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1.
Starokozhev E  Sieg K  Fries E  Püttmann W 《Chemosphere》2011,82(10):1482-1488
Laboratory experiments were performed to investigate the partitioning behavior of a set of diverse volatile organic compounds (VOCs). After equilibration at a temperature of 25 °C, the VOC concentrations were measured by headspace method in combination with gas chromatography/mass spectrometry (GC/MS). The obtained data were used to determine the partition coefficients (KP) of VOCs in a gas-liguid-solid system. The results have shown that the presence and nature of solid materials in the working solution control the air-water partitioning of dissolved VOCs. The air/solution partitioning of BTEX and C9-C10 aldehydes was most affected in the presence of diesel soot. KP values decreased by a factor ranging from 1.5 for toluene to 3.0 for ethylbenzene. The addition of mineral dust in the working solution exhibited greater influence on the partitioning of short aldehydes. KP values decreased by a factor of 1.8. The experimental partition coefficients were used to develop a predictive model for partitioning of BTEX and n-aldehydes between air, water and solid phases.  相似文献   

2.
A scale-free network model with surface and vertical field measurements was used to identify the connectivity distribution of the scale-free network behavior of ambient volatile organic compounds (VOCs). The results show that the carbon number (C n ) with the total amount of C n compounds (P(C n )) possesses an explicit relationship with the scale-free network behavior. The proportionate coefficient (α) and exponent ( γ) of the scale-free network model with spatial and temporal variations are estimated and discussed. The analytical results demonstrate that although photochemical reactions cause the VOCs fraction variation, they do not alter the fraction of C n compounds observably. Therefore, the values of α and of γ did not vary with time, but with local regional characteristics. The results indicate that the influence of local VOCs emissions occurs at a height of 100 m, but becomes insufficient at a height of 300 m. Air mass mixing increases with greater height; thus, the influence of regional characteristics at a height of 700 m is low. Finally, a successful empirical model was established to evaluate the distribution of surface VOCs in various regions.  相似文献   

3.
There are a number of difficulties associated with the quantitative analysis of volatile organic compounds (VOCs) in atmospheric particles. Therefore, majority of the previous studies on VOCs associated with particles have been qualitative. Air samples were collected in Izmir, Turkey to determine ambient particle and gas phase concentrations of several aromatic, oxygenated and halogenated VOCs. Samples were quantitatively analyzed using thermal desorption–gas chromatography/mass spectrometry. Gas-phase concentrations ranged between 0.02 (bromoform) and 4.65 μg m−3 (toluene) and were similar to those previously measured at the same site. Particle-phase concentrations ranged from 1 (1,3-dichlorobenzene) to 933 pg m−3 (butanol). VOCs were mostly found in gas-phase (99.9±0.25%). However, the particulate VOCs had comparable concentrations to those reported previously for semivolatile organic compounds. The distribution of particle-phase VOCs between fine (dp<2.5 μm) and coarse (2.5 μm<dp<10 μm) fractions was also investigated. It was found that VOCs were mostly associated with fine particles.  相似文献   

4.
A chemical mass balance (CMB) receptor model was used for estimating the diurnal contributions of VOC emission sources to the ambient C2–C9 VOC concentration in Seoul, Korea. For this purpose, the VOC concentrations were measured in the morning, the afternoon, and the evening. The samples were collected using a 2-h integrated SUMMA canister. The source profiles were developed for the CMB calculation in the Seoul area. To investigate the effect of the chemical reaction loss of VOCs on the CMB calculation, the modified model employing a decay factor and the standard model that considers no loss were compared. The modified model estimated that the vehicle exhaust (52%) was the largest leading source of VOCs in the Seoul atmosphere, followed by the use of solvents (26%), gasoline evaporation (15%), the use of liquefied petroleum gas (LPG) (5%), and the use of liquefied natural gas (LNG) (2%). Relative source contribution for vehicle exhaust showed a clear diurnal variation with a high in the morning and evening and a low in the afternoon, while the contribution of evaporative emissions (gasoline evaporation and solvent usage) showed a different diurnal pattern from that of the vehicle exhaust, exhibiting a high in the afternoon and evening and a low in the morning. It was found that the difference between the total source contribution (μg m−3) estimated from these two models was not statistically significant. However, when the paired-sample t-test is applied to the individual sources, a significant difference was found for the vehicle exhaust and the solvent use. In addition, the modified model brought forth a better performance with high R2 and low χ2 as compared to those obtained from the standard model in the CMB calculation. The vehicle exhaust and solvent use were estimated to be the largest and the second largest contributors to ambient benzene as well as ozone formation potential (OFP), respectively. Based on above results we believe that incorporating the reaction loss in the CMB calculations helps to better fit the source profile to the ambient VOC concentrations. However, the reaction loss does not significantly affect the estimation of source contributions.  相似文献   

5.
The dispersion of VOCs emitted by a municipal solid waste landfill was studied for a period of over one year. Sixteen VOCs were monitored: linear alkanes from C7 to C11, BTEX, trimethylbenzene, trichlorethylene, tetrachlorethylene, α and β-pinenes, limonene. The analytical procedure was first comprised of static long-term sampling of about 2 months using radial diffusion Radiello tubes containing activated carbon, followed by extraction by solvent (i.e. CS2) and GC/MS analysis. The results were initially analysed on the basis of the total concentration of the quantified VOCs, then by examining the concentrations of certain selected compounds. The influence of different parameters such as operating conditions, meteorological conditions and site morphology was highlighted on the basis of total VOC concentrations. In order to study the VOC's dispersion more closely, 5 compounds were chosen: toluene, benzene, limonene, and the sum trichlorethylene + tetrachlorethylene, as a “marker”, to verify the origin of the VOCs emitted. The results showed that the main source of VOCs is the open cell and lead to different hypotheses on interferences from neighbouring sources and to the proposal of solutions to limit the emission of VOCs and their dispersion. To our knowledge, this type of study has not been accomplished until this day.  相似文献   

6.
Nonmethane hydrocarbons (NMHCs) are important precursors of ozone and other photo oxidants. We presented continuous hourly average concentrations of 45 C2–C10 NMHCs measured in urban area of Dallas, USA from 1996 to 2004. Most of the selected compounds are good variables with less noise. The top 10 species with high ozone-generating potential were identified according to their concentrations and reactivities. The ambient concentrations of abundant anthropogenic emission hydrocarbons measured in Dallas were about 2–4 times of the background values measured in the remote areas with adjacent latitude. The time series for anthropogenic emission hydrocarbons showed an obvious seasonal cycle with relatively high concentration in winter and low concentration in summer. The sinusoidal function with a linearly decreasing factor could well fit the time series of NMHCs. The phase of seasonal cycle for the aromatic hydrocarbons of toluene, m/p xylene and o-xylene that might come from both vehicle emission and solvent utilities evaporation was about 1 month earlier than that for alkanes and alkenes that mainly came from vehicle emission. Ambient NMHCs in Dallas decreased with a stable rate during 1996–2004. For most of compounds with high ozone-generating potential, the rate of ambient concentration decrease was higher or much higher than the rate of volatile organic compounds (VOCs) source emission reduction estimated by EPA's National Emission Inventory. On weekdays, the morning hydrocarbon concentration peak was coincident with morning traffic rush time in Dallas. Another concentration peak was delayed to afternoon traffic rush time. The characteristics of VOCs sources, photochemical removal processes and atmospheric dilution could be interpreted by the diurnal variations of benzene/ethylbenzene (B/E), toluene/ethylbenzene (T/E) and xylene/ethylbenzene (X/E). The ratio of VOC/NOx measured in Dallas was substantially smaller than that calculated for USA cities. Ozone formation in Dallas was VOC sensitive.  相似文献   

7.
ABSTRACT

The initial solid-phase concentration of volatile organic compounds (VOCs) is a key parameter influencing the emission characteristics of many indoor materials. Solid-phase measurements are typically made using solvent extraction or thermal headspace analysis. The high temperatures and chemical solvents associated with these methods can modify the physical structure of polymeric materials and, consequently, affect mass transfer characteristics.

To measure solid-phase concentrations under conditions resembling those in which the material would be installed in an indoor environment, a new technique was developed for measuring VOC concentrations in vinyl flooring (VF) and similar materials. A 0.09-m2 section of new VF was punched randomly to produce ~200 0.78-cm2 disks. The disks were milled to a powder at -140 °C to simultaneously homogenize the material and reduce the diffusion path length without loss of VOCs. VOCs were extracted from the VF particles at room temperature by fluidized-bed desorption (FBD) and by direct thermal desorption (DTD) at elevated temperatures. The VOCs in the extraction gas from FBD and DTD were collected on sorbent tubes and analyzed by gas chromatog-raphy/mass spectrometry (GC/MS). Seven VOCs emitted by VF were quantified. Concentration measurements by FBD ranged from 5.1 |ig/g VF for n-hexadecane to 130 |Jg/g VF for phenol. Concentrations measured by DTD were higher than concentrations measured by FBD. Differences between FBD and DTD results may be explained using free-volume and dual-mobility sorption theory, but further research is necessary to more completely characterize the complex nature of a diffusant in a polymer matrix.  相似文献   

8.
《Chemosphere》2013,90(11):1426-1436
Volatile organic compounds (VOCs) from several different municipal solid wastes’ treatment plants in Mallorca (Spain) have been analysed by thermal desorption–gas chromatography–mass spectrometry (TD–GC–MS). Ambient (immission) air was collected during February and March 2011 by active sampling onto sorbents Tenax™ TA and Carboxen™ 1000. The study presents the chemical characterisation of 93 volatile organic compounds (VOCs) from an overall set of 84 immission air samples. 70 VOCs were positively identified.The linear fit for all 93 external standard calibration, from 10 mg L−1 to 150 mg L−1 (n = 4), was within the range 0.974 < r2 < 0.998. Limits of detection of the method (LOD) for all the standards were within the range 1.1–4,213 pg, as the absolute standard amount spiked into sorbent tubes in 1 μL standard mixture (dissolved in methanol).Overall results stated systematic correlation between waste’s nature and VOCs’ air composition. Organic wastes show main contribution of terpenes, waste water sludge residues’ of reduced sulphured compounds (RSCs) and municipal solid wastes show contribution of a wide sort of VOCs. The use of a chemometric approach for variable’s reduction to 12 principal components enables evaluation of similarities and dissimilarities between facilities. PCA clearly related samples to its corresponding facility on the basis of their VOCs composition and the ambient temperature.  相似文献   

9.
空气中挥发性有机物监测技术的研究进展   总被引:13,自引:0,他引:13  
讨论了空气中挥发性有机化合物(VOCs)的监测分析方法研究进展。重点介绍了空气中VOCs的采集、分析和测定;简要叙述了样品前处理的新方法--固相微萃取法(SPME)与其它前处理方法的研究概况。  相似文献   

10.
Abstract

An activated sludge aeration tank (40 × 40 × 300 cm, width × length × height) with a set of 2-mm orifice air spargers was used to treat gas-borne volatile organic compounds (VOCs; toluene, p-xylene, and dichloromethane) in air streams. The effects of liquid depth (Z), aeration intensity (G/A), the overall mass-transfer rate of oxygen in clean water (K L a O2 ), the Henry’s law constant of the tested VOC (H), and the influent gaseous VOC concentration (C 0) on the efficiency of removal of VOCs were examined and compared with a literature-cited model. Results show that the measured VOC removal efficiencies and those predicted by the model were comparable at a G/A of 3.75–11.25 m3/m2·hr and C 0 of ~1000–6000 mg/m3. Experimental data also indicated that the designed gas treatment reactor with K L a O2 = 5–15 hr?1 could achieve >85% removal of VOCs with H = 0.24–0.25 at an aerated liquid depth of 1 m and >95% removal of dichloromethane with H = 0.13 at a 1-m liquid depth.  相似文献   

11.
Uptake of aromatic hydrocarbons (AH) by ice crystals during vapor deposit growth was investigated in a walk-in cold chamber at temperatures of 242, 251, and 260 K, respectively. Ice crystals were grown from ambient air in the presence of gaseous AH namely: benzene (C6H6), toluene (methylbenzene, C7H8), the C8H10 isomers ethylbenzene, o-, m-, p-xylene (dimethylbenzenes), the C9H12 isomers n-propylbenzene, 4-ethyltoluene, 1,3,5-trimethylbenzene (1,3,5-TMB), 1,2,4-trimethylbenzene (1,2,4-TMB), 1,2,3-trimethylbenzene (1,2,3-TMB), and the C10H14 compound tert.-butylbenzene. Gas-phase concentrations calculated at 295 K were 10.3–20.8 μg m−3. Uptake of AH was detected by analyzing vapor deposited ice with a very sensitive method composed of solid-phase micro-extraction (SPME), followed by gas chromatography/mass spectrometry (GC/MS).Ice crystal size was lower than 1 cm. At water vapor extents of 5.8, 6.0 and 8.1 g m−3, ice crystal shape changed with decreasing temperatures from a column at a temperature of 260 K, to a plate at 251 K, and to a dendrite at 242 K. Experimentally observed ice growth rates were between 3.3 and 13.3×10−3 g s−1 m−2 and decreased at lower temperatures and lower value of water vapor concentration. Predicted growth rates were mostly slightly higher.Benzene, toluene, ethylbenzene, and xylenes (BTEX) were not detected in ice above their detection limits (DLs) of 25 pg gice−1 (toluene, ethylbenzene, xylenes) and 125 pg gice−1 (benzene) over the entire temperature range. Median concentrations of n-propylbenzene, 4-ethyltoluene, 1,3,5-TMB, tert.-butylbenzene, 1,2,4-TMB, and 1,2,3-TMB were between 4 and 176 pg gice−1 at gas concentrations of 10.3–10.7 μg m−3 calculated at 295 K. Uptake coefficients (K) defined as the product of concentration of AH in ice and density of ice related to the product of their concentration in the gas phase and ice mass varied between 0.40 and 10.23. K increased with decreasing temperatures. Values of Gibbs energy (ΔG) were between −4.5 and 2.4 kJ mol−1 and decreased as temperatures were lowered. From the uptake experiments, the uptake enthalpy (ΔH) could be determined between −70.6 and −33.9 kJ mol−1. The uptake entropy (ΔS) was between −281.3 and −126.8 J mol−1 K−1. Values of ΔH and ΔS were rather similar for 4-ethlytoluene, 1,3,5-TMB and tert.-butylbenzene, whereas 1,2,3-TMB showed much higher values.  相似文献   

12.
《Chemosphere》1996,33(5):865-877
The use of stable isotope of organic-carbon, organic-13C, as a tracer for the determination of the concentration of tetrachloroethylene (PCE), CA, in Heterosigma akashiwo and Skeletonema costatum was examined. CA determined by the 13C and GC methods showed good agreement with each other. This suggests that it is reasonable and reliable to determine the bioconcentration potentail of PCE in marine algae. Fitting values of bioconcentration potentail parameters, including uptake rate constant k1, elimination rate constant k2 and bioconcentration factor on the basis of dry weight BCFD, were done not only to the time course for PCE uptake by the algae with the bioconcentration model, but also to experimental data for “percent inhibition(%)∼exposure concentration of PCE∼time” with the combined bioconcentration and probability model. The values obtained from the bioconcentration model were consistent with those from the combined bioconcentration and probability model. With the parameters (such as k1, k2, growth rate constant kG, critical concentration of HOCs in the organism resulting in growth inhibition CA1 and spread factor S) the variability in toxicity (such as EC10, EC50, EC70) can be estimated from the combined bioconcentration and probability model, which fits well with the experimental observations.  相似文献   

13.
The photo-Fenton reaction was applied as a novel method for the removal of volatile organic compounds (VOCs) in the gas phase, and its effectiveness was experimentally examined. In conventional VOCs removal methods using a photocatalyst or ozone, VOCs are oxidized in the gas phase. Therefore, incompletely oxidized intermediates, which may have adverse effects on health, are likely to contaminate the treated air. On the other hand, in the VOCs removal method developed in this study, because the VOCs are oxidized in the liquid phase by the photo-Fenton reaction, any incompletely oxidized intermediates produced are confined to the liquid phase. As a result, the contamination of the treated air by these harmful intermediates can be prevented. Using a semi-batch process, it was found that the removal efficiency for toluene in a one-pass test (residence time of 17 s) was 61%, for an inlet toluene gas concentration of 930 ppbv, an initial iron ion concentration of 20 mg L−1, and an initial hydrogen peroxide concentration of 630 mg L−1. The removal efficiency was almost constant as long as H2O2 was present in the solution. Proton transfer reaction mass spectrometry analysis confirmed the absence of any incompletely oxidized intermediates in the treated air.  相似文献   

14.
Particle-bound polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/Fs) in ambient air were monitored together with particulate matter less than 10 μm (PM10) at three sampling sites of the Andean city of Manizales, Colombia; during September 2009 and July 2010. PCDD/Fs ambient air emissions ranged from 1 fg WHO-TEQ m−3 to 52 fg WHO-TEQ m−3 in particulate fraction. The PM10 concentrations ranged from 23 μg m−3 to 54 μg m−3. Concentrations of PM10 and PCDD/Fs in ambient air observed for Manizales - a medium sized city with a population of 380 000 - were comparable to concentrations in larger cities. The highest concentrations of PCDD/Fs and PM10 found in this study were determined at the central zone of the city, characterized by public transportation density, where diesel as principal fuel is used. In addition, hypothetical gas fractions of PCDD/Fs were calculated from theoretical Kp data. Congener profiles of PCDD/Fs exhibited ratios associated with different combustion sources at the different sampling locations, ranging from steel recycling to gasoline and diesel engines. Taking into account particle and gas hypothetical fraction of PCDD/Fs, Manizales exhibited values of PCDD/Fs equivalent to rural and urban-industrial sites in the southeast and center of the city respectively. Poor correlation of PCDDs with PM10 (r = −0.55 and r = 0.52) suggests ambient air PCDDs were derived from various combustion sources. Stronger correlation was observed of PCDFs with PM10. Poor correlation between precipitation and reduced PM10 concentration in ambient air (r = −0.45) suggested low PM10 removal by rainfall.  相似文献   

15.
16.
VOCs are important precursors of the atmospheric ozone formation species. This study investigated the airborne concentrations of 52 VOCs at two air quality monitoring stations, Daliao and Tzouying, during wintertime in southern Taiwan. Airborne VOCs samples were taken in stainless steel canisters four times per day and analyzed via gas chromatography/mass spectrometry. Maximum increment reactivity (MIR) was used to evaluate the ozone formation potential in this ozone non-attainment region. Toluene, propane, isopentane, propene, n-butane, n-pentane and isoprene contributed 78–79% of the 52 VOCs in Daliao. Toluene, 1-butene, isopentane, propene, propane, n-undecane, and n-butane contributed 71–77% of the 52 VOCs in Tzouying. The VOCs concentrations were higher in Daliao due to the high toluene emissions from a paint plant and a solvent plant in the nearby industrial district. The 24-h VOC concentrations averaged 25 ppb higher in Tzouying than in Daliao. The ozone formation potential of airborne VOCs was 1687–2730 and 1717–2261 μg-O3/g-VOCs in Daliao and Tzouying, respectively. Ozone concentrations in Tzouying were 44 ppb higher than in Daliao during the 1200–1600 sampling period.  相似文献   

17.
《Environmental Forensics》2002,3(3-4):219-225
Naturally weathered oil residues from an arid dumpsite in Al-Alamein, Egypt were analyzed for monoaromatic and triaromatic steranes to demonstrate the utility of biomarker compounds in assessing the chemical composition changes during the degradation of the released oil residues in a terrestrial environment. The characterizations of individual aromatic compounds were based on gas chromatography/mass spectrometry (GC/MS) analyses. The results showed that triaromatic sterane distributions were similar in the oil residues of varying weathering degradation extents and correlated with a fresh crude oil sample of the Western Desert-sourced oil. Molecular ratios of triaromatic sterane compounds (ratios of C2820R /C2820S, C2720R /C2820R, and C2820S /[C2620R + C2720S ]) were proved to be suitable for source identification. Major changes in chemical compositions during weathering of the oil residues were the depletion of short chain mono- and tri-aromatic steranes in samples that had undergone extensive degradation. The results of triaromatic sterane distribution are in good agreement with weathering classification based on the analyses of saturate and aromatic hydrocarbons and the ratios of n -alkanes, PAHs and saturate biomarker compounds.  相似文献   

18.
The research team analyzed the emission characteristics of gaseous pollutants, including volatile organic compounds (VOCs), from biomass combustion in improved stoves in rural China. The research included measurements from five biofuels and two stove types in the months of January, April, and September. The measurements were conducted according to U.S. EPA Method 25 using a collection system with a cooling device and two-level filters. CO, CO2, NOx, CH4 and THC analyzers were used for in-field, real-time emission measurements. The emission data indicate that gaseous pollutants were emitted at higher concentrations in the early combustion stage and lower concentrations in the later stage. CH4 and THC, as well as CO and CO2, presented positive relationships during the whole entire combustion process for all tests. The chemical profiles of flue gas samples were analyzed by GC/MS and GC/FID/ECD. Aromatics, carbonyls, and alkenes & alkynes dominated the VOC emissions, respectively accounting for 37%, 33%, and 23% of total VOC emissions by volume. Benzene was the most abundant VOC species, consisting of 17.3 ± 8.1% of VOCs, followed by propylene (11.3 ± 3.5%), acetone (10.8 ± 8.2%), toluene (7.3 ± 5.7%) and acetaldehyde (6.5 ± 7.3%). Carbon mass balance approach was applied to calculate CO, CO2, CH4, NOx, and VOC species emission factors. This analysis includes a discussion of the differences among VOC emission factors of different biofuel-stove combinations.  相似文献   

19.
Unique daily measurements of water-soluble organics in fine (<2 μm) and coarse (>2 μm) aerosols were conducted at Alert in the Canadian Arctic in winter to spring of 1992. They yield insight into photochemical production and loss of organics during long-range transport and ozone depletion events following polar sunrise. Comprehensive analyses of α, ω-dicarboxylic acids (C2–C12), ω-oxocarboxylic acids (C2–C9) and α-dicarbonyls (C2, C3) as well as pyruvic acid and aromatic (phthalic) diacid were conducted using GC and GC/MS techniques. Oxalic (C2) acid was generally the dominant diacid species in both fine and coarse fractions, followed by malonic (C3) and succinic (C4) acids. Concentrations of total diacids in the fine aerosol fraction (0.2–64 ng m−3) were 5–60 times higher than those in the coarse fraction (0.01–3 ng m−3). After polar sunrise in early-March, the total concentration of fine aerosol diacids increased by a factor of 3–5 while the coarse mode did not change significantly. From dark winter to sunlit spring, temporal changes in correlations and ratios of these water-soluble organics to vanadium and sulfate measured simultaneously suggest that atmospheric diacids and related organic compounds are largely controlled by long-range atmospheric transport of polluted air during winter, but they are significantly affected by photochemical production. The latter can occur in sunlight either during transport to the Arctic or during photochemical events associated with surface ozone depletion and bromine chemistry near Alert in spring. Conversion of gaseous precursors to particulate matter via photochemical oxidation was intensified at polar sunrise, resulting in a peak in the ratio of total diacids to V. During ozone depletion events, complex patterns are indicated in photochemical production and loss depending on the diacid compound. Unsaturated (maleic and phthalic) diacids were inversely correlated with particulate Br whereas saturated diacids (C2–C4) positively correlated with particulate Br. These results suggest that Br chemistry associated with ozone depletion leads to degradation of unsaturated diacids and to the production of smaller saturated diacids.  相似文献   

20.
Abstract

The evaluation of emissions of volatile organic compounds (VOCs) during processing of resins is of interest to resin manufacturers and resin processors. An accurate estimate of the VOCs emitted from resin processing has been difficult due to the wide variation in processing facilities. This study was designed to estimate the emissions in terms of mass of emitted VOC per mass of resin processed.

A collection and analysis method was developed and validated for the determination of VOCs present in the emissions of thermally processed acrylonitrile butadiene styrene (ABS) resins. Four composite resins were blended from automotive, general molding, pipe, and refrigeration grade ABS resins obtained from the manufacturers. Emission samples were collected in evacuated 6-L Summa canisters and then analyzed using gas chromatography/flame ionization detection/mass selective detection (GC/FID/MSD). Levels were determined for nine target analytes detected in canister samples, and for total VOCs detected by an inline GC/FID. The emissions evolved from the extrusion of each composite resin were expressed in terms of mass of VOCs per mass of processed resin. Styrene was the principal volatile emission from all the composite resins. VOCs analyzed from the pipe resin sample contained the highest level of styrene at 402 μg/g. An additional collection and detection method was used to determine the presence of aerosols in the emissions. This method involved collecting particulates on glass fiber filters, extracting them with solvents, and analyzing them using gas chromatography/mass spectrometry (GC/MS). No significant levels of any of the target analytes were detected on the filters.  相似文献   

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