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1.
In an effort to better quantify wintertime particulate matter (PM) and the contribution of wood smoke to air pollution events in Fresno, CA, a field campaign was conducted in winter 2003-2004. Coarse and fine daily PM samples were collected at five locations in Fresno, including residential, urban, and industrial areas. Measurements of collected samples included gravimetric mass determination, organic and elemental carbon analysis, and trace organic compound analysis by gas chromatograph mass spectrometry (GC/MS). The wood smoke tracer levoglucosan was also measured in aqueous aerosol extracts using high-performance anion exchange chromatography coupled with pulsed amperometric detection. Sample preparation and analysis by this technique is much simpler and less expensive than derivatized levoglucosan analysis by GC/MS, permitting analysis of daily PM samples from all five of the measurement locations. Analyses revealed low spatial variability and similar temporal patterns of PM2.5 mass, organic carbon (OC), and levoglucosan. Daily mass concentrations appear to have been strongly influenced by meteorological conditions, including precipitation, wind, and fog events. Fine PM (PM2.5) concentrations are uncommonly low during the study period, reflecting frequent precipitation events. During the first portion of the study, levoglucosan had a strong relationship to the concentrations of PM2.5 and OC. In the later portion of the study, there was a significant reduction in levoglucosan relative to PM2.5 and OC. This may indicate a change in particle removal processes, perhaps because of fog events, which were more common in the latter period. Combined, the emissions from wood smoke, meat cooking, and motor vehicles appear to contribute approximately 65-80% to measured OC, with wood smoke, on average, accounting for approximately 41% of OC and approximately 18% of PM2.5 mass. Two residential sites exhibit somewhat higher contributions of wood smoke to OC than other locations.  相似文献   

2.
A winter PM2.5 episode that achieved a maximum 24-h average of 138 μg m−3 at the Fresno Supersite in California's San Joaquin Valley between 2 and 12 January, 2000 is examined using 5-min to 1-h continuous measurements of mass, nitrate, black carbon, particle-bound PAH, and meteorological measurements. Every day PM2.5 sampling showed that many episodes, including this one, are missed by commonly applied sixth-day monitoring, even though quarterly averages and numbers of US air quality standard exceedances are adequately estimated. Simultaneous measurements at satellite sites show that the Fresno Supersite represented PM2.5 within the city, and that half or more of the urban concentrations were present at distant, non-urban locations unaffected by local sources. Most of the primary particles accumulated during early morning and nighttime, decreasing when surface temperatures increased and the shallow radiation inversion coupled to a valleywide layer. When this coupling occurred, nitrate levels increased rapidly over a 10–30 min period as black carbon and gaseous concentrations dropped. This is consistent with a conceptual model in which secondary aerosol forms above the surface layer and is effectively decoupled from the surface for all but the late-morning and early afternoon period. Primary pollutants, such as organic and black carbon, accumulate within the shallow surface layer in urban areas where wood burning and vehicle exhaust emissions are high. Such a model would explain why earlier studies find nitrate concentrations to be nearly the same among widely separated sites in urban areas, as winds aloft of 1 to 6 m s−1 could easily disperse the elevated aerosol throughout the valley.  相似文献   

3.
ABSTRACT

As part of a pilot study into the chemical and physical properties of Australian fine particles, a suite of aerosol samples was collected at Ti Tree Bend in Launceston, Tasmania, during June and July 1997. This period represents midwinter in the Southern Hemisphere, a period when aerosol sources in Launceston are dominated by smoke from domestic wood burning. This paper describes the results from this measurement campaign, with the aim of assessing the effect of wood smoke on the chemical and physical characteristics of ambient aerosol. A micro orifice uniform deposit impactor (MOUDI) was used to measure the size distributions of the aerosol from 0.05 to 20 n m aerodynamic diameter. Continuous measurements of fine particle mass were made using a PM2.5 tapered element oscillating microbalance (TEOM) and light scattering coefficients at 530 nm were measured with nephelometers.

Mass size distributions tended to be bimodal, with the diameter of the dominant mode tending to smaller sizes with increases in total mass. Non-sea salt potassium and polycyclic aromatic hydrocarbons (PAHs) were used as chemical tracers for wood smoke. Wood smoke was found to increase absolute particle mass (enough to regularly exceed air quality standards), and to concentrate mass in a single mode below 1 μm aerodynamic diameter. The acid-base equilibrium of the aerosol was altered by the wood smoke source, with free acidity hydrogen ion, non-sea salt sulfate, and ammonium concentrations being higher and the concentration of all species, including nitrate (to differing extents), focused in the fine particle size ranges. The wood smoke source also heavily influenced the aerosol scattering efficiency, adding to a strong diurnal cycle in both mass concentration and light scattering.  相似文献   

4.
Abstract

Air quality data collected in the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) are analyzed to qualitatively assess the processes affecting secondary aerosol formation in the San Joaquin Valley (SJV). This region experiences some of the highest fine particulate matter (PM2.5) mass concentrations in California (≤188 μg/m3 24-hr average), and secondary aerosol components (as a group) frequently constitute over half of the fine aerosol mass in winter. The analyses are based on 15 days of high-frequency filter and canister measurements and several months of wintertime continuous gas and aerosol measurements. The phase-partitioning of nitrogen oxide (NOx)-related nitrogen species and carbonaceous species shows that concentrations of gaseous precursor species are far more abundant than measured secondary aerosol nitrate or estimated secondary organic aerosols. Comparisons of ammonia and nitric acid concentrations indicate that ammonium nitrate formation is limited by the availability of nitric acid rather than ammonia. Time-resolved aerosol nitrate data collected at the surface and on a 90-m tower suggest that both the daytime and nighttime nitric acid formation pathways are active, and entrainment of aerosol nitrate formed aloft at night may explain the spatial homogeneity of nitrate in the SJV. NOx and volatile organic compound (VOC) emissions plus background O3 levels are expected to determine NOx oxidation and nitric acid production rates, which currently control the ammonium nitrate levels in the SJV. Secondary organic aerosol formation is significant in winter, especially in the Fresno urban area. Formation of secondary organic aerosol is more likely limited by the rate of VOC oxidation than the availability of VOC precursors in winter.  相似文献   

5.
Abstract

Air pollutants were collected in Logan, Cache County, UT, in February 1993 during two periods of atmospheric inversion accompanied by fog. The following atmospheric species were determined: (1) gaseous SO2, NO2 (semi-quantitatively),HNO3, NH3, and HF; (2) fine particulate SO4 =, NO3 -, NH4 +, F–, H+, C, Si, S, K, Ca, Ti, Mn, Fe, Ni, Cu, Zn, Pb, Se, Br, and Sr, and; (3) fine particulate mass, which was calculated. The major components of fine particulate matter were carbonaceous material, ammonium nitrate, and ammonium sulfate, while the soil component was small. Calculated, fine particulate mass averaged 80 μg/m3 and reached concentrations as high as 120 μg/m3. SO2/Sox and NO2/NOy mole ratios generally varied between 0.2 and 0.1 during inversions. These ratios also showed moderate but consistent diurnal patterns. The emission inventory for Cache County indicates sources of SO2 and NOx but not significant amounts of primary sulfate and nitrate. The observations reported here indicate there is significant conversion of SO2 and NOx in the presence of excess oxidants to sulfuric and nitric acid that are neutralized by excess ammonia.  相似文献   

6.
Abstract

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 µm or less in aerodynamic diameter (PM2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO4 2?], nitrate [NO3 ?], ammonium [NH4 +]), metals, and metal oxides and compared with the measured PM2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and β-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12–42 µg m?3. Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.  相似文献   

7.
ABSTRACT

The organic fraction of aerosol emitted from a vegetable oil processing plant was studied to investigate the contribution of emissions to ambient particles in the surrounding area. Solvent-soluble particulate organic compounds emitted from the plant accounted for 10% of total suspended particles. This percentage was lower in the receptor sites (less than 6% of total aerosol mass). Nonpolar, moderate polar, polar, and acidic compounds were detected in both emitted and ambient aerosol samples. The processing and combustion of olive pits yielded a source with strong biogenic characteristics, such as the high values of the carbon preference index (CPI) for all compound classes. Polycyclic aromatic hydrocarbons (PAHs) detected in emissions were associated with both olive pits and diesel combustion. The chromatographic profile of dimethyl-phenanthrenes (DMPs) was characteristic of olive pit combustion. Organic aerosols collected in two receptor sites provided a different pattern.

The significant contribution of vehicular emissions was identified by CPI values (~1) of n-alkanes and the presence of the unresolved complex mixture (UCM). In addition, PAH concentration diagnostic ratios indicated that emissions from catalyst and noncatalyst automobiles and heavy trucks were significant. The strong even-to-odd predominance of n-alkanols, n-alkanoic acids, and their salts indicated the contribution of a source with biogenic characteristics. However, the profile of DMPs at receptor sites was similar to that observed for diesel particulates. These differences indicated that the contribution of vegetable oil processing emissions to the atmosphere was negligible.  相似文献   

8.
Oxygenated additives in gasoline are designed to decrease the ozone-forming hydrocarbons and total air toxics, yet they can increase the emissions of aldehydes and thus increase human exposure to these toxic compounds. This paper describes a study conducted to characterize targeted aldehydes in microenvironments in Sacramento, CA, and Milwaukee, WI, and to improve our understanding of the impact of the urban environment on human exposure to air toxics. Data were obtained from microenvironmental concentration measurements, integrated, 24-h personal measurements, indoor and outdoor pollutant monitors at the participants' residences, from ambient pollutant monitors at fixed-site locations in each city, and from real-time diaries and questionnaires completed by the technicians and participants. As part of this study, a model to predict personal exposures based on individual time/activity data was developed for comparison to measured concentrations. Predicted concentrations were generally within 25% of the measured concentrations. The microenvironments that people encounter daily provide for widely varying exposures to aldehydes. The activities that occur in those microenvironments can modulate the aldehyde concentrations dramatically, especially for environments such as “indoor at home.” By considering personal activity, location (microenvironment), duration in the microenvironment, and a knowledge of the general concentrations of aldehydes in the various microenvironments, a simple model can do a reasonably good job of predicting the time-averaged personal exposures to aldehydes, even in the absence of monitoring data. Although concentrations of aldehydes measured indoors at the participants' homes tracked well with personal exposure, there were instances where personal exposures and indoor concentrations differed significantly. Key to the ability to predict exposure based on time/activity data is the quality and completeness of the microenvironmental characterizations for the chemicals of interest. Consistent with many earlier studies, personal exposures are difficult to predict using data from regional outdoor monitors.  相似文献   

9.
Abstract

Levels of the monosaccharide anhydride (MA) levoglucosan and its isomeric compounds galactosan and mannosan were quantified in the PM10 fraction (particulate matter ≤10 µm in aerodynamic diameter) of ambient aerosols from an urban (Oslo) and a suburban (Elverum) site in Norway, both influenced by small-scale wood burning. MAs are degradation products of cellulose and hemicellulose, and levoglucosan is especially emitted in high concentrations during pyrolysis and combustion of wood, making it a potential tracer of primary particles emitted from biomass burning. MAs were quantified using a novel high-performance liquid chromatography/ high-resolution mass spectrometry-time of flight method. This approach distinguishes between the isomeric compounds of MAs and benefits from the limited sample preparation required before analysis, and no extensive derivatization step is needed. The highest concentrations of levogucosan, galactosan, and mannosan (∑MA) were recorded in winter because of wood burning for residential heating (∑MAMAX = 1,240 ng m-3). This finding was substantiated by a relatively high correlation (R2 = 0.64) between the levoglucosan concentration and decreasing ambient temperature. At the suburban site, ∑MA accounted for 3.1% of PM10, whereas the corresponding level at the urban site was 0.6%. The mass size distribution of MAs associated with atmospheric aerosols was measured using a Berner cascade impactor. The size distribution was characterized with a single mode at 561 nm. Ninety-five percent of the mass concentration of the MAs was found to be associated with particles <2 µm. A preliminary attempt to estimate the contribution of wood burning to the mass concentration of PM10 in Oslo using levoglucosan as a tracer indicates that 24% comes from wood burning. This is approximately a factor of 2 lower than estimated by the AirQUIS dispersion model.  相似文献   

10.
As a part of the effort to understand the structure of long-range transported aerosol plumes and local pollution, aerosol observations monitored the mass concentrations and number-size distributions during the period August 2006 to July 2009 near the top of Mt. Haruna (1365 m), an isolated mountain in the Kanto Plain in Japan. The mass concentrations observed at Mt. Haruna and plain sites showed a seasonal variation with a maximum in spring and summer, respectively. The spring peaks in aerosols at Mt. Haruna were probably caused by long-range transport of mineral dust and anthropogenic particles from the Asian continent. The summer peaks at the plain sites was attributed to local pollution from the Tokyo metropolitan area. Three examples of 2007 Asian dust events were investigated to show that aerosols may be dispersed in a complicated three-dimensional structure and that delayed arrivals of the dust plumes at plain sites compared to Mt. Haruna were not a rare case. Because of the boundary layer being stable at night, the dust layer was advected eastward without the vertical mixing before sunrise. This study suggests that after thermal convection activated by sunlight during daytime Asian dust transported in the free troposphere may be brought down into the atmospheric boundary layer, increasing the dust concentration there.  相似文献   

11.
Chemical characteristics of aerosol and rainfall samples collected at five sites in Minnesota and one site in west-central Wisconsin during the summer of 1982 were generally similar with respect to the relative proportions of major constituents. The most abundant species measured in the aerosol was sulfate, occurring predominantly in the fine fraction ( < 2.5 μm aerodynamic diameter). The rain chemistry was also dominated by sulfate but not to the same extent as the aerosol. The concentrations of crustal materials in both the aerosol and the rain followed a gradient in which concentrations increased with proximity of the sampling site to the prairie. The concentrations of crustal materials in the aerosol were correlated with their concentrations in subsequent rain, whereas concentrations of other constituents were not significantly correlated between aerosol and rain. Since the aerosol was sampled at the surface this result provided evidence that crustal materials were transported at lower altitudes and were scavenged to a greater degree by below-cloud mechanisms. The measured components in aerosols were divided by factor analysis into: ammonium sulfates, crustal materials, and a group containing nitrates, metals and other materials.  相似文献   

12.
Abstract

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During our study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition of Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Our results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 μm, corresponding with the wavelength region of visible light, which accounted for ~72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH4)2SO4, NH4NO3, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein.  相似文献   

13.
Time variations of soiling index measurements obtained from three AISI smoke samplers located in Central Montreal during the period January I960-April 1963 are analyzed. A marked seasonal cycle is found, with midwinter smokiness two to three times midsummer values. The mean value at an elevation of 600 ft on the summit of ML Royal is only 21% of that in the city below. A 46% reduction in smoke is also observed at the location adjacent to the large Mt. Royal Park. The. average weekend reduction in smoke is approximately 20% with a significant change in the diurnal pattern on Sunday. There are two basic types of weekday daily cycle. A winter type with small amplitude, and morning and evening maxima of similar magnitude; a secondary late evening peak is also noted. A summer type with large amplitude and a marked morning maximum. The time of morning peak at the upper station lags behind the lower stations by 2-3 hr in the winter, but in the summer the peaks occur almost simultaneously. These two types are related to the interaction of the daily cycles in both smoke production and ventilation of the city’s atmosphere.  相似文献   

14.
15.
Atmospheric precipitation samples have been collected at six sites in the London (U.K.) area and at one rural site. Levels of lead and cadmium have been determined and are readily related to local sources of air pollution. A quantitative assessment is made of the metallic pollution resulting from removal of metals from the atmosphere In precipitation and it is compared to the contribution of other pollution pathways.  相似文献   

16.
The General Motors Research Laboratories and the Sloan-Kettering Institue for Cancer Research are collaborating to determine the contribution by automotive vehicles to the polynuclear aromatic hydrocarbons in city air. Sampling of particulate matter at the rate of 140 M3/min (5000 cfm) was carried out at two heavily-trafficked sites in Detroit and one suburban site in Warren, Michigan. Carbon monoxide was determined continuously, and particulate matter was analyzed for “tar,” polynuclear aromatic hydrocarbons, lead, vanadium, and sulfates. Polynuclear aromatic hydrocarbons in automobile exhaust gas are assumed to be dispersed in air along with carbon monoxide or lead from automobiles. It is further assumed that automobiles are the sole source of carbon monoxide and lead in the atmosphere. Concentrations of carbon monoxide and lead in exhaust gas and in the air are utilized to estimate the percentage of polynuclear aromatic hydrocarbons in the air attributable to automobiles. The mean automobile contributions to benzo(a)pyrene in the air, based on lead concentrations, were 18% at a Freeway Interchange, 5% in a downtown commercial area, and 42% in suburban Warren. The average concentrations of benzo(a)pyrene at the sites were 6 μg/103 M3, 7 μg/103 M3 and 1 μg/103 M3, respectively. Mean contributions based on carbon monoxide concentrations were approximately twice the levels based on lead concentrations. Benzo(a)pyrene and benz(a)anthracene in air were not statistically related to carbon monoxide or lead in air, but were higher in winter than in summer, probably because of the higher levels of these materials emitted in space heating combustion in winter.  相似文献   

17.
To demonstrate a method for the identification of mutagenic components in organic fractions of ambient aerosols, the mutagenic activity was studied in samples collected simultaneously for six consecutive days during the summer of 1931 at an urban site and a suburban site in southeast Michigan. The filter samples were extracted with dichloromethane and fractionated by thin layer chromatography (TLC) into sixteen fractions. The individual TLC fractions were then examined by the Ames test using tester strains TA98, TA98NR and TA98DNP6. Similar daily variations in the activity and the mutagenicity profiles of the TLC fractions occurred at both sites. In samples collected from both locations, approximately half of the mutagenic activity was found in the four most polar fractions of the particulate extracts. The remaining mutagenic activity was distributed among the less polar fractions where PAH, nitro-PAH and dinitro-PAH would be eluted. The mutagenic activity in all fractions decreased sharply when tested with two nitroreductase deficient tester strains, TA98NR and TA98DNP6, indicating that the mutagens (especially those in the polar fractions) were nitro-substituted polycyclic aromatic hydrocarbon compounds. Three nitro compounds, 1-nitropyrene, 1,6-dinitropyrene and 1,8-dinitropyrene were detected by high performance liquid chromatography (HPLC) but could account for no more than 3% of the total airborne mutagenicity. A National Bureau of Standards' Ambient Particulate Sample (SRM No. 1649), collected for a long sampling period of 18 months, differed markedly from the urban and suburban Michigan samples in its mutagenicity profile.  相似文献   

18.
Data on the adsorption and transformation rates of diazinon, parathion, tetrachlorvinphos and triazophos in soils were collected from a survey of the literature. As little information is available on their mobility, the adsorption of tetrachlorvinphos and triazophos on three soils was measured in a slurry experiment. Properties of diazinon were introduced into a computer model simulating glasshouse soil systems in a simplified way. The leaching of diazinon from the root zone was calculated to be zero. The properties of the other three organophosphates indicate that in similar computations leaching from the root zone would have been even lower.Samples from tile drains and water courses in areas with many glasshouses were analysed by gas-liquid chromatography. The concentration of the four organophosphate insecticides in almost all of the samples of water from tile drains was below the detectable limit. However in samples from the water courses, pesticide residues were found regularly, sometimes at fairly high concentrations. Thus contamination of water courses would seem to be produced not by leaching of pesticides through the soil but by other pathways.  相似文献   

19.
Rapid expansion of coastal anthropogenic development means that critical foraging and developmental habitats often occur near highly polluted and urbanized environments. Although coastal contamination is widespread, the impact this has on long-lived vertebrates like the green turtle (Chelonia mydas) is unclear because traditional experimental methods cannot be applied. We coupled minimally invasive sampling techniques with health assessments to quantify contaminant patterns in a population of green turtles resident to San Diego Bay, CA, a highly urbanized and contaminated estuary. Several chemicals were correlated with turtle size, suggesting possible differences in physiological processes or habitat utilization between life stages. With the exception of mercury, higher concentrations of carapace metals as well as 4,4′-dichlorodiphenyldichloroethylene (DDE) and γ chlordane in blood plasma relative to other sea turtle studies raises important questions about the chemical risks to turtles resident to San Diego Bay. Mercury concentrations exceeded immune function no-effects thresholds and increased carapace metal loads were correlated with higher levels of multiple health markers. These results indicate immunological and physiological effects studies are needed in this population. Our results give insight into the potential conservation risk contaminants pose to sea turtles inhabiting this contaminated coastal habitat, and highlight the need to better manage and mitigate contaminant exposure in San Diego Bay.  相似文献   

20.
NASA is examining Space Shuttle launch impacts. Solid rocket exhaust includes ?60 tons HCL and ?87 tons alumina particles emitted below 2.5 km, of which 50-80% forms an altitude stabilized exhaust cloud (EC). Several 60% smaller Titan-Ill EC were sampled by aircraft for this study. Three distinct features are presented: (a) An analysis of HCL (gaseous plus aqueous) data traces. Total range of peak HCL was 25-0.5 ppm (3-300 min) for 8 EC. Power-law decays of peak HCL applied. Calculated HCL dispersions for 7 standard meteorologies are also shown, (b) An analysis of simultaneous HCL (g), HCL (g + aq) data for 2 EC. Vapor-liquid HCL/H2O equilibria were calculated for a flat surface aqueous aerosol. HCL partitioning varied with EC dilution and H2O content. HCL (aq) and aqueous mass fraction maximized early at >3 molal and >0.1 mg/g air. Calculated H2O (g + aq) compared favorably with independent EC measurements, (c) An analysis of wet deposition after EC interception at ?30 min by a convective storm. A 28 km2 acid chloride (1 < pH < 3) footprint was defined. In conclusion, (a) HCL dispersion in large EC tends to follow power-law decay, but HCL concentration may vary widely (100 times after 1 h) with meteorology, (b) HCL (g/aq) and H2O (g/aq) partitioning is consistent with equilibrated acid aerosol compositions, and (c) localized deposition of highly acidic rain may occur sometimes.  相似文献   

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