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1.
The objective of this work is to analyze Fe, Mn, Cr, Cd, Cu, Pb, and Zn distributions in the water column in terms of total, dissolved, and particulate concentrations in the Salado River (Santa Fe – Argentina); their relationship with total, dissolved and suspended solids; and the impact of two pollution sources on the watercourse: a stream that collects domestic and industrial wastewater discharges of the region and a direct discharge that releases urban and industrial effluents to the river. Water samples obtained from 5 surveys were analyzed. The Salado River transported a load of heavy metals that ranged from 700 g/s to 2200 g/s of Fe, 20 g/s to 60 g/s of Mn and 1 g/s to 3 g/s of Cr. Results show that most metals were found in particulate form, that the metal input from the direct discharge may be significant at low water levels, whereas a lesser impact was produced by the stream, and that both pollution sources were negligible at high water levels.  相似文献   

2.
The speciation of mercury (Hg) in Minamata Bay (Japan) was studied over a 2-year period (2006?C2008). Concentrations of dissolved total Hg, dissolved methylmercury (MeHg), particulate total Hg, and suspended solids were 0.43?±?0.14 ng/l (mean?±?standard deviation), 0.10?±?0.06 ng/l, 3.04?±?2.96 ng/l, and 5.94?±?2.10 mg/l, respectively. Correlations between concentrations of particulate total Hg and suspended solids at four depths (surface: 0 m; mid-depth: ?6 m, ?10 m; and bottom +1 m layer) were only significant in the bottom +1 m layer. The mean dissolved MeHg concentration and the ratio of dissolved MeHg to dissolved total Hg were considerably higher in summer compared to other seasons. The data suggest that bottom sediment was not the sole source of MeHg, and that MeHg may be produced in the water column by the conversion of divalent Hg eluted from resuspended bottom sediment. The correlation between seawater characteristics such as salinity, temperature, dissolved oxygen (DO), and dissolved MeHg concentration indicates that Hg methylation could be influenced by the heterotrophic activity of microorganisms in the seawater. In particular, inverse correlations were observed between DO, salinity, and MeHg concentration. However, dissolved MeHg concentrations did not correlate with seawater characteristics such as pH or chlorophyll-a.  相似文献   

3.
Dissolved and particulate mercury distributions were determined in the three largest Siberian rivers and in adjacent Arctic coastal waters during two cruises. Water samples were collected in the Lena River and its mixing zone in the Laptev Sea in September 1991, and in the Ob and Yenisei Rivers and the adjacent Kara Sea in September 1993. Average total dissolved Hg concentration was 5.0 pM in the Lena River, 2.8 pM in the Ob River and 1.5 pM in the Yenisei River. Mercury content of suspended particulate matter was low, averaging 0.17 mg kg?1 in the Lena and 0.05 mg kg?1 in the Ob and Yenisei Rivers. These concentrations are lower than those observed in other world rivers affected by local input of man-made origin. In the estuarine mixing zones, higher concentrations of dissolved and particulate Hg which may originate from the spring flood were found. The carbon cycle is apparently a driving mechanism for Hg distribution in Arctic coastal waters. Particulate Hg content was positively correlated with the content of organic matter of the particles. In the Kara Sea, uptake by phytoplankton is suspected to be responsible for the increase in particulate Hg levels. Mercury fluxes from the three rivers to the Arctic Shelf are estimated and compared to direct atmospheric inputs.  相似文献   

4.
A number of closely related acid digestion procedures are proposed for the accurate analysis of animal tissue, plant tissue, sediment and particulate samples. A closed teflon vessel is employed to reduce contamination and to speed up digestion. Procedures which minimize evaporations should be employed where applicable. Hydrofluoric acid is essential when plant tissue, sediment and particulate material are to be dissolved. Accuracy and precision is assessed using standard reference samples.  相似文献   

5.
Mechanisms of Phosphorus Control in Urban Streams Receiving Sewage Effluent   总被引:1,自引:0,他引:1  
Urban streams often are a major source of phosphorus (P) to rivers, primarily due to large inputs of sewage effluent. A good example of this is Chicago (Illinois, USA) area streams, which make up most of the flow of the upper Illinois River. Even though streams in this section of the Mississippi River basin are characteristic hard-water systems and exhibit high calcium and carbonate concentrations, the precipitation of Ca–P minerals is minimal and phosphate is not removed from the water column. The objective of this study was to determine the chemical mechanisms controlling P activity in Chicago area streams. Measurement of dissolved ion activities on filtered surface water samples demonstrated that an average of 79% of P in the study streams was dissolved and the remaining was particulate (<0.05 μm and >1.0 μm in diameter, respectively). Neither a P colloidal-size fraction nor a correlation between dissolved and particulate Fe and P was observed. Thermodynamic modeling and SEM-EDS analysis of particulate matter in filter residues indicated that dissolved P may adsorb and co-precipitate on the surface of calcite rather than precipitating in a pure Ca–P mineral phase. Although SEM-EDS results also suggested that P was adsorbed to silicate minerals, organic residues likely dominated the P-containing particulate fraction. Sediment extraction results indicated that organic P was one of two major P components in the stream bottom. The Fe-associated P fraction represented the largest sediment-P fraction, and with little association between Fe and P in the overlying water, dissolved inorganic P may have aided in the authigenic formation of an Fe–P sediment phase. Overall, results suggest that pH combined with Ca and Mg activity are the dominant chemical controls on P chemistry in this P enriched system.  相似文献   

6.
Gold-coated denuders have been used to separate gas phase and particulate phase Hg in air samples. The denuders were 65 cm long with a 0.4 cm i.d. and were capable of removing >99.9% of the vapor phase elemental Hg in an air stream at flow rates of about 1 L min?1. Data were obtained at different sampling locations around the city of Göteborg. The concentration of particulate Hg was found to be within the range of 0.11 to 0.57 ng m?3, which corresponds to 2.8 to 16.9% of the total airborne Hg. Positive correlations between the concentration of particulate Hg and that of soot and suspended particles as well as a negative correlation between the concentration of particulate Hg and relative humidity were observed.  相似文献   

7.
The upper Great Egg Harbor River watershed in New Jersey’s Coastal Plain is urbanized but extensive freshwater wetlands are present downstream. In 2006–2007, studies to assess levels of total mercury (THg) found concentrations in unfiltered streamwater to range as high as 187 ng/L in urbanized areas. THg concentrations were <20 ng/L in streamwater in forested/wetlands areas where both THg and dissolved organic carbon concentrations tended to increase while pH and concentrations of dissolved oxygen and nitrate decreased with flushing of soils after rain. Most of the river’s flow comes from groundwater seepage; unfiltered groundwater samples contained up to 177 ng/L of THg in urban areas where there is a history of well water with THg that exceeds the drinking water standard (2,000 ng/L). THg concentrations were lower (<25 ng/L) in unfiltered groundwater from downstream wetland areas. In addition to higher THg concentrations (mostly particulate), concentrations of chloride were higher in streamwater and groundwater from urban areas than in those from downstream wetland areas. Methylmercury (MeHg) concentrations in unfiltered streamwater ranged from 0.17 ng/L at a forest/wetlands site to 2.94 ng/L at an urban site. The percentage of THg present as MeHg increased as the percentage of forest + wetlands increased, but also was high in some urban areas. MeHg was detected only in groundwater <1 m below the water/sediment interface. Atmospheric deposition is presumed to be the main source of Hg to the wetlands and also may be a source to groundwater, where wastewater inputs in urban areas are hypothesized to mobilize Hg deposited to soils.  相似文献   

8.
Abstract

Rapid and accurate determination of low‐level (0.01 to 1.0 mg L?1) phosphorus (P) concentrations in farm canal water is important in evaluating water quality in the Everglades Agricultural Area (EAA) canals in south Florida. Two U.S. Environmental Protection Agency methods, persulfate digestion (365.1) and Kjeldahl digestion with mercury oxide (365.4), were used to analyze total P (TP) and total dissolved P (TDP) in two sets of representative canal water samples collected at low‐flow conditions in 2003 and high‐flow conditions in 2004. Quality assurance samples (blanks, duplicates, and spikes) were included to evaluate differences between the two digestion methods. Precision analysis had a mean of less than 5% for both TP and TDP using both methods. The high coefficient of correlations (r>0.98) indicated that the two methods were significantly correlated in determining TP and TDP of the samples. Low detection limits (0.004 mg L?1) were achieved by the persulfate method. This method offers many other advantages over the mercury digestion: it produces no toxic mercury waste, uses less time, and uses a lower temperature. High suspended solids in canal water samples were not proven to be a problem when using the persulfate digestion, though lower spike recoveries were observed than those when using the mercury digestion. We conclude that persulfate digestion is a more sensitive and environmentally responsible alternative to and is, as precise as, the mercury method for routine determination of TP and TDP in water samples. This information is useful to environmental laboratories in monitoring P concentrations in surface and groundwater.  相似文献   

9.
Although many sources of Hg to surface waters have been identified including atmospheric deposition, resuspension of contaminated sediments, and direct discharges, there are very few recent data on ambient concentrations in the large lakes. Thus, an investigation of Hg concentrations in Lake Champlain and Lake Michigan was completed in the summer of 1993. Three depths of water including the microlayer, 30 cm below the surface, and 1 m below the thermocline were collected for each sampling event using ultra-clean techniques. All samples were processed in the field for dissolved and particulate fractions in a portable plastic enclosure equipped with a HEPA filter, and then analyzed by dual amalgamation and cold vapor atomic fluorescence spectroscopy in a Class 100 clean room at the University of Michigan. In addition, samples were analyzed for other trace metals by ICP-MS. Results from the two field investigations include the following: (1) On average, Lake Michigan water samples had higher concentrations of Hg than Lake Champlain; (2) There was no consistent pattern of Hg concentrations in the water column; (3) There was variability in the concentrations of Hg from the same depths over consecutive sampling periods. This paper discusses these results, and examines the relationship between the patterns in mercury concentrations and other physical and chemical data collected during the investigation.  相似文献   

10.
改良剂降低富磷蔬菜地土壤磷和氮流失的作用   总被引:3,自引:1,他引:3  
为了解不同改良剂对土壤中磷和氮的稳定作用,进行田间试验研究在施用量为2.5t/hm2时氢氧化铝、石灰石粉、石膏、氯化钙和粉煤灰5种改良剂对蔬菜地地表径流中磷和氮浓度的影响。结果表明,改良剂施用可明显降低土壤有效磷和水溶性磷含量,轻微增加土壤中NH4+-N含量,但对土壤中NO3--N影响不大。施用改良剂可显著降低蔬菜地地表径流中总磷、溶解态磷、颗粒态磷和NH4+-N的浓度,增加水溶性有机氮浓度,但对水溶性总氮和NO3--N浓度影响不明显。与对照比较,施用氢氧化铝、石灰石粉、石膏、氯化钙和粉煤灰5种改良剂的地表径流中总磷浓度下降比例平均分别为13.68%,35.54%,38.72%,43.77%和45.02%,溶解态磷浓度下降比例平均分别为16.05%,32.42%,48.75%,55.38%和38.98%;NH4+-N浓度下降比例平均分别为24.21%,37.84%,11.31%,10.08%和55.56%。总体上,施用氯化钙和粉煤灰降低地表径流中磷浓度的效果好于其他改良剂。  相似文献   

11.
A mass balance model was developed to simulate mercury (Hg) cycling in Onondaga Lake, New York. MERC4, a U.S. Environmental Protection Agency model of the physical and biogeochemical transport and transformation of Hg, was modified by the addition of input from two supporting models (Fish Bioenergetics Model 2 and a lake eutrophication model) to model the transport of Hg into and out of plankton and fish. The model calculates the concentrations of total Hg, methylmercury, elemental Hg, and ionic Hg in both dissolved and particulate forms in the water column. The model was calibrated to an extensive data set of temporally and spatially variable Hg concentrations in Onondaga Lake in 1992. In addition to standard transport processes of advection and dispersion included in MERC4, the Onondaga Lake Mercury Model includes remineralization to simulate release of Hg from settling particulates before incorporation into sediment. The model provides an analytical framework for understanding and predicting the behavior of Hg in Onondaga Lake and has potential use in evaluating the relative impact of different source control and remedial alternatives.  相似文献   

12.
Research on mercury (Hg) distribution and speciation was carried out in Lake Baikal, a large, strong-oligotrophic freshwater reservoir in Siberia, Russia, during June 1992 and march 1993. In summer, total Hg in the water column ranged from 0.14 to 0.77 ng Hg/L, with the highest concentrations observed in the central basin of the lake in surface water samples. Labile inorganic Hg was found to be 7 to 20 % of the total Hg content. Highest total Hg concentrations were found in river waters: up to 2 ng Hg/L. Labile methylmercury (MeHg) concentrations ranged from 2 to 38 pg Hg/L in the water column, with the higher concentrations in the central part of the lake, and showing a slight increase in near bottom waters. Labile MeHg makes up 1 to 15 % of the total Hg content in the water column, with larger fractions in deep waters. The slight increase of the MeHg gradient with depth corresponds with the O2 minimum region. Highest MeHg concentrations were observed in river waters (up to 145 pg Hg/L) and in some bays of the lake (up to 160 pg Hg/L). In these high temperature- and phytoplankton-rich water masses, the MeHg-fraction increased up to 35 % of total Hg. Labile MeHg concentrations in water samples taken in winter in the southern basin (under the ice cover), showed slightly higher concentrations than in summer, possibly due to an early spring bloom. In rainwater, total Hg ranged from 3 to 20 ng Hg/L and MeHg from 0.1 to 0.25 ng Hg/L. In snow, a large fraction of total Hg is bound to particulate matter; concentrations of total Hg ranged from 8 to 60 ng Hg/L and labile MeHg from 0.1 to 0.25 ng Hg/L. Atmospheric Hg was found to be 0.73 to 2.31 ng/m3 as gaseous Hg and 0.005 to 0.02 ng/m3 in its particulate form. Spatial distribution patterns of atmospheric Hg show slightly higher concentrations over the central part of the lake and the Selenga river delta. In winter, atmospheric Hg values (measured in the southern region), ranged from 1.2 to 6.1 ng/m3 as total gaseous Hg and 0.02 to 0.09 ng/m3 as total particulate Hg, and are higher than in summer, probably influenced by coal burning and traffic by the local population. MeHg contents in fish ranged from 20 ng Hg/g dry weight in small Cottocomephorus to 300 ng Hg/g dry weight in pike and trout species, which were caught in organic-rich waters.  相似文献   

13.
An automatic flow-batch system that includes two borosilicate glass chambers to perform sample digestion and cold vapor atomic absorption spectroscopy determination of mercury in honey samples was designed. The sample digestion was performed by using a low-cost halogen lamp to obtain the optimum temperature. Optimization of the digestion procedure was done using a Box-Behnken experimental design. A linear response was observed from 2.30 to 11.20 μg Hg L(-1). The relative standard deviation was 3.20% (n = 11, 6.81 μg Hg L(-1)), the sample throughput was 4 sample h(-1), and the detection limit was 0.68 μg Hg L(-1). The obtained results with the flow-batch method are in good agreement with those obtained with the reference method. The flow-batch system is simple, allows the use of both chambers simultaneously, is seen as a promising methodology for achieving green chemistry goals, and is a good proposal to improving the quality control of honey.  相似文献   

14.
The Tekran 2537A mercury vapour analyser, designed to measure Hg in air by cold vapour atomic fluorescence spectrometry, has been modified to determine Hg in solution. The new ‘front-end’, required to generate Hg° vapour from acidified waters or acid leachates, is described. Using 1% NaBH4 as reducing agent, a 12 mL water sample can be analysed, at a rate of 1 every 6 min, for Hg to a detection limit of 0.8 ppt (ng L-1). Instrumental precision is typically 1% relative standard deviation (RSD) at levels of Hg from 10 to 200 ppt. Results for 10 analyses of the international water standard, NIST 1642b, are 1530±20 ppt Hg, agreeing well with the certified value of 1480±130 ppt. Nineteen geological standard reference materials (soils, sediments and tills) were used to assess accuracy. Results for these samples, digested in aqua regia in triplicate, showed good agreement with recommended values for all but two, SO-3 and TILL-1. However, results by this method for these two standards were confirmed by an independent method, direct atomic absorption spectrometry. Average method precision was shown to be 5% RSD over the range 10 ng g- 1 to 35 μg g-1 Hg.  相似文献   

15.
Different species of mercury have different physical/chemical properties and thus behave quite differently in air pollution control equipment and in the atmosphere. In general, emissions of mercury from coal combustion sources are approximately 20–50% elemental mercury (Hg°) and 50–80% divalent mercury (Hg(II)), which may be predominantly HgCl2. Emissions of mercury from waste incinerators are approximately 10–20% Hg° and 75–85% Hg(II). The partitioning of mercury in flue gas between the elemental and divalent forms may be dependent on the concentration of particulate carbon, HCl and other pollutants in the stack emissions. The emission of mercury from combustion facilities depends on the species in the exhaust stream and the type of air pollution control equipment used at the source. Air pollution control equipment for mercury removal at combustion facilities includes activated carbon injection, sodium sulfide infection and wet lime/limestone flue gas desulfurization. While Hg(II) is water-soluble and may be removed from the atmosphere by wet and dry deposition close to combustion sources, the combination of a high vapor pressure and low water-solubility facilitate the long-range transport of Hg° in the atmosphere. Background mercury in the atmosphere is predominantly Hg°. Elemental mercury is eventually removed from the atmosphere by dry deposition onto surfaces and by wet deposition after oxidation to water-soluble, divalent mercury.  相似文献   

16.
Mercury (Hg) was measured in stream water and precipitation in the Loch Vale watershed in Rocky Mountain National Park, Colorado, during 2001–2002 to investigate processes controlling Hg transport in high-elevation ecosystems. Total Hg concentrations in precipitation ranged from 2.6 to 36.2 ng/L and showed a strong seasonal pattern with concentrations that were 3 to 4 times higher during summer months. Annual bulk deposition of Hg was 8.3 to 12.4 μ g/m2 and was similar to deposition rates in the Midwestern and Northeastern U.S. Total Hg concentrations in streams ranged from 0.8 to 13.5 ng/L and were highest in mid-May on the rising limb of the snowmelt hydrograph. Stream-water Hg was positively correlated with dissolved organic carbon suggesting organically complexed Hg was flushed into streams from near-surface soil horizons during the early stages of snowmelt. Methylmercury (MeHg) in stream water peaked at 0.048 ng/L just prior to peak snowmelt but was at or below detection (< 0.040 ng/L) for the remainder of the snowmelt season. Annual export of total Hg in Loch Vale streams ranged from 1.2 to 2.3 μ g/m2, which was less than 20% of wet deposition, indicating the terrestrial environment is a net sink of atmospheric Hg. Concentrations of MeHg in stream water and corresponding watershed fluxes were low, indicating low methylation rates or high demethylation rates or both.  相似文献   

17.
Water pollution in response to accelerated land-use/land cover changes has drawn concerns because of public health and environmental impacts. The study was conducted to evaluate the impact of land use/land cover changes, seasonal, and location on water quality of streams within the Wheeler Lake Watershed basin in northern Alabama. Temporal water samples from 18 sheppard streams were randomly collected in 2000 and 2001, processed and analyzed for pH, and total nitrogen (TN), dissolved (Dp), particulate (Pp) and total phosphorus (Tp), dissolved oxygen (DO) and soluble lead (Pb) concentration, employing standard methods of analysis. The data were normalized and integrated into a simple index (WQCIndex) to evaluate stream water quality. Results showed that the urban proportion of the total watershed basin had increased from 2.9 to 14.7% with an associated loss of agricultural (8.9%) and wetland (4.8%) covers from 1992 to 2000. A change in land-use/land covers in association with seasonal and location variation significantly affected stream water quality. Total nitrogen concentration in stream water had a peak during the summer at 34% above the annual mean. While both Pp and Tp concentrations peaking during the summer at 24% above the annual mean and about 25% below the annual mean during spring, the DO concentrations were 46% above the annual mean during the fall and 18 to 26% below annual mean during summer. The WQCIndex had responded very seasonal and showed significant identical trends, with 21% degradation in water quality during the summer above the annual mean and improvement during the spring at 20% above the annual mean. Upstream water had a significantly greater Pp and Tp (21 to 28%) concentration than at down- and middle streams water. Location and seasonal variations had significant interactive effects on Pp, Tp and DO concentration of stream water. Total amount of seasonal rainfall significantly accounted 99.6% of the variations in WQCIndex. Increasing seasonal mean relative humidity, air and soil temperature, evaporation and solar radiation had positive relationship with the variations in WQCIndex. Among the water quality parameters, both Pp and Tp were correlated (r 2 = 0.998?*?) to each other, and accounted for more than 80% variability of the WQCIndex. Highly significant positive linear relationship between Pp and Tp concentration suggested that 99.8% of the P in stream water is in Pp form which probably transported with sediments in surface runoff. In other words, Pp is the main pollutant responsible for degradation of stream water quality in the Wheeler lake basin. Routine measurement of either Pp or Tp concentration could be used as sensitive and early indicator of temporal changes in stream water quality even when the other parameters changed negligibly or remain unchanged.  相似文献   

18.
The role of the hyporheic zone in mercury (Hg) cycling has received limited attention despite the biogeochemically active nature of this zone and, thus, its potential to influence Hg behavior in streams. An assessment of Hg geochemistry in the hyporheic zone of a coarse-grained island in the Coast Fork Willamette River in Oregon, USA, illustrates the spatially dynamic nature of this region of the stream channel for Hg mobilization and attenuation. Hyporheic flow through the island was evident from the water-table geometry and supported by hyporheic-zone chemistry distinct from that of the bounding groundwater system. Redox-indicator species changed abruptly along a transect through the hyporheic zone, indicating a biogeochemically reactive stream/hyporheic-zone continuum. Dissolved organic carbon (DOC), total Hg, and methylmercury (MeHg) concentrations increased in the upgradient portion of the hyporheic zone and decreased in the downgradient region. Total Hg (collected in 2002 and 2003) and MeHg (collected in 2003) were correlated with DOC in hyporheic-zone samples: r 2?=?0.63 (total Hg-DOC, 2002), 0.73 (total Hg-DOC, 2003), and 0.94 (MeHg-DOC, 2003). Weaker Hg/DOC association in late summer 2002 than in early summer 2003 may reflect seasonal differences in DOC reactivity. Observed correlations between DOC and both total Hg and MeHg reflect the importance of DOC for Hg mobilization, transport, and fate in this hyporheic zone. Correlations with DOC provide a framework for conceptualizing and quantifying Hg and MeHg dynamics in this region of the stream channel, and provide a refined conceptual model of the role hyporheic zones may play in aquatic ecosystems.  相似文献   

19.
Although much is known about chemical denudation and nutrient cycling through catchments, little has been done to identify and explain changes in major ion flux upon urbanization. Fifty-two weekly samples of precipitation and stream waters were analyzed for 9 major ions totaling 95% of the total dissolved solids for a catchment in southern England. Net major ion export rates from the urban area are between 2 and 104 times those for the rural areas. This increase is attributed both to accelerated denudation and non-denudational anthropogenic sources. Estimates of both components indicate that between 50 and 60% of the dissolved ions removed from urban areas is non-denudational. This translates to possible increases in the chemical denudation rate of up to six-fold upon urbanization.  相似文献   

20.
Polycyclic aromatic hydrocarbons (PAHs) are one class of chemical compounds that (1) are present at low to trace levels in unburned cigarette filler, and (2) are predominantly generated during combustion. According to a recent report of the International Agency for Research on Cancer, 10 carcinogenic PAHs together with 53 other known carcinogens are present in cigarette smoke. Accurate quantification of these chemicals helps assess public health risk to both smokers and nonsmokers exposed to second-hand smoke. We have developed and validated a specific and sensitive method for measuring these 10 carcinogenic PAHs in the particulate phase of mainstream tobacco smoke. Cigarette smoke particulate, produced using standard machine smoking protocols, was collected on glass fiber Cambridge filter pads. The particulate matter was solvent extracted, purified by solid-phase extraction, and analyzed by liquid chromatography/atmospheric pressure photoionization tandem mass spectrometry using isotopically labeled analogues as internal standards. Our method's limits of detection ranged from 11 to 166 pg and achieved sufficient reproducibility and accuracy to provide useful information on a range of cigarettes having dramatically different machine-smoked tar and nicotine deliveries. The identity of each PAH analyte was established from chromatographic retention time, analyte-specific fragmentation patterns, and relative peak area ratios of the product/precursor ion pairs. This new method provides higher sensitivity, specificity, and throughput than did earlier methods. We found relatively consistent PAH levels among a selection of domestic full-flavor cigarettes. The PAH levels in smoke from highly ventilated light and ultralight cigarettes were low when smoked using ISO (International Organization for Standardization) conditions. However, if highly ventilated cigarettes were smoked under more intense conditions (e.g., larger or more frequent puffs, vents blocked), their PAH levels equaled or exceeded their full-flavor counterparts under ISO conditions.  相似文献   

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