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1.
A sensitive and reliable method is described for the determination of aromatic and chlorinated hydrocarbons (benzene, toluene, o-, m-, p-xylene, trichloromethane, trichloroethane, trichloroethene and tetrachloroethene) in indoor and outdoor air at environmental concentration levels. The procedure can be easily extended to other VOCs. Using passive samplers the VOCs have been adsorbed onto charcoal during a four-week sampling period and subsequently desorbed with carbon disulfide. After injection with a cold split-splitless multi-injector the VOCs have been separated by capillary gas chromatography. Quantification has been achieved using an electron capture detector (ECD) and a flame ionization detector (FID) switched in series. A limit of about 1 g/m3 for aromatic hydrocarbons and of about 0.01 g/m3 for chlorinated hydrocarbons has been obtained. The procedure has been successfully applied in the framework of a field study to measure indoor and outdoor air concentrations in Essen and Borken, two differently polluted areas of Northrhine-Westphalia.  相似文献   

2.
This paper describes the process of determining the presence of volatile organic compounds in air emissions from industrial wastewater treatment plants (WWTP). The analytical method, based on thermal desorption-gas chromatography-mass spectrometry, was developed to simultaneously determine of 99 volatile organic compounds (VOCs) in air samples. This method is rapid, environmentally-friendly (since no organic solvents are used to extract the analytes) and compatible with a large range of thermally stable polar and apolar compounds. The target VOCs were selected on the basis of their occurrence in real samples and their adverse effects on the environment and human health. To cover the wide range of target compounds, multisorbent tubes filled with Tenax TA and Carbograph 1TD were used. Method validation showed good repeatabilities, low detection limits, a high linear range and good recoveries. At a fixed sample volume of 600?mL no significant losses for any of the target compounds were found in the samples. Stability during storage indicated that samples must be keep refrigerated at 4°C and analysed within three days of collection. Real samples were taken from air emissions of an industrial wastewater treatment plant located in the Southern Industrial Area of Tarragona (Spain) with the aim of studying its contribution as a source of atmospheric VOCs. This WWTP collects wastewater from several chemical factories which produce isocyanates, polyurethanes, chlorinated organics and functional chemicals among other products. Samples from the collecting tank after the primary sedimentation showed higher VOC concentrations than samples from the secondary treatment tank. The most abundant VOCs found in these emissions are included in the USEPA List of Hazardous Air Pollutants. The highest values correspond to acrylonitrile (up to 1843?µg?m?3) and styrene (up to 573.70?µg?m?3). The levels of chloroform, 1,4-dioxane, ethylbenzene, 1,2,3-trimethylbenzene and 1,4-diethylbenzene were also high.  相似文献   

3.
This study provides data on the occurrence of volatile organic compounds (VOCs) in the biogas emission from a landfill located on the island of Mallorca (Balearic Islands, Spain), where 200,000 tonnes of urban solid wastes are dumped every year. Three different sampling cells, of differing waste ageing were investigated in August 2008, during the main tourist season and the warmest possible weather conditions. Samples were collected in Nalophan? bags according to the standard European method EN 13725 followed by VOCs adsorption onto Carboxen 1000? and Tenax TA? materials prior to thermal desorption and analysis by GC-MS. In total 42 VOCs were analysed, using external standards, out of which 36 were positively identified. Detected VOCs in µg?m?3 were alkanes (19–62), aldehydes (65–98), ketones (78–129), alcohols (67–78), esters (25–33), BTEX (83–106), halogenated compounds (16–39), terpens (1.4–2.4) and reduced sulphur compounds (2.6–4.2), showing different concentrations on each one of the three cells. Emitted VOCs showed some similarities with other previous studies from China and Turkey, while large differences to an Italian study. The benzene-to-toluene ratio (B:T) showed values in the range of 0.13 to 0.20 characteristic of biogas. H2S and NH3 gases emitted by the landfill were measured in-situ utilising Dräger? Tubes for Short-Term-Measurements, showing concentration levels of ≤800?µg?m?3 and <300?µg?m?3, respectively, which is higher than the determined VOCs in accordance with previous studies. Samples were examined with dynamic olfactometry following standard European method EN 13725, to determine a potential statistical linear correlation between odour and VOC concentrations. Such correlations were not observed probably owing to the large number of compounds emitted from garbage which are not quantified, yet causing positive results in olfactometry.  相似文献   

4.
The quality of the environmental air from indoor swimming pools has been associated with various health risks. Particular attention has focused on the effects of chronic lung exposure to chlorine and its by-products, especially in young children. We developed a simple, non-toxic approach to detect and monitor nitrogen trichloride air levels in the indoor swimming pool environment. The proposed Impinger Method (IM) was used to measure the environmental levels of nitrogen trichloride (NCl3) in 17 indoor swimming pools located in Northern Italy. This new analytical protocol is based on a colorimetric reaction commonly employed to detect the total and free chlorine levels in water. Specifically, IM allows the entrapment of NCl3 into a water solution containing diethyl-p-phenylenediamine (DPD 1) and Potassium Iodide (DPD 3). NCl3 from the air environment reacts with DPD 3 releasing iodine, which reacts with DPD 1 and produces a coloration proportional to the amount of NCl3 from the sampled indoor swimming pool air. Our sampling of the monitored swimming pool environments evidenced a mean NCl3 level (637?±?220?µg/m3) higher than the recommended WHO value (500?µg/m3). The IM was validated in terms of linearity (R 2?=?0.996), limit of detection (3.6?µg/m3) and repeatability (CV?=?1.7%), demonstrating easy-to-use characteristics, good efficiency and low cost.  相似文献   

5.
The aim of the present study was to develop a new analytical method of chromatographic determination of two important markers of ETS exposure: nicotine and 3-vinylpyridine (3-ethenylpyridine, 3-EP) in mainstream (MS) and sidestream (SS) smoke of one single cigarette and in indoor air using direct solid phase extraction combined with gas chromatography. The method can be utilised for both nicotine and 3-EP determination in SS and MS of one single cigarette as well as it allows for a precise determination of compound distribution in indoor air. The application of the same analytical method for both kinds of samples allows anticipating indoor air distribution of both analysed compounds in a very precise way. The precision of the method (calculated as a relative standard deviation) was 9.78% for nicotine and 2.67% for 3-EP; whereas the accuracy (evaluated by a recovery study conducted at three different levels) was 70.1 and 87.3%, respectively. The limit of detection was 0.06 µg per cigarette for both nicotine and 3-EP. The method was evaluated by determining the compounds of interest in two commercially available brands of cigarettes as well as in the reference cigarettes 3R4F and also in indoor air polluted with tobacco smoke. Determined levels of compounds of interest in MS varied from 586 to 772 (nicotine) µg per cigarette and from 3.5 to 10.7 (3-EP) µg per cigarette. In SS smoke the level varied from 14,370 to 22,590 (nicotine) µg per cigarette and from 185 to 550 (3-EP) µg per cigarette, whereas levels in indoor air polluted with tobacco smoke varied from 50.1 to 157.3 (nicotine) µg m?3and from 7.7 to 20.8 (3-EP) µg m?3.  相似文献   

6.
Competitive adsorption on adsorptive solid-phase microextraction (SPME) fibres implies careful determination of operating conditions for reliable quantitative analysis of VOCs in indoor air. With this objective, two analytical approaches, involving non-equilibrium and equilibrium extraction, were compared. The average detection limit obtained for GC-MS analysis of nine VOCs by the equilibrium method is 0.2 μg m−3, compared with 1.9 μg m−3 with the non-equilibrium method. The effect of the relative humidity of the air on the calibration plots was studied, and shown to affect acetone adsorption only. Hence, the concentrations that can be accurately determined are up to 9 μmol m−3. The methods were then applied to indoor air containing different concentrations of VOCs. The non-equilibrium method, involving short extraction time, can be used for detection of pollution peaks whereas equilibrium extraction is preferable for measurement of sub-μg m−3 ground concentration levels.   相似文献   

7.
A new method for the simultaneous determination of 12 volatile organic compounds (trans-1,2-dichloroethene, 1,1,1-trichloroethane, benzene, 1,2-dichloroethane, trichloroethene, toluene, 1,1,2-trichloroethane, tetrachloroethene, ethylbenzene, m-, p-, o-xylene) in water samples by headspace solid phase microextraction (HS–SPME)–gas chromatography mass spectrometry (GC–MS) was described, using a 100?µm PDMS (polydimethylsiloxane) coated fibre. The response surface methodology was used to optimise the effect of the extraction time and temperature, as well as the influence of the salt addition in the extraction process. Optimal conditions were extraction time and temperature of 30?min and ?20°C, respectively, and NaCl concentration of 4?mol?L?1. The detection limits were in the range of 1.1?×?10?3–2.3?µg?L?1 for the 12 volatile organic compounds (VOCs). Global uncertainties were in the range of 4–68%, when concentrations decrease from 250?µg?L?1 down to the limits of quantification. The method proved adequate to detect VOCs in six river samples.  相似文献   

8.
Ground-based ambient air monitoring was conducted at five different locations in and around Patiala city (29°49′–30°47′N Latitude, 75°58′–76°54′E Longitude) in Northern India in order to determine the impact of open burning of rice (Oriza sativa) crop residues on concentration levels of suspended particulate matter (SPM), sulphur dioxide (SO2) and nitrogen dioxide (NO2). Covering sensitive, residential, agricultural, commercial and urban areas, sampling of these pollutants was organised during August 2006 to January 2007 and August 2007 to January 2008 casing two rice crop residue burning periods (October–November) using a high volume sampling technique combined with gaseous sampling systems. Gravimetric analysis was used in the estimation of total suspended particulate matter (TSPM) whereas SO2 and NO2 concentration was determined using spectrophotometer (Specord205, Analytikjena). Monthly average concentrations of SPM, SO2 and NO2 have shown significant up and down features at all the selected sampling sites during the study period. Monthly average concentrations (24 hour) of SPM, SO2 and NO2 varied from 100 ± 11 µg m?3 to 547 ± 152 µg m?3, 5 ± 4 µg m?3 to 55 ± 34 µg m?3 and 9 ± 5 µg m?3 to 91 ± 39 µg m?3. Substantially higher concentrations were recorded at the commercial area site as compared to the other sampling sites for all the targeted air pollutants. Levels of SPM, SO2 and NO2 showed clear increase during the burning months (October–November) incorporated with the effect of meteorological parameters especially wind direction, precipitation and atmospheric temperature.  相似文献   

9.
A lesser degree of information is available with respect to microenvironments associated with potential exposure to naphthalene, in comparison with other volatile organic compounds. The current study investigated the levels of benzene as well as naphthalene, both in the indoor and outdoor air of apartments and in the cabins of passenger cars. Two groups of 20 apartment buildings (20 new and 20 old) were chosen on the basis of the selection criteria (apartment location and size). In addition, 10 actual commuters were recruited for this study. The equal number of drivers was recruited for the study for comparison of two types of fuels for vehicles (five drivers of gasoline-fuelled and five drivers of diesel-fuelled passenger cars). Indoor naphthalene concentrations were similar between old and new apartments, while the benzene concentrations in new apartments were significantly higher than those of old apartments. The naphthalene concentrations in bedrooms, where wardrobes with moth repellent (MRs) were placed, were significantly higher than those for living rooms where no MRs were present. In turn, these indoor concentrations were significantly higher than outdoor levels. It is noteworthy that the mean and median values of naphthalene measured in the bedrooms exceeded the USEPA RfC (inhalation reference concentration) of 3?µg?m?3, and the living room values were close to the RfC, while the residential benzene levels exceeded the European benzene limit of 5?µg?m?3. In contrast, the maximum outdoor levels were well below that of the RfC. The use of passenger cars appeared to be a significant daily activity for both naphthalene and benzene exposure. The naphthalene-to-benzene ratios varied with the type of microenvironments. Both the indoor naphthalene and benzene concentrations in the present study were much higher than those of other studies.  相似文献   

10.
《Microchemical Journal》2009,91(2):99-106
Increasing mass tourism can generate important microclimatic perturbations and also elevate indoor pollution by the transport of fine particulate matter. The purpose of this research was to study the indoor air conditions in the Royal Museum of Wawel Castle in Cracow, Poland, displaying amongst other valuable works of art also a unique collection of Flemish tapestries. The investigation involved in the determination of transport and deposition of particulate matter brought in by visitors. The microclimate inside the exhibition rooms was also monitored. Samples of suspended particulates were collected inside and outside the museum in winter and summer 2006. On days with intensive tourist visits the concentration of total suspended particulates was significantly higher (i.e., 130 µg/m3 in winter and 49 µg/m3 in summer) than on those days without tourists (i.e., 73 µg/m3 and 22 µg/m3 in winter and summer, respectively). The concentrations of all investigated elements were also considerably higher during the tourist flow. This was especially valid for soil dust associated elements (Si, K, Ca, Al, and Ti), with considerably higher levels in summer than winter. This could be linked with much more frequent tourist activity in the summer period. Also, the concentration of Cl was much higher in winter than summer, due to the use of de-icing salts on the roads and pavements.  相似文献   

11.
《Analytical letters》2012,45(13):2281-2293
The goal of this study was to evaluate the efficiency of microwave-assisted extraction for the recovery of pyrethroid and organophosphorus insecticides adsorbed on quartz fiber filters and C18 disks used for indoor air sampling. The extraction solvent, temperature, and time were optimized by spiking tests. The recoveries for the insecticides obtained by microwave-assisted extraction with acetone at 50°C for 5 min were between 71.9% and 119.2% with relative standard deviations between 0.3% and 9.3% at two spike levels (0.1 µg and 1.0 µg). The results of the microwave-assisted extraction under the validation conditions were comparable to those obtained by Soxhlet extraction, which was used as a reference technique. In a preliminary analysis, resmethrin and tetramethrin were determined in the indoor air of an apartment unit at concentrations of 7.8 ng/m3 and 66.0 ng/m3, respectively, using the microwave-assisted extraction-based method with gas chromatography/mass spectrometry.  相似文献   

12.
We report a multi‐instrument characterization of the carbon particles in carbon/polymer/nanodiamond core‐shell materials used for high‐performance liquid chromatography. These particles are prepared by the carbonization/pyrolysis of poly(divinylbenzene) (PDVB) microspheres. Scanning electron microscopy showed that the particles (4.9 µm initially) decreased in size after air oxidation (to 4.4 µm) and again after carbonization (down to 3.5 µm) but remained highly spherical. Brunauer–Emmett–Teller measurements showed low surface areas initially (as received: 1.6 m2/g, after air oxidation: 2.6 m2/g) but high values after carbonization (445 m2/g). Fourier transform infrared spectroscopy revealed the changes in the functional groups after air oxidation (C = O and C–O stretches appear), carbonization (carbon‐oxygen containing moieties disappear), and acid treatment (reintroduction of carbon‐oxygen containing moieties). X‐ray photoelectron spectroscopy (XPS) and elemental analysis revealed the surface and bulk oxygen contents before and after treatments. By XPS, the atom percent oxygen for the as received, air oxidized, carbonized, and acid treated particles are 8.7, 16.6, 3.7, and 13.8, respectively, and by elemental analysis, the percent oxygen in the materials is 0.6, 8.1, 0.9, 16.9, respectively. A principal components analysis of time‐of‐flight secondary ion mass spectrometry data identified ions that were enhanced in the different materials, where almost 90% of the variation in the analyzed peak areas was captured by two principle components. X‐ray diffraction and Raman spectroscopy suggested that the carbonized PDVB was disordered. Thermogravimetric analysis showed significant differences between the differently treated PDVB microspheres. This work applies directly to a commercial product and the process for preparing it. Copyright © 2015 John Wiley & Sons, Ltd.  相似文献   

13.
The particulates are collected on Whatman 41 cellulose filters and decomposed with sulfuric acid and hydrogen peroxide; bismuth is then measured by hydride generation/atomic absorption spectrometry. The detection limis is 0.08 ng m?3 if 500 m3 of air is filtered through an 11-cm filter. Generally, the precision is better than 10%. The concentrations found in Ghent, Belgium varied between 0.1 and 0.8 ng m?3. Bismuth was also determined in NBS Orchard leaves (SRM 1571); a value of 98.5 ± 15 ng g?1 was found.  相似文献   

14.
《Microchemical Journal》2009,91(2):93-98
Nitrogen dioxide (NO2) concentrations were used to evaluate the air quality before and after the infrastructural change of an important traffic artery in Mortsel, Antwerp (Belgium). During the reconstruction works two pairs of traffic lanes were reduced to one in each direction. Two sampling campaigns were conducted: the first one before the works in 2003 and the second one in 2005, after the road works were finished. Sampling was performed on a weekly base with the use of passive diffusion tubes on the streets, and also indoors in nearby houses. The samples were analyzed by ion chromatography, from which data the NO2 concentrations in air could be calculated. These results were compared with NO2 values from the air monitoring station 42R801 of the Flemish Environment Agency in Borgerhout, Antwerp. On the base of different NO2 concentrations, correlated well with the traffic density, sampling locations were classified into three groups as follows: 1) ‘heavily polluted’ (heavy traffic); 2) ‘moderately polluted’ (medium traffic); or 3) ‘less polluted’ (low traffic density). Sampling sites located further from the road works, enclosed to the group ‘less polluted’, showed the lowest NO2 concentrations. The highest NO2 level was found for the locations close to reconstruction works, which belonged to the group ‘heavily polluted’. The contribution of NO2 was at the same level before and after the road works. During the first campaign it ranged from 30 ± 7 µg/m3 to 71 ± 11 µg/m3 and during the second sampling it was between 36 ± 17 µg/m3 and 73 ± 17 µg/m3. These modernization works had no impact on preventing the traffic-related pollutant as NO2 and as a consequence no significant effect on the air quality in the studied region. It has been proven that the impact of traffic on the air quality is unmistakably high and simply reduction of the number of the traffic lanes, intended to discourage the traffic flow, had apparently no environmentally advantageous effect.  相似文献   

15.
A method was developed for sampling and selective quantitative determination of typical volatile organic compounds (VOCs) in ambient urban air. A mobile and self-contained dual-channel air sampling tool based on solid phase adsorption was constructed. A simple calibration procedure circumventing the adsorption/desorption process was designed. The method was validated for seven “key-analytes”: n-hexane, 3-methyl-2-pentene, benzene, tetrachloroethene, styrene, 1,2,4-trimethylbenzene and acetophenone. The complete air sampling equipment is easily accommodated in a business suitcase. The lower limits of the practical working ranges are between 0.1 μg m–3 (tetrachloroethene) and 1.2 μg m–3 (benzene). Air samples were collected at a location in Salzburg with heavy motor vehicle traffic and measured in order to prove a satisfactory method performance under practical monitoring conditions.  相似文献   

16.
A simple, rapid and sensitive method was developed and validated for the analysis of C2–C5 volatile fatty acids (VFAs) in ambient air. This method involves preconcentration of VFAs with a sodium carbonate-impregnated silica gel tube, ultrasonic extraction with pure water, partition of VFAs to diethyl ether and determination using gas chromatography with a mass selective detector in the selected ion monitoring mode. A water-resistant free fatty acid phase capillary column was used to directly separate C2–C5 VFAs without the time-consuming derivatisation process. The limits of detection ranged from 0.001 to 0.003 µg m?3 and the limits of quantification ranged from 0.003 to 0.010 µg m?3. The validated method was successfully applied to the analysis trace-level VFAs in ambient air and in air samples from a landfill with perceived odour pollution.  相似文献   

17.
Most water contaminations with volatile organic compounds (VOCs) are traceable to leaking underground fuel reservoirs, solvent storage vessels, agricultural practices, industrial residues, and deficient wastewater treatment and disposal. In order to perform effective monitoring of such organic micropollutants in a straightforward manner, a multiresidue method for the determination of 23 VOCs (trihalomethanes (THMs), BTEX and chlorinated solvents) in water has been developed using solid-phase microextraction (SPME) and capillary gas chromatography–mass spectrometry (GC–MS). This group includes also methyl-tert-butyl ether, epichlorhydrine, and vinyl chloride which present additional analytical difficulties. Three different fibres were assayed: 7-µm polydimethylsiloxane (PDMS), 100-µm PDMS, and 75-µm Carboxen-PDMS, and the extraction conditions were optimized. The best results for the majority of the analytes and mainly for those with the lowest signals were obtained using the Carboxen-PDMS fibre after 15 min of extraction in the headspace mode at a room temperature of 20 ± 2°C. The analytical sensitivity, linearity, precision, accuracy, and uncertainties have been studied for method validation in agreement with the international standard ISO/IEC 17025:2005. The limits of detection achieved with the proposed method (0.06–0.17 µg L?1) are adequate to determine the VOCs at the restrictive levels established by the European legislation. This was a decisive achievement to enable the analysis of all VOCs listed under the drinking-water directive in a single assay. The method exhibits performance capabilities suitable for routine analysis of VOCs in drinking-water by quality-control laboratories as enforced by EU Directives. The method is currently being used for this purpose, and participation in proficiency tests was assessed, with encouraging results.  相似文献   

18.
This study describes the optimisation of an analytical method to determine 54 volatile organic compounds (VOCs) in air samples by active collection on multisorbent tubes, followed by thermal desorption and gas chromatography-mass spectrometry. Two multisorbent beds, Carbograph 1/Carboxen 1000 and Tenax/Carbograph 1TD, were tested. The latter gave better results, mainly in terms of the peaks that appeared in blank chromatograms. Temperatures, times and flow desorption were optimised. Recoveries were higher than 98.9%, except methylene dichloride, for which the recovery was 74.9%. The method's detection limits were between 0.01 and 1.25 μg m−3 for a volume sample of 1200 ml, and the repeatability on analysis of 100 ng of VOCs, expressed as relative standard deviation for n = 3, was lower than 4% for all compounds. Urban and industrial air samples from the Tarragona region were analysed. Benzene, toluene, ethylbenzene and xylenes (BTEX) were found to be the most abundant VOCs in urban air. Total VOCs in urban samples ranged between 18 and 307 μg m−3. Methylene chloride, 1,4-dichlorobenzene, chloroform and styrene were the most abundant VOCs in industrial samples, and total VOCs ranged between 19 and 85 μg m−3.  相似文献   

19.
The main aim of this study was to present the effects of barbecue smoke on a small-scale environment, a national park under the influence of intense barbecue smoke, and to scientifically support the sustainable usage of the park. Twelve-weekly bulk deposition samples were collected directly at the barbecuing area, and the samples were analysed for 16 US EPA’s priority PAH compounds and major ions. The mean concentrations of the individual PAHs in the bulk deposition samples ranged from 11.8 ng L?1 (Ane) to 1085 ± 581 ng L?1 (IcdP). The most frequently observed PAH compounds in the bulk deposition samples were Np, Anp, Flr, Phe, An, Flu, BkF, BaP and IcdP. The mean total PAH deposition fluxes were determined as 3.6 ± 5.6 µg m?2 day?1. The chloride, potassium and the sulphate fluxes were determined as 145.2 ± 267.8 µg m?2 day?1, 182.9 ± 291.9 µg m?2 day?1, and 111.9 ± 65.9 µg m?2 day?1, respectively. Dominant ions in the bulk deposition samples were potassium ion, chloride and sulphate which addressed as the fingerprint of barbecue grilling.  相似文献   

20.
Air quality monitoring could potentially improve exposure estimates for use in epidemiological studies. We investigated air quality by monitoring concentrations of 222Rn near the ground and particulate matter (PM) with an aerodynamic diameter less than or equal to 10 μm (PM10) and 2.5 μm (PM2.5) for Bucharest-Magurele periurban area. Atmospheric radon concentrations have been continuously monitored near the ground at 1 m height as well as at 10 m height. This paper presents time-series of radon concentrations monitoring in air near the ground measured during 1 January 2011–1 January 2012 by use of solid state nuclear track detectors SSNTD CR-39, exposed for 10 days periods. The daily average atmospheric radon concentration near the ground registered at 1 m height was found to be in range of 40.25 ± 7.53 Bq/m3, which was comparable with the daily average radon concentration of 44.92 ± 9.94 Bq/m3 recorded for period 1 August 2011–20 December 2011 at 10 m height by AlphaGUARD Radon monitor. Also, was done a comparative analysis of spatio-temporal variations in time series of outdoor radon concentration and PM in two size fractions (PM10 and PM2.5) in Bucharest Magurele area for 2011 year. The predominant recorded component in PM10 was PM2.5. Observational results show that recorded yearly average PM2.5 and PM10 concentrations were 35.96 μg/m3 and 40.91 μg/m3, respectively. The average ratio of PM2.5/PM10 was 87.9 % at this sampling site. However, in densely populated Bucharest urban and suburban areas the mean daily EC limit values for PM10, PM2.5 and attached 222Rn are frequently exceeded leading to serious public concern during the last years. The ambient air pollution measurements like as PM10 and PM2.5 levels are used as a proxy for personal exposure levels. Have been investigated also meteorological effects on the temporal patterns of atmospheric radon and particle matter.  相似文献   

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