly pollution index (PI) for each monitoring site was further mapped to compare the within-group variations in temporal dynamics for different functional zones. Rotated principal component analysis and receptor model (absolute principle component score-multiple linear regression, APCS-MLR) revealed that potential pollution sources and their corresponding contributions varied among the four functional zones. Variations of APCS values for each site of one functional zone as well as their annual average values highlighted the uncertainties associated with cross space-time effects in source apportionment. All these results reinforce the notion that the concept of zoning should be taken seriously in water pollution control. Being applicable to other rivers, the framework of management-oriented source apportionment is thus believed to have potentials to offer new insights into water management and advance the source apportionment framework as an operational basis for national and local governments.