In this paper, the pooled NO 2 association with nonaccidental mortality is examined across 10 cities in Canada in single-and two-pollutant time-series models. The results reaffirm that NO 2 has the strongest association with mortality, particularly in the warm season. Although attributing such effects to NO 2 cannot be ruled out, it is plausible that NO 2 is acting as an indicator for some other exposure affecting the population. This could include PM 2.5 , as has been suggested from some personal exposure data, but it could also be indicating a more specific type of PM 2.5 , such as traffic-related particles, given that in cities the main source of NO 2 is motor vehicle exhaust. NO 2 could also be acting as a surrogate for other pollutant(s) originating from motor vehicles or high-temperature combustion, such as volatile organic compounds (VOCs) or polycyclic aromatic hydrocarbons. Another possibility is other oxidized nitrogen species (''NO z '') or photochemically produced pollutants that can co-vary with NO 2 , especially during urban stagnation events. Data to test these different possibilities across several Canadian cities are examined. The focus is on correlations in time or space between NO 2 and other pollutants that are more strongly linked to vehicle emissions. The results support the hypothesis that NO 2 is a better indicator than PM 2.5 of a range of other toxic pollutants. This includes VOCs, aldehydes, NO z and particle-bound organics in motor vehicle exhaust. Thus, overall, the strong effect of NO 2 in Canadian cities could be a result of it being the best indicator, among the pollutants monitored, of fresh combustion (likely motor vehicles) as well as photochemically processed urban air.
Phthalates have been used extensively as plasticizers to improve the flexibility of polymers, and they also have found many industrial applications. They are ubiquitous in the environment and have been detected in a variety of environmental and biological matrices. The goal of this study was to develop a method for the determination of 17 phthalate esters in house dust. This method involved sonication extraction, sample cleanup using solid phase extraction, and isotope dilution GC/MS/MS analysis. Method detection limits (MDLs) and recoveries ranged from 0.04 to 2.93 μg/g and from 84 to 117%, respectively. The method was applied to the analysis of phthalates in 38 paired household vacuum samples (HD) and fresh dust (FD) samples. HD and FD samples compared well for the majority of phthalates detected in house dust. Data obtained from 126 household dust samples confirmed the historical widespread use of bis(2-ethylhexyl) phthalate (DEHP), with a concentration range of 36 μg/g to 3840 μg/g. Dibutyl phthalate (DBP), benzyl butyl phthalate (BzBP), diisononyl phthalate (DINP), and diisodecyl phthalate (DIDP) were also found in most samples at relatively high concentrations. Another important phthalate, diisobutyl phthalate (DIBP), was detected at a frequency of 98.4% with concentrations ranging from below its MDL of 0.51 μg/g to 69 μg/g.
Measurement of particle-bound organic carbon (OC) may be complicated by sampling artifacts such as adsorption of gas-phase species onto particles or filters or evaporation of semivolatile compounds off the particles. A denuder-based integrated organic gas and particle sampler (IOGAPS), specifically designed to minimize sampling artifacts, has been developed to sample atmospheric carbonaceous aerosols. IOGAPS is designed to first remove gas-phase chemicals via sorption to the XAD-coated denuder, and subsequently particles are trapped on a quartz filter. A backup sorbent system consisting of sorbent- (XAD-4 resin) impregnated filters (SIFs) was used to capture the semivolatile OC that evaporates from the particles accumulated on the upstream quartz filter. A traditional filter pack (FP) air sampler, which uses a single quartz filter to collect the particles, was employed for comparison in this study. Elemental and organic carbon were determined from filter punches by a thermal optical transmittance aerosol carbon analyzer. Field measurements show that there was no significant difference between the elemental carbon concentrations determined by the FP and IOGAPS, indicating that particle loss during the transit through the denuder tube was negligible. Compared with the OC determined by FP (3.9-12.6 microg of C/m3), the lower OC observed on the quartz filter in the IOGAPS (2.2-6.0 microg of C/m3) was expected because of the removal of gas-phase organics by the denuder. Higher semivolatile organic carbon (SVOC) on the backup SIFs during the night (1.24-8.43 microg of C/m3) suggests that more SVOC, emitted from primary sources or formed as secondary organic compounds, partitions onto the particles during the night because of the decreased ambient temperature. These data illustrate the utility of an IOGAPS system to more accurately determine the particle-bound OC in comparison to FP-based systems.
An integrated analytical method for the simultaneous determination of five parabens (methyl-, ethyl-, propyl-, butyl-, and benzyl-), triclosan, and methyl triclosan in indoor house dust was developed based on gas chromatographic-mass spectrometric technique (GC/MS). Analytes were extracted from dust samples by sonication. After sample cleanup by solid-phase extraction (SPE), the extracts were derivatized with N-methyl-N-(trimethylsilyl)trifluoroacetamide (MSTFA) and then analyzed by gas chromatography coupled with ion trap mass spectrometry operated in multiple reaction monitoring (MRM) mode. For quantitation, isotope-labelled internal standards were used for each corresponding target analyte. Only 0.05 g of dust sample was needed for the analysis. Method detection limits ranged from 6.5 to 10 ng/g, and absolute recoveries from 74% to 92%. The developed method demonstrated good repeatability and reproducibility, with relative standard deviations (RSDs) less than 16% for all the analytes. The analytes were determined in dust samples collected using two vacuum sampling methods from 63 Canadian homes: a sample of fresh or "active" dust (FD) collected using a Pullman-Holt vacuum sampler, and a composite sample taken from the household vacuum cleaner (HD). Methyl paraben, propyl paraben, and triclosan were detected in all HD and FD samples. HD samples yielded median values for methyl paraben, propyl paraben, and triclosan of 1080, 463, and 378 ng/g, respectively, which were comparable to the FD sample medians of 1120, 618 and 571 ng/g. Ethyl paraben was detected at frequencies of 89% in FD and 73% in HD samples, with median values of 52 and 25 ng/g, respectively. Butyl paraben was detected at frequencies of 44% in FD and 75% in HD samples, with median values of <10 and 59 ng/g, respectively. Benzyl paraben and methyl triclosan were not detected in any of the samples collected by either method. Samples collected according to the fresh dust protocol agreed with the household vacuum samples 90% of the time. Widely scattered concentration levels were observed for target analytes from this preliminary set of 63 Canadian samples, which suggests a wide variability in Canadian household exposures to these chemicals.
A new method for the simultaneous determination of 11 synthetic musks and one fragrance compound in house dust was developed. The nitro musks included musk ketone (MK, 4-tert-butyl-3,5-dinitro-2,6-dimethylacetophenone), musk xylene (MX, 1-tert-butyl-3,5-dimethyl-2,4,6-trinitrobenzene), musk ambrette (1-tert-butyl-2-methoxy-4-methyl-3,5-dinitrobenzene) and musk moskene (1,1,3,3,5-pentamethyl-4,6-dinitroindane). The polycyclic musk compounds were 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta-(γ)-2-benzopyran (HHCB), 7-acetyl-1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydronaphthalene (AHTN), 4-acetyl-1,1-dimethyl-6-tert-butylindane, 6-acetyl-1,1,2,3,3,5-hexamethylindane, 5-acetyl-1,1,2,6-tetramethyl-3-isopropylindane, 6,7-dihydro-1,1,2,3,3-pentamethyl-4(5H)-indanon. The one macrocyclic musk was 1,4-dioxacycloheptadecane-5,17-dione. The bicyclic hydrocarbon fragrance compound (1,2,3,4,5,6,7,8-octahydro-2,3,8,8-tetramethylnaphthalen-2yl)ethan-1-one (OTNE) and HHCB-lactone (4,6,6,7,8,8-hexamethyl-1H,3H,4H,6H,7H, 8H-indeno[5,6-c]pyran-1-one), a degradation product of HHCB, were also analysed. NIST SRM 2781 (domestic sludge) and SRM 2585 (organic contaminants in house dust) were analysed for these target compounds. The method was applied for the analysis of 49 paired samples collected using two vacuum sampling methods: a sample of fresh or "active" dust (FD) collected using a Pullman-Holt vacuum sampler, and a household dust (HD) sample taken from the participants' vacuum cleaners. Method detection limits and recoveries ranged from 12 to 48 ng/g and 54 to 117 %, respectively. AHTN, HHCB, OTNE and HHCB-lactone were detected in all samples, with median concentrations of 552, 676, 252 and 453 ng/g for FD samples, respectively; and 405, 992, 212 and 492 ng/g for HD samples, respectively. MX and MK were detected with high frequencies but with much lower concentrations. The two sampling methods produced comparable results for the target analytes. Widely scattered concentration levels were observed for target analytes from this set of 49 house dust samples, suggesting a wide variability in Canadian household exposure to synthetic musks.
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