Development of lead source-specific exposure standards based on aggregate exposure assessment: Bayesian inversion from biomonitoring information to multipathway exposure

Exposure of children to lead is of great concern, and the exposure standards for different media are important for protecting public safety. However, these media-specific standards often fail to ensure the safety of children even when environmental lead levels are lower than the quality standards since humans are often exposed to lead via multiple pathways. To establish exposure standards to protect children from hazards associated with exposure to lead, an analytical tool for assessing aggregate exposure to lead based on Bayesian hierarchical model was developed, and then was used to update the external lead exposure of diet, paint, soil, air and drinking water using the blood lead levels in Chinese children aged 1-6 years. On the basis of updated external exposure, the source allocations for diet, paint, soil, air, and drinking water in China were 65.80 ± 7.92%, 16.98 ± 7.88%, 13.65 ± 5.05%, 3.36 ± 1.75%, and 0.20 ± 0.14%, respectively. Based on the estimated source allocations, the exposure standards were evaluated to be 0.2 μg/m(3), 24.25 mg/kg, 0.027 μg/L, 0.051 μg/mg, 0.042 μg/mg, 38.02 μg/mg for air, soil, water, grains, vegetables, and paint, respectively. Since the standards setting procedure was based on the multipathway aggregate exposure assessment of lead, the newly proposed exposure standards should ensure the safety of children.     

Pollutant concentrations within households in Lao PDR and association with housing characteristics and occupants' activities

The paper presents the results of a study conducted to investigate indoor air quality within residential dwellings in Lao PDR. Results from PM(10), CO, and NO(2) measurements inside 167 dwellings in Lao PDR over a five month period (December 2005-April 2006) are discussed as a function of household characteristics and occupant activities. Extremely high PM(10) and NO(2) concentrations (12 h mean PM(10) concentrations 1275 ± 98 μg m(-3) and 1183 ± 99 μg m(-3) in Vientiane and Bolikhamxay provinces, respectively; 12 h mean NO(2) concentrations 1210 ± 94 μg m(-3) and 561 ± 45 μg m(-3) in Vientiane and Bolikhamxay, respectively) were measured within the dwellings. Correlations, ANOVA analysis (univariate and multivariate), and linear regression results suggest a substantial contribution from cooking and smoking. The PM(10) concentrations were significantly higher in houses without a chimney compared to houses in which cooking occurred on a stove with a chimney. However, no significant differences in pollutant concentrations were observed as a function of cooking location. Furthermore, PM(10) and NO(2) concentrations were higher in houses in which smoking occurred, suggestive of a relationship between increased indoor concentrations and smoking (0.05 < p < 0.10). Resuspension of dust from soil floors was another significant source of PM(10) inside the house (634 μg m(-3), p < 0.05).     

烧鸡油炸烟气中PM2.5浓度及有害物质含量的测定

测定了烧鸡在油炸期间产生的炯气 中PM25、甲醛的质量浓度及烟气颗粒物中有害成分3,4-苯并芘、杂环胺类化合物的含量.结果表明:油炸烟气中PM25最高检出质量浓度为2440μ.g/m3,甲醛最高检出质量浓度为0.270mg/m3,分别超过我国窄气质量标准中PM25二级质量浓度限值(75μg/m3)和大气污染物排放标准中甲醛排放限值(0.20mg/m3)的31.5倍和0.35倍;PM25颗粒物中3,4-苯并芘检出含量为18.35～30.68μ.g/g,杂环胺检出含量14.87～37.72μg/g.     

Use of personal-indoor-outdoor sulfur concentrations to estimate the infiltration factor and outdoor exposure factor for individual homes and persons

A study of personal, indoor, and outdoor exposure to PM2.5 and associated elements has been carried out for 37 residents of the Research Triangle Park area in North Carolina. Participants were selected from persons expected to be at elevated risk from exposure to particles, and included 29 persons with hypertension and 8 cardiac patients with implanted defibrillators. Participants were monitored for 7 consecutive days in each of four seasons. One goal of the study was to estimate the contribution of outdoor PM2.5 to indoor concentrations. This depends on the infiltration factor Finf, the fraction of outdoor PM2.5 remaining airborne after penetrating indoors. After confirming with our measurements the findings of previous studies that sulfur has few indoor sources, we estimated an average Finf for each house based on indoor/outdoor sulfur ratios. These estimates ranged from 0.26 to 0.87, with a median value of 0.55. Since these estimates apply only to particles of size similar to that of sulfur particles (0.06-0.5 microm diameter), and since larger particles (0.5-2.5 microm) have lower penetration rates and higher deposition rates, these estimates are likely to be higher than the true infiltration factors for PM2.5 as a whole. In summer when air conditioners were in use, the sulfur-based infiltration factor was at its lowest (averaging 0.50) for most homes, whereas the average Finf for the other three seasons was 0.62-0.63. Using the daily estimated infiltration factor for each house, we calculated the contribution of outdoor PM2.5 to indoor air concentrations. The indoor-generated contributions to indoor PM2.5 had a wider range (0-33 microg/m3) than the outdoor contributions (5-22 microg/m3). However, outdoor contributions exceeded the indoor-generated contributions in 27 of 36 homes. A second goal of the study was to determine the contribution of outdoor particles to personal exposure. This is determined by the "outdoor exposure factor" Fpex, the fraction of outdoor PM2.5 contributing to personal exposure. As with Finf, we estimated Fpex by the personal/outdoor sulfur ratios. The estimates ranged from 0.33 to 0.77 with a median value of 0.53. Outdoor air particles were less important for personal exposures than for indoor concentrations, with the median outdoor contribution to personal exposure just 49%. We regressed the outdoor contributions to personal exposures on measured outdoor PM2.5 at the central site. The regressions had R2 values ranging from 0.19 to 0.88 (median = 0.73). These values provide an indication of the extent of misclassification error in epidemiological estimates of the effect of outdoor particles on health.     

Development and in-home testing of the Pretoddler Inhalable Particulate Environmental Robotic (PIPER Mk IV) sampler

Exposure and dose estimation are essential to understanding the etiology of environmentally linked childhood diseases. The behavior of resuspended particulate matter (PM) suggests that stationary measurements may underestimate household exposures in young children (ages 6-36 months). Because of the size and weight of the sampling equipment, use of personal samplers in this age group is either difficult or impossible. The Pretoddler Inhalable Particulate Environmental Robotic (PIPER Mk IV) sampler has been developed to provide a surrogate method to ascertain personal exposures to PM for this age group. As part of a study of childhood asthma, 55 homes in central New Jersey were tested. Simultaneous sampling for inhalable PM using stationary (110 cm height) and PIPER mobile sampler were carried out. In homes with bare floors (N=21), the absolute difference was 3.9 μg/m3 (SE=3.01; p=0.217) and relative difference (PIPER/Stationary) was 1.12 (linearized SE=0.11). On carpets (N=34), the absolute difference was 54.1 μg/m3 (SE=13.50; p=0.0003), and the relative difference was 2.30 (linearized SE=0.34). The results confirm the importance of understanding the personal dust cloud caused by children's activity in a room, particularly when rugs or carpets are present.     

Carbon monoxide as a tracer for assessing exposures to particulate matter in wood and gas cookstove households of highland Guatemala

Kitchen-area 22-h gravimetric PM2.5 and passive diffusion stain-tube carbon monoxide (CO) concentrations were measured in homes with open fire and improved wood cookstoves in two studies. In the first study (Guat-2), which also studied homes with gas cookstoves, three samples were collected per stove condition from each of three test houses. In the second study (Guat-3), one sample was collected per house from 15 open fire and 25 improved-stove houses. CO personal samples were also taken for mother and child in both studies. Spearman correlation coefficients (R) between kitchen-area CO and PM2.5 levels in homes using open fires or impoved wood cookstoves were high ranging from 0.92 (Guat-2) to 0.94 (Guat-3), as were those between the personal samples for mother and child ranging from 0.85 (Guat-3) to 0.96 (Guat-2). In general, the correlations were lower for less-polluted conditions. The study found that CO is a good proxy for PM2.5 in homes using open fires or planchas (improved wood cookstove with chimney) but not under gas stove use conditions. It also determined that mother personal CO is a good proxy for child's (under 2 years of age) personal CO and that area CO measurements are not strongly representative of personal CO measurements. These results generally support the use of Draeger CO passive diffusion tubes as a proxy for PM2.5 in such cases where a single type of emission source is the predominant source for CO and PM2.5.     

Optical remote sensing to quantify fugitive particulate mass emissions from stationary short-term and mobile continuous sources: part II. Field applications

Quantification of emissions of fugitive particulate matter (PM) into the atmosphere from military training operations is of interest by the United States Department of Defense. A new range-resolved optical remote sensing (ORS) method was developed to quantify fugitive PM emissions from puff sources (i.e., artillery back blasts), ground-level mobile sources (i.e., movement of tracked vehicles), and elevated mobile sources (i.e., airborne helicopters) in desert areas that are prone to generating fugitive dust plumes. Real-time, in situ mass concentration profiles for PM mass with particle diameters <10 μm (PM(10)) and <2.5 μm (PM(2.5)) were obtained across the dust plumes that were generated by these activities with this new method. Back blasts caused during artillery firing were characterized as a stationary short-term puff source whose plumes typically dispersed to <10 m above the ground with durations of 10-30 s. Fugitive PM emissions caused by artillery back blasts were related to the zone charge and ranged from 51 to 463 g PM/firing for PM(10) and 9 to 176 g PM/firing for PM(2.5). Movement of tracked vehicles and flying helicopters was characterized as mobile continuous sources whose plumes typically dispersed 30-50 m above the ground with durations of 100-200 s. Fugitive PM emissions caused by moving tracked vehicles ranged from 8.3 to 72.5 kg PM/km for PM(10) and 1.1 to 17.2 kg PM/km for PM(2.5), and there was no obvious correlation between PM emission and vehicle speed. The emission factor for the helicopter flying at 3 m above the ground ranged from 14.5 to 114.1 kg PM/km for PM(10) and 5.0 to 39.5 kg PM/km for PM(2.5), depending on the velocity of the helicopter and type of soil it flies over. Fugitive PM emissions by an airborne helicopter were correlated with helicopter speed for a particular soil type. The results from this range-resolved ORS method were also compared with the data obtained with another path-integrated ORS method and a Flux Tower method.     

Estimation of size-resolved ambient particle density based on the measurement of aerosol number, mass, and chemical size distributions in the winter in beijing

Simultaneous measurements of aerosol size, distribution of number, mass, and chemical compositions were conducted in the winter of 2007 in Beijing using a Twin Differential Mobility Particle Sizer and a Micro Orifice Uniform Deposit Impactor. Both material density and effective density of ambient particles were estimated to be 1.61 ± 0.13 g cm(-3) and 1.62 ± 0.38 g cm(-3) for PM(1.8) and 1.73 ± 0.14 g cm(-3) and 1.67 ± 0.37 g cm(-3) for PM(10). Effective density decreased in the nighttime, indicating the primary particles emission from coal burning influenced the density of ambient particles. Size-resolved material density and effective density showed that both values increased with diameter from about 1.5 g cm(-3) at the size of 0.1 μm to above 2.0 g cm(-3) in the coarse mode. Material density was significantly higher for particles between 0.56 and 1.8 μm during clean episodes. Dynamic Shape Factors varied within the range of 0.95-1.13 and decreased with particle size, indicating that coagulation and atmospheric aging processes may change the shape of particles.     

Source contributions to atmospheric gases and particulate matter in the southeastern United States

A new approach for determining the contributions of emission sources to concentrations of particulate matter and gases is developed using the chemical mass balance (CMB) method and the U.S. EPA's National Emission Inventory (NEI). The approach apportions combined gas-phase and condensed-phase concentrations of individual compounds as well as PM(2.5) mass. Because the NEI is used to provide source emission profiles for CMB analysis, the method generates information on the consistency of the NEI with ambient monitoring data. The method also tracks secondary species to primary source emissions, permitting a more complete accounting of the impact of aggregated source types on PM(2.5) mass concentrations. An example application is presented using four years of monitoring data collected at eight sites in the Southeastern Aerosol Research and Characterization (SEARCH) network. Including both primary and secondary species, area sources contributed 2.0-3.7 μg m(-3) (13-26%), point sources contributed 3.0-4.6 μg m(-3) (22-33%), and mobile sources contributed 1.0-6.0 μg m(-3) (9-42%) to mean PM(2.5) mass concentrations. Whereas the NEI generally accounts for the ambient concentrations of gases and particles, certain anomalies are identified, especially related to carbonaceous compounds and dust.     

Waterpipe-associated particulate matter emissions.

Waterpipe tobacco smoking is increasingly common worldwide, and evidence about its harmful effects to smokers is emerging. However, no studies have investigated the potential exposure of nonsmokers to waterpipe smoke. We measured particulate matter (PM) emissions (PM2.5, PM10) before and during laboratory sessions in which 20 individuals used a waterpipe to smoke tobacco and 20 individuals smoked a cigarette (10 for each particle-size/smoking-method), as well as 10 waterpipe and 10 cigarette smoldering sessions (i.e., without a smoker). A TSI-SidePak aerosol monitor obtained PM2.5, PM10 background, smoking, and maximum levels. Mean PM2.5 rose 447% for waterpipe (from 48 microg/m3 background to 264 microg/m3 smoking), and by 501% for cigarettes (from 44 microg/m3 to 267 microg/m3), whereas mean PM10 rose by 563% for waterpipe (from 55 microg/m3 to 365 microg/m3), and by 447% for cigarettes (from 52 microg/m3 to 287 microg/m3) (p<.05 for all). The increase in PM during cigarette smoking was due primarily to PM2.5, given that the proportion of PM2.5 from total PM10 increase was 95% compared with 70% for waterpipe (p<.05). Maximum PM2.5 was 908 microg/m3 for waterpipe and 575 microg/m3 for cigarettes, whereas maximum PM10 was 1052 microg/m3 for waterpipe and 653 microg/m3 for cigarettes. Mean PM2.5 and PM10 smoldering levels did not differ from background for waterpipe but were significantly higher for cigarettes (PM2.5: 33-190 microg/m3; PM10: 42-220 microg/m3). Policymakers considering clean air regulations should include waterpipe tobacco smoking, and the public should be warned about this source of smoke exposure.     

PM2.5 of ambient origin: estimates and exposure errors relevant to PM epidemiology

Epidemiological studies routinely use central-site particulate matter (PM) as a surrogate for exposure to PM of ambient (outdoor) origin. Below we quantify exposure errors that arise from variations in particle infiltration to aid evaluation of the use of this surrogate, rather than actual exposure, in PM epidemiology. Measurements from 114 homes in three cities from the Relationship of Indoor, Outdoor and Personal Air (RIOPA) study were used. Indoor PM2.5 of outdoor origin was calculated as follows: (1) assuming a constant infiltration factor, as would be the case if central-site PM were a "perfect surrogate" for exposure to outdoor particles; (2) including variations in measured air exchange rates across homes; (3) also incorporating home-to-home variations in particle composition, and (4) calculating sample-specific infiltration factors. The final estimates of PM2.5 of outdoor origin take into account variations in building construction, ventilation practices, and particle properties that result in home-to-home and day-to-day variations in particle infiltration. As assumptions became more realistic (from the first, most constrained model to the fourth, least constrained model), the mean concentration of PM2.5 of outdoor origin increased. Perhaps more importantly, the bandwidth of the distribution increased. These results quantify several ways in which the use of central site PM results in underestimates of the ambient PM2.5 exposure distribution bandwidth. The result is larger uncertainties in relative risk factors for PM2.5 than would occur if epidemiological studies used more accurate exposure measures. In certain situations this can lead to bias.     

Urinary methoxyphenol biomarkers and woodsmoke exposure: comparisons in rural Guatemala with personal CO and kitchen CO, levoglucosan, and PM2.5

Urinary methoxyphenols have been proposed as biomarkers for woodsmoke exposure, but few field studies have been undertaken. We evaluated these biomarkers for assessing the exposure to woodsmoke of householders in rural Guatemala. The study population was a subset (10 female cooks, 2 female non-cooks, and 8 male non-cooks ranging in age from 7 to 60) drawn from those participating in a longterm randomized intervention trial (RESPIRE) in the highlands. All households rely solely on woodburning for cooking and home heating. Approximately half of the homes in the trial used open woodfires in the home, while the intervention group used cookstoves, called "planchas, "that vent most of the woodsmoke outdoors through a chimney. Corrected for creatinine levels, 16 of the 19 methoxyphenols measured were lower in the urine of cooks using the plancha; and 11 of the 19 compounds were lower in the urine of non-cooks from homes using the plancha. Furthermore, the 4 low-molecular-weight syringyl methoxyphenols (syringol, methysyringol, ethylsyringol, propylsyringol) were each moderately correlated (r2 = 0.71,0.64, 0.68, 0.53 respectively, with all p < 0.05) with personal exposure measurements determined by carbon monoxide (CO) passive diffusion tubes, but not with CO in exhaled breath. 48-Hour kitchen area measurements of PM2.5 mass, PM2.5 levoglucosan, and CO were highly correlated (>0.89) with each other and moderately correlated (0.54-0.78) with personal CO measurements. Although based on relatively few measurements, this study demonstrates that the urinary concentrations of specific methoxyphenols may be effective biomarkers of short-term exposures to inhaled woodsmoke in field conditions.     

Spatiotemporal aspects of real-time PM(2.5): low- and middle-income neighborhoods in Bangalore, India

We measured outdoor fine particulate matter (PM(2.5)) concentrations in a low- and a nearby middle-income neighborhood in Bangalore, India. Each neighborhood included sampling locations near and not near a major road. One-minute average concentrations were recorded for 168 days during September 2008 to May 2009 using a gravimetric-corrected nephelometer. We also measured wind speed and direction, and PM(2.5) concentration as a function of distance from road. Average concentrations are 21-46% higher in the low- than in the middle-income neighborhood, and exhibit differing spatiotemporal patterns. For example, in the middle-income neighborhood, median concentrations are higher near-road than not near-road (56 versus 50 μg m(-3)); in the low-income neighborhood, the reverse holds (68 μg m(-3) near-road, 74 μg m(-3) not near-road), likely because of within-neighborhood residential emissions (e.g., cooking; trash combustion). A moving-average subtraction method used to infer local- versus urban-scale emissions confirms that local emissions are greater in the low-income neighborhood than in the middle-income neighborhood; however, relative contributions from local sources vary by time-of-day. Real-time relative humidity correction factors are important for accurately interpreting real-time nephelometer data.     

Emission factors, size distributions, and emission inventories of carbonaceous particulate matter from residential wood combustion in rural China

Published emission factors (EFs) often vary significantly, leading to high uncertainties in emission estimations. There are few reliable EFs from field measurements of residential wood combustion in China. In this study, 17 wood fuels and one bamboo were combusted in a typical residential stove in rural China to measure realistic EFs of particulate matter (PM), organic carbon (OC), and elemental carbon (EC), as well as to investigate the influence of fuel properties and combustion conditions on the EFs. Measured EFs of PM, OC, and EC (EF(PM), EF(OC), and EF(EC), respectively) were in the range of 0.38-6.4, 0.024-3.0, and 0.039-3.9 g/kg (dry basis), with means and standard derivation of 2.2 ± 1.2, 0.62 ± 0.64, and 0.83 ± 0.69 g/kg, respectively. Shrubby biomass combustion produced higher EFs than tree woods, and both species had lower EFs than those of indoor crop residue burning (p < 0.05). Significant correlations between EF(PM), EF(OC), and EF(EC) were expected. By using a nine-stage cascade impactor, it was shown that size distributions of PM emitted from tree biomass combustions were unimodal with peaks at a diameter less than 0.4 μm (PM(0.4)), much finer than the PM from indoor crop residue burning. Approximately 79.4% of the total PM from tree wood combustion was PM with a diameter less than 2.1 μm (PM(2.1)). PM size distributions for shrubby biomasses were slightly different from those for tree fuels. On the basis of the measured EFs, total emissions of PM, OC, and EC from residential wood combustion in rural China in 2007 were estimated at about 303, 75.7, and 92.0 Gg.     

Temporal trends in atmospheric PM₂.₅, PM₁₀, elemental carbon, organic carbon, water-soluble organic carbon, and optical properties: impact of biomass burning emissions in the Indo-Gangetic Plain

The first simultaneous measurements and analytical data on atmospheric concentrations of PM(2.5), PM(10), inorganic constituents, carbonaceous species, and their optical properties (aerosol optical depth, AOD; absorption coefficient, b(abs); mass absorption efficiency, σ(abs); and single scattering albedo, SSA) from an urban site (Kanpur) in the Indo-Gangetic Plain are reported here. Significantly high aerosol mass concentration (>100 μg m(-3)) and AOD (> 0.3) are seen as a characteristic feature throughout the sampling period, from October 2008 to April 2009. The temporal variability in the mass fractions of carbonaceous species (EC, OC, and WSOC) is pronounced during October-January when emissions from biomass burning are dominant and OC is a major constituent (～30%) of PM(2.5) mass. The WSOC/OC ratio varies from 0.21 to 0.65, suggesting significant contribution from secondary organic aerosols (SOAs). The mass fraction of SO(4)(2-) in PM(2.5) (Av: 12.5%) exceeds that of NO(3)(-) and NH(4)(+). Aerosol absorption coefficient (@ 678 nm) decreases from 90 Mm(-1) (in December) to 20 Mm(-1) (in April), and a linear regression analysis of the data for b(abs) and EC (n = 54) provides a measure of the mass absorption efficiency of EC (9.6 m(2) g(-1)). In contrast, scattering coefficient (@ 678 nm) increases from 98 Mm(-1) (in January) to 1056 Mm(-1) (in April) and an average mass scattering efficiency of 3.0 ± 0.9 m(2) g(-1) is obtained for PM(10) samples. The highest b(scat) was associated with the dust storm event (April 17, 2009) over northern Iraq, eastern Syria, and southern Turkey; thus, resulting in high SSA (0.93 ± 0.02) during March-April compared to 0.82 ± 0.04 in October-February. These results have implications to large temporal variability in the atmospheric radiative forcing due to aerosols over northern India.     

甘草黄酮对大气细颗粒物PM2.5引起肺泡巨噬细胞损伤的保护作用

目的:研究甘草黄酮对大气细颗粒物PM2.5(SRM 2786)导致的大鼠肺泡巨噬细胞(NR8383)损伤的保护作用。方法:实验分为对照组、模型组(125 μg/mL SRM 2786)与不同浓度甘草黄酮给药组(3.125、6.25、12.5、25 μg/mL+125 μg/mL SRM 2786),药物作用24 h后分别用MTT法检测细胞存活率、细胞形态观察、酶联免疫法(Elisa)检测细胞上清液肿瘤坏死因子α(TNF-α)、白介素6(IL-6)及白介素1β(IL-1β)的含量、各组细胞NO和ROS释放及细胞中SOD活性和GSH-PX含量。结果:相较于对照组,125 μg/mL SRM 2786诱导可减少细胞贴璧生长且显著降低细胞存活率、SOD活性和GSH-PX含量、提高TNF-α、IL-6及IL-1β三种细胞因子的释放及细胞ROS和NO释放(p<0.01);而3.125~25 μg/mL甘草黄酮可使大部分悬浮细胞重新贴璧且显著提高下降的细胞存活率,显著抑制SRM 2786诱导的炎症细胞因子的释放和ROS释放、显著提高SOD活性及GSH-PX含量(p<0.05或 p<0.01),6.25~25 μg/mL甘草黄酮可显著降低SRM 2786导致的NO释放(p<0.05或p<0.01)。结论:甘草黄酮可显著提高由细颗粒物SRM 2786降低的细胞存活率和提高抗氧化酶活性、抑制炎性因子释放及氧化应激,其机制可能与其抗炎性损伤和氧化损伤有关。     

Land use regression model for ultrafine particles in Amsterdam

There are currently no epidemiological studies on health effects of long-term exposure to ultrafine particles (UFP), largely because data on spatial exposure contrasts for UFP is lacking. The objective of this study was to develop a land use regression (LUR) model for UFP in the city of Amsterdam. Total particle number concentrations (PNC), PM10, PM2.5, and its soot content were measured directly outside 50 homes spread over the city of Amsterdam. Each home was measured during one week. Continuous measurements at a central urban background site were used to adjust the average concentration for temporal variation. Predictor variables (traffic, address density, land use) were obtained using geographic information systems. A model including the product of traffic intensity and the inverse distance to the nearest road squared, address density, and location near the port explained 67% of the variability in measured PNC. LUR models for PM2.5, soot, and coarse particles (PM10, PM2.5) explained 57%, 76%, and 37% of the variability in measured concentrations. Predictions from the PNC model correlated highly with predictions from LUR models for PM2.5, soot, and coarse particles. A LUR model for PNC has been developed, with similar validity as previous models for more commonly measured pollutants.     

Particulate oxidative burden associated with firework activity

Firework events are capable of inducing particulate matter (PM) episodes that lead to exceedances of regulatory limit values. As short-term peaks in ambient PM concentration have been associated with negative impacts on respiratory and cardiovascular health, we performed a detailed study of the consequences of firework events in London on ambient air quality and PM composition. These changes were further related to the oxidative activity of daily PM samples by assessing their capacity to drive the oxidation of physiologically important lung antioxidants including ascorbate, glutathione and urate (oxidative potential, OP). Twenty-four hour ambient PM samples were collected at the Marylebone Road sampling site in Central London over a three week period, including two major festivals celebrated with pyrotechnic events: Guy Fawkes Night and Diwali. Pyrotechnic combustion events were characterized by increased gas phase pollutants levels (NO(x) and SO(2)), elevated PM mass concentrations, and trace metal concentrations (specifically Sr, Mg, K, Ba, and Pb). Relationships between NO(x), benzene, and PM(10) were used to apportion firework and traffic source fractions. A positive significant relationship was found between PM oxidative burden and individual trace metals associated with each of these apportioned source fractions. The level of exposure to each source fraction was significantly associated with the total OP. The firework contribution to PM total OP, on a unit mass basis, was greater than that associated with traffic sources: a 1 μg elevation in firework and traffic PM fraction concentration was associated with a 6.5 ± 1.5 OP(T) μg(-1) and 5.2 ± 1.4 OP(T) μg(-1) increase, respectively. In the case of glutathione depletion, firework particulate OP (3.5 ± 0.8 OP(GSH) μg(-1)) considerably exceeded that due to traffic particles (2.2 ± 0.8 OP(GSH) μg(-1)). Therefore, in light of the elevated PM concentrations caused by firework activity and the increased oxidative activity of this PM source, there is value in examining if firework derived PM is related to acute respiratory outcomes.     

Comparison of light scattering devices and impactors for particulate measurements in indoor,outdoor, and personal environments

Short-term monitoring of individual particulate matter (PM) exposures on subjects and inside residences in health effect studies have been sparse due to the lack of adequate monitoring devices. The recent development of small and portable light scattering devices, including the Radiance nephelometer (neph) and the personal DataRAM (pDR) has made this monitoring possible. This paper evaluates the performance of both the passive pDR and neph (without any size fractionation inlet) against measurements from both Harvard impactors (HI2.5) and Harvard personal environmental monitors (HPEM2.5) for PM2.5 in indoor, outdoor, and personal settings. These measurements were taken at the residences and on the person of nonsmoking elderly subjects across the metropolitan Seattle area and represent a wide range of light scattering measurements directly related to exposures and health effects. At low PM levels, nephs provided finer resolution and more precise measurements (precision = 3-8% and uncertainty = 2.8 x 10(-7) m(-1) or <1 microg/m3) than the pDRs. The unbiased precision of pDRs above 10 microg/m3 is around 5% (with an unbiased uncertainty of 4.4 microg/m3). The 24-h average responses of the pDR and neph, as compared to 24-h integrated gravimetric measurements, are not affected by indoor sources of PM. When regressed against 24-h gravimetric measurements, nephs showed higher coefficients of determination (R2 = 0.81-0.93) than pDRs (R2 = 0.77-0.84). The default mass calibration on the pDRs generally overestimated indoor HI2.5 measurements by 56%. When carried by subjects, the pDR overestimated the HPEM2.5 measurements by approximately 27%. Collocated real-time indoor nephs and pDRs at diverse residential sites had varied coefficients of determination across homes (R2 = 0.75-0.96), and the difference between pDR and neph responses increased during cooking hours. This difference was larger during baking or frying episodes than during other cooking or cleaning activities. Relative humidity, ranging between 25% and 64% indoors in our study, was not a significant factor affecting the differences in neph or pDR response. In summary, for nonsmoking residences, the mass scattering efficiency (m2/g) of a stationary indoor neph on a 24-h basis does not vary by residence, including residences with and without cooking activities. This is also true forthe pDR. These same stationary indoor pDRs and nephs correlate well with each other, even on a 10-min basis, in the absence of indoor source activities. The fact that these activities comprised a relatively small percentage (cooking + cleaning = 2.3%) of the overall sampling time meant that the overall correlation between these two instruments for all time periods was good. However, when examining the cooking and cleaning periods separately, the correlation was not very good. Thus, during these short-term PM episodes, the 24-h average calibrations versus gravimetric mass should be used with caution. Both devices should be potentially useful in future exposure assessment and health effects studies.     

Canadian house dust study: lead bioaccessibility and speciation

Vacuum samples were collected from 1025 randomly selected urban Canadian homes to investigate bioaccessible Pb (Pb(S)) concentrations in settled house dust. Results indicate a polymodal frequency distribution, consisting of three lognormally distributed subpopulations defined as "urban background" (geomean 58 μg g(-1)), "elevated" (geomean 447 μg g(-1)), and "anomalous" (geomean 1730 μg g(-1)). Dust Pb(S) concentrations in 924 homes (90%) fall into the "urban background" category. The elevated and anomalous subpopulations predominantly consist of older homes located in central core areas of cities. The influence of house age is evidenced by a moderate correlation between house age and dust Pb(S) content (R(2) = 0.34; n = 1025; p < 0.01), but it is notable that more than 10% of homes in the elevated/anomalous category were built after 1980. Conversely, the benefit of home remediation is evidenced by the large number of homes (33%) in the background category that were built before 1960. The dominant dust Pb species determined using X-ray Absorption Spectroscopy were as follows: Pb carbonate, Pb hydroxyl carbonate, Pb sulfate, Pb chromate, Pb oxide, Pb citrate, Pb metal, Pb adsorbed to Fe- and Al-oxyhydroxides, and Pb adsorbed to humate. Pb bioaccessibility estimated from solid phase speciation predicts Pb bioaccessibility measured using a simulated gastric extraction (R(2) = 0.85; n = 12; p < 0.0001). The trend toward increased Pb bioaccessibility in the elevated and anomalous subpopulations (75% ± 18% and 81% ± 8%, respectively) compared to background (63% ± 18%) is explained by the higher proportion of bioaccessible compounds used as pigments in older paints (Pb carbonate and Pb hydroxyl carbonate). This population-based study provides a nationally representative urban baseline for applications in human health risk assessment and risk management.