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1.
An evolving body of evidence suggests an adverse relation between persistent organochlorine pollutants (POPs) and menstruation, though prospective longitudinal measurement of menses is limited and served as the impetus for study. We prospectively assessed the relation between a mixture of persistent organochlorine compounds and menstrual cycle length and duration of bleeding in a cohort of women attempting to become pregnant. Eighty-three (83%) women contributing 447 cycles for analysis provided a blood specimen for the quantification of 76 polychlorinated biphenyls and seven organochlorine pesticides, and completed daily diaries on menstruation until a human chorionic gonadotropin confirmed pregnancy or 12 menstrual cycles without conception. Gas chromatography with electron capture detection was used to quantify concentrations (ng g−1 serum); enzymatic methods were used to quantify serum lipids (mg dL−1). A linear regression model with a mixture distribution was used to identify chemicals grouped by purported biologic activity that significantly affected menstrual cycle length and duration of bleeding adjusting for age at menarche and enrollment, body mass index, and cigarette smoking.A significant 3-d increase in cycle length was observed for women in the highest tertile of estrogenic PCB congeners relative to the lowest tertile (β = 3.20; 95% CI 0.36, 6.04). A significant reduction in bleeding (<1 d) was observed among women in the highest versus lowest tertile of aromatic fungicide exposure (γ = −0.15; 95% CI −0.29, −0.00). Select POPs were associated with changes in menstruation underscoring the importance of assessing chemical mixtures for female fecundity.  相似文献   

2.
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   

3.
Marine background levels of non-sea-salt- (nss-) SO42− (5.0–9.7 neq m−3), NH4+ (2.1–4.4 neq m−3) and elemental carbon (EC) (40–80 ngC m−3) in aerosol samples were measured over the equatorial and South Pacific during a cruise by the R/V Hakuho-maru from November 2001 to March 2002. High concentrations of nss-SO42− (47–94 neq m−3), NH4+ (35–94 neq m−3) and EC (130–460 ngC m−3) were found in the western North Pacific near the coast of the Asian continent under the influence of the Asian winter monsoon. Particle size distributions of ionic components showed that the equivalent concentrations of nss-SO42− were balanced with those of NH4+ in the size range of 0.06<D<0.22 μm, whereas the concentration ratios of NH4+ to nss-SO42− in the size range of D>0.22 μm were decreased with increase in particle size. We estimated the source contributions of those aerosol components in the marine background air over the equatorial and South Pacific. Biomass burning accounted for the large fraction (80–98% in weight) of EC and the minor fraction (2–4% in weight) of nss-SO42−. Marine biogenic source accounted for several tens percents of NH4+ and nss-SO42−. In the accumulation mode, 70% of particle number existed in the size range of 0.1<D<0.2 μm. In the size rage of 0.06<D<0.22 μm, the dominant aerosol component of (NH4)2SO4 would be mainly derived from the marine biogenic sources.  相似文献   

4.
Due to the high temporal and spatial variability of N2O fluxes, estimates of N2O emission from temperate forest ecosystems are still highly uncertain, particularly at larger scales. Although highest N2O emissions with up to 7.0 kg N ha−1 yr−1 were mainly reported for soils affected by stagnant water, most of the reported gas flux measurements were performed at forest sites with well-aerated soils yielding mostly to low mean annual emission rates less than 1.0 kg N ha−1 yr−1. This study compares N2O fluxes from upland (Cambisols) and temporally water-logged (Gleysols, Histosols) soils of the Central Black Forest (South-West Germany) over a period of 2 yr. Mean annual N2O fluxes from investigated soils ranged between 0.2 and 3.9 kg N ha−1 yr−1. The fluxes showed a large variability between the different soil types. Emissions could be clearly ranked in the following order: Cambisols (0.26–0.75 kg N ha−1 yr−1)<Gleysols (1.37–2.68 kg N ha−1 yr−1)<Histosol (3.66–3.95 kg N ha−1 yr−1). Although the Cambisols cover two-thirds of the investigated area, only about half of the overall N2O is emitted from this soil type. Therefore, regional or national N2O fluxes from temperate forest soils are underestimated if soils characterised by intermediate aeration conditions are disregarded.  相似文献   

5.
Indo-Gangetic (IG) alluvial plains, one of the largest river basins in the world, suffers from the long range transport of mineral dust from the western arid and desert regions of Africa, Arabia and Rajasthan during the summer (pre-monsoon season, April–June). These dust storms influence the aerosol optical depth (AOD) across the IG plains. The Kanpur AERONET (Aerosol Robotic Network) station and Moderate Resolution Imaging Spectro-radiometer (MODIS) data show pronounced effect on the aerosol optical properties and aerosol size distribution during major dust storm events over the IG plains that have significant effect on the aerosol radiative forcing (ARF). The multi-band AOD, from AERONET and MODIS, show contrasting changes in wavelength dependency over dust affected regions. A time collocated (±30 min) validation of AERONET AOD with MODIS Terra (level 2 swath product) over Kanpur, at a common wavelength of 550 nm for the period 2001–2005 show moderate correlation (R2∼0.6) during the summer season. The average surface forcing is found to change by −23 W m−2 during dust events and the top of the atmosphere (TOA) forcing change by −11 W m−2 as compared to the non-dusty clear-sky days. A strong correlation is found between AOD at 500 nm and the ARF. At surface, the correlation coefficient between AOD and ARF is found to be high (R2=0.925) and is found to be moderate (R2=0.628) at the TOA. The slope of the regression line gives the aerosol forcing efficiency at 500 nm of about −46±2.6 W m−2 and −17±2.5 W m−2 at the surface and the TOA, respectively. The ARF is found to increase with the advance of the dry season in conjunction with the gradual rise in AOD (at 500 nm) from April (0.4–0.5) to June (0.6–0.7) over the IG plains.  相似文献   

6.
Canopy scale emissions of isoprene and monoterpenes from Amazonian rainforest were measured by eddy covariance and eddy accumulation techniques. The peak mixing ratios at about 10 m above the canopy occurred in the afternoon and were typically about 90 pptv of α-pinene and 4–5 ppbv of isoprene. α-pinene was the most abundant monoterpene in the air above the canopy comprising ≈50% of the total monoterpene mixing ratio. Measured isoprene fluxes were almost 10 times higher than α-pinene fluxes. Normalized conditions of 30°C and 1000 μmol m−2 s−1 were associated with an isoprene flux of 2.4 mg m−2 h−1 and a β-pinene flux of 0.26 mg m−2 h−1. Both fluxes were lower than values that have been specified for Amazon rainforests in global emission models. Isoprene flux correlated with a light- and temperature-dependent emission activity factor, and even better with measured sensible heat flux. The variation in the measured α-pinene fluxes, as well as the diurnal cycle of mixing ratio, suggest emissions that are dependent on both light and temperature. The light and temperature dependence can have a significant effect on the modeled diurnal cycle of monoterpene emission as well as on the total monoterpene emission.  相似文献   

7.
For over one year, the Environmental Protection Commission of Hillsborough County (EPCHC) in Tampa, Florida, operated two dichotomous sequential particulate matter air samplers collocated with a manual Federal Reference Method (FRM) air sampler at a waterfront site on Tampa Bay. The FRM was alternately configured as a PM2.5, then as a PM10 sampler. For the dichotomous sampler measurements, daily 24-h integrated PM2.5 and PM10–2.5 ambient air samples were collected at a total flow rate of 16.7 l min−1. A virtual impactor split the air into flow rates of 1.67 and 15.0 l min−1 onto PM10–2.5 and PM2.5 47-mm diameter PTFE® filters, respectively. Between the two dichotomous air samplers, the average concentration, relative bias and relative precision were 13.3 μg m−3, 0.02% and 5.2% for PM2.5 concentrations (n=282), and 12.3 μg m−3, 3.9% and 7.7% for PM10–2.5 concentrations (n=282). FRM measurements were alternate day 24-h integrated PM2.5 or PM10 ambient air samples collected onto 47-mm diameter PTFE® filters at a flow rate of 16.7 l min−1. Between a dichotomous and a PM2.5 FRM air sampler, the average concentration, relative bias and relative precision were 12.4 μg m−3, −5.6% and 8.2% (n=43); and between a dichotomous and a PM10 FRM air sampler, the average concentration, relative bias and relative precision were 25.7 μg m−3, −4.0% and 5.8% (n=102). The PM2.5 concentration measurement standard errors were 0.95, 0.79 and 1.02 μg m−3; for PM10 the standard errors were 1.06, 1.59, and 1.70 μg m−3 for two dichotomous and one FRM samplers, respectively, which indicate the dichotomous samplers have superior technical merit. These results reveal the potential for the dichotomous sequential air sampler to replace the combination of the PM2.5 and PM10 FRM air samplers, offering the capability of making simultaneous, self-consistent determinations of these particulate matter fractions in a routine ambient monitoring mode.  相似文献   

8.
The photooxidation of methylhydroperoxide (MHP) and ethylhydroperoxide (EHP) was studied in the aqueous phase under simulated cloud droplet conditions. The kinetics and the reaction products of direct photolysis and OH-oxidation were studied for both compounds. The photolysis frequencies obtained were JMHP=4.5 (±1.0)×10−5 s−1 and JEHP=3.8 (±1.0)×10−5 s−1 for MHP and EHP respectively at 6 °C. The rate constants of OH-oxidation of MHP at 6 °C were 6.3 (±2.6)×108 M−1 s−1 and 5.8 (±1.9)×108 M−1 s−1 relative to ethanol and 2-propanol respectively, and the rate constant of OH-oxidation of EHP was 2.1 (±0.6)×109 M−1 s−1 relative to 2-propanol at 6 °C. The reaction products obtained were not only the corresponding aldehydes, but also the corresponding acids, and hydroxyhydroperoxides as primary reaction products. The yields for these products were sensitive to the pH value. The carbon balance was higher than 85% for all experiments, showing that most reaction products were detected. A chemical mechanism was proposed for each reaction, and the atmospheric implications were discussed.  相似文献   

9.
《Chemosphere》2007,66(11):1949-1958
Detailed analyses of persistent organic pollutants (POPs) such as organochlorine pesticides (OCPs), hexachlorocyclohexane (HCH) isomers (HCHs), dichlorodiphenyltrichloro ethane (DDT) and its metabolites (DDTs) and congeners of polychlorinated biphenyls (PCBs) in soil and surface water from the northeastern São Paulo, Brazil allowed the evaluation of the contamination status, distribution and possible pollution sources. The pesticides and PCBs demonstrated markedly different distributions, reflecting different agricultural, domestic and industrial usage in each region studied. The ranges of HCH, DDT, and PCBs concentrations in the soil samples were 0.05–0.92, 0.12–11.01, 0.02–0.25 ng g−1 dry wt, respectively, and in the surface water samples were 0.02–0.6, 0.02–0.58 and 0.02–0.5 ng l−1, respectively. Overall elevated levels of DDT and PCB were recorded in region 2, a site very close to melting, automotive batteries industries, and agricultural practice regions. High ratios of metabolites of DDT to DDT isomers revealed the recent use of DDT in this environment. The sources of contamination are closely related to human activities, such as domestic and industrial discharge, street runoff, agricultural pesticides and soil erosion, due to deforestation as well as atmospheric transport.  相似文献   

10.
《Chemosphere》2013,90(11):1307-1315
This study investigated the presence and distribution of 22 antibiotics, including eight quinolones, nine sulfonamides and five macrolides, in the water, sediments, and biota samples from Baiyangdian Lake, China. A total of 132 samples were collected in 2008 and 2010, and laboratory analyses revealed that antibiotics were widely distributed in the lake. Sulfonamides were the dominant antibiotics in the water (0.86–1563 ng L−1), while quinolones were prominent in sediments (65.5–1166 μg kg−1) and aquatic plants (8.37–6532 μg kg−1). Quinolones (17.8–167 μg kg−1) and macrolides [from below detection limit (BDL) to 182 μg kg−1] were often found in aquatic animals and birds. Salvinia natans exhibited the highest bioaccumulation capability for quinolones among three species of aquatic plants. Geographical differences of antibiotic concentrations were greatly due to anthropogenic activities. Sewage discharged from Baoding City was likely the main source of antibiotics in the lake. Risk assessment of antibiotics on aquatic organisms suggested that algae and aquatic plants might be at risk in surface water, while animals were likely not at risk.  相似文献   

11.
The occurrence of persistent toxic substances (PTS) in China and possibly their regional transport in the Yellow and East China Seas region was studied. Organochlorines in atmospheric gas-phase and particulate matter were collected by high-volume sampling (filters and polyurethane foams) during 2 weeks in June 2003 (dry season) simultaneously at a Yellow Sea coastal site in an urban area, Qingdao, China, and a rural island site, Gosan, Jeju Island, Korea. Using GC methods, the samples were analysed for 9 persistent organic pollutants (POPs) regulated under the global POP convention, namely aldrin, chlordane (cis- and trans-isomers CC and TC), DDT and metabolites (o,p′-DDT, p,p′-DDD, and p,p′-DDE), dieldrin, endrin, heptachlor, hexachlorobenzene (HCB), mirex and PCB (congeners number 28, 52, 101, 153 and 180), and for hexachlorocyclohexane (α-, β- and γ-isomers), a PTS and now considered for regulation under the convention, too. At the coastal site additionally o,p′-DDE and -DDD, β-endosulfan, isodrin, heptachlorepoxide and δ-HCH, and at the island site additionally p,p′-DDT and 12 additional PCB congeners were analysed. 9 samples were collected at the coastal and 15 (for PCBs 5) at the island site. Long-range advection pathways were determined based on analysed back-trajectory calculations.The mean concentrations of DDT and its metabolites, HCB, HCH, and PCB at the coast were in the 100–1000 pg m−3 range. Higher concentrations prevailed during nighttime. The levels were in general lower at the island site, but not for DDT. Local sources are likely. PCBs were even 2 orders of magnitude lower, suggesting that PCBs are not subject to regional transport but elevated concentrations in air are limited to the source areas. Organochlorine pesticide levels on the other hand were seemingly determined by regional transport over Mainland China rather than by emissions in the coastal area. The currently used pesticides mirex and chlordane were found at elevated levels, i.e. 79 (6.6–255) and 36 (<6–71) pg m−3, respectively, at the coast but not over the island. The POPs pesticides aldrin, dieldrin and endrin, never registered in China, were mostly found at <10 pg m−3 except for endrin at the coastal site (up to 400 pg m−3) and aldrin at the island site (up to 50 pg m−3).  相似文献   

12.
Forty native Mediterranean plant species were screened for emissions of the C5 and C10 hydrocarbons, isoprene and monoterpenes, in five different habitats. A total of 32 compounds were observed in the emissions from these plants. The number of compounds emitted by different plant species varied from 19 (Quercus ilex) to a single compound emission, usually of isoprene. Emission rates were normalised to generate emission factors for each plant species for each sampling event at standard conditions of temperature and light intensity. Plant species were categorised according to their main emitted compound, the major groups being isoprene, α-pinene, linalool, and limonene emitters. Estimates of habitat fluxes for each emitted compound were derived from the contributing plant species’ emission factors, biomass and ground cover. Emissions of individual compounds ranged from 0.002 to 505 g ha−1 h−1 (camphene from garrigue in Spain in autumn and isoprene from riverside habitats in Spain in late spring; respectively). Emissions of isoprene ranged from 0.3 to 505 g ha−1 h−1 (macchia in Italy in late spring and autumn; and riverside in Spain in late spring; respectively) and α-pinene emissions ranged from 0.51 to 52.92 g ha−1 h−1 (garrigue in Spain in late spring; and forest in France in autumn; respectively). Habitat fluxes of most compounds in autumn were greater than in late spring, dominated by emissions from Quercus ilex, Genista scorpius and Quercus pubescens. This study contributes to regional emission inventories and will be of use to tropospheric chemical modellers.  相似文献   

13.
A field experiment was conducted in a rice–winter wheat rotation agroecosystem to quantify the direct emission of N2O for synthetic N fertilizer and crop residue application in the 2002–2003 annual cycle. There was an increase in N2O emission accompanying synthetic N fertilizer application. Fertilizer-induced emission factor for N2O (FIE) averaged 1.08% for the rice season, 1.49% for the winter wheat season and 1.26% for the whole annual rotation cycle. The annual background emission of N2O totaled 4.81 kg N2O–N ha−1, consisting of 1.24 kg N2O–N ha−1 for rice, 3.11 kg N2O–N ha−1 for wheat seasons. When crop residue and synthetic N fertilizer were both applied in the fields, crop residue-induced emission factor for N2O (RIE) was estimated as well. When crop residue was retained at the rate of 2.25 and 4.50 t ha−1 for each season, the RIE averaged 0.64% and 0.27% for the whole annual rotation cycle, respectively. Based on available multi-year data of N2O emissions over the whole rice–wheat rotation cycle at 3 sites in southeast China, the FIE averaged 1.02% for the rice season, 1.65% for the wheat season. On the whole annual cycle, the FIE for N2O ranged from 1.05% to 1.45%, with an average of 1.25%. Annual background emission of N2O averaged 4.25 kg ha−1, ranging from 3.62 to 4.87 kg ha−1. It is estimated that annual N2O emission in paddy rice-based agroecosystem amounts to 169 Gg N2O–N in China, accounting for 26–60% of the reported estimates of total emission from croplands in China.  相似文献   

14.
The quality of an emission calculation model based on emission factors measured on roller test stands and statistical traffic data was evaluated using source strengths and emission factors calculated from real-world exhaust gas concentration differences measured upwind and downwind of a motorway in southwest Germany. Gaseous and particulate emissions were taken into account. Detailed traffic census data were taken during the measurements. The results were compared with findings of similar studies.The main conclusion is the underestimation of CO and NOx source strengths by the model. On the average, it amounts to 23% in case of CO and 17% for NOx. The latter underestimation results from an undervaluation by 22% of NOx emission factors of heavy-duty vehicles (HDVs). There are significant differences between source strengths on working days and weekends because of the different traffic split between light-duty vehicles (LDVs) and HDVs. The mean emission factors of all vehicles from measurements are 1.08 g km−1 veh−1 for NOx and 2.62 g km−1 veh−1 for CO. The model calculations give 0.92 g km−1 veh−1 for NOx and 2.14 g km−1 veh−1 for CO.The source strengths of 21 non-methane hydrocarbon (NMHC) compounds quantified are underestimated by the model. The ratio between the measured and model-calculated emissions ranges from 1.3 to 2.1 for BTX and up to 21 for 16 other NMHCs. The reason for the differences is the insufficient knowledge of NMHC emissions of road traffic.Particulate matter emissions are dominated by ultra-fine particles in the 10–40 nm range. As far as aerosols larger than 29 nm are concerned, 1.80×1014 particles km−1 veh−1 are determined for all vehicles, 1.22×1014 particles km−1 veh−1 and an aerosol volume of 0.03 cm3 km−1 veh−1 are measured for LDVs, and for HDVs 7.79×1014 particles km−1 veh−1 and 0.41 cm3 km−1 veh−1 are calculated. Traffic-induced turbulence has been identified to have a decisive influence on exhaust gas dispersion near the source.  相似文献   

15.
Currently, in operational modelling of NH3 deposition a fixed value of canopy resistance (Rc) is generally applied, irrespective of the plant species and NH3 concentration. This study determined the effect of NH3 concentration on deposition processes to individual moorland species. An innovative flux chamber system was used to provide accurate continuous measurements of NH3 deposition to Deschampsia cespitosa (L.) Beauv., Calluna vulgaris (L.) Hull, Eriophorum vaginatum L., Cladonia spp., Sphagnum spp., and Pleurozium schreberi (Brid.) Mitt. Measurements were conducted across a wide range of NH3 concentrations (1–140 μg m−3).NH3 concentration directly affects the deposition processes to the vegetation canopy, with Rc, and cuticular resistance (Rw) increasing with increasing NH3 concentration, for all the species and vegetation communities tested. For example, the Rc for C. vulgaris increased from 14 s m−1 at 2 μg m−3 to 112 s m−1 at 80 μg m−3. Diurnal variations in NH3 uptake were observed for higher plants, due to stomatal uptake; however, no diurnal variations were shown for non-stomatal plants. Rc for C. vulgaris at 80 μg m−3 was 66 and 112 s m−1 during day and night, respectively. Differences were found in NH3 deposition between plant species and vegetation communities: Sphagnum had the lowest Rc (3 s m−1 at 2 μg m−3 to 23 at 80 μg m−3), and D. cespitosa had the highest nighttime value (18 s m−1 at 2 μg m−3 to 197 s m−1 at 80 μg m−3).  相似文献   

16.
Static chamber method was adopted to measure the surface exchanges of NO and NO2 between three kinds of agricultural lands and the atmosphere during spring–summer period in the Yangtze Delta, China. The average NO fluxes were 20.9, 27.4 and 21.4 ng N m−2 s−1, respectively, for cabbage (CA, cultivation of celery occurred along with cabbage), potato (PO) and soybean (SY) fields. The average NO2 fluxes were −1.12, 0.93 and −0.68 ng N m−2 s−1, respectively, for the cabbage, potato and soybean fields. Apparently, negative linear correlation was found between the NO2 fluxes from the CK plot (tilled conventionally but did not cultivate any seeds) and its ambient concentrations, and the compensation point was calculated to be 0.92 ppbv. The total NO emission from the vegetable lands and SY land in this region during spring–summer period was roughly estimated to be 15.9 Gg N, which accounted for about 11.2% of the estimated value of total NO emissions in the July of 1999 from Chinese agricultural fields.  相似文献   

17.
We reconstructed the historical trends in atmospheric deposition of nitrogen to Cape Cod, Massachusetts, from 1910 to 1995 by compiling data from literature sources, and adjusting the data for geographical and methodological differences. The reconstructed data suggest that NO3-N wet deposition to this region increased from a low of 0.9 kg N ha−1 yr−1 in 1925 to a high of approximately 4 kg N ha−1 yr−1 around 1980. The trend in NO3-N deposition has remained since the early 1980s at around 3.6 kg N ha−1 yr−1. In contrast, NH4-N wet deposition decreased from more than 4 kg N ha−1 yr−1 in the mid 1920s to about 1.5 kg N ha−1 yr−1 from the late-1940s until today. Emissions of NOx-N in the Cape Cod airshed increased at a rate of 2.1 kg N ha−1 per decade since 1910, a rate that is an order of magnitude higher than NO3-N deposition. Estimates of NH3 emissions to the northeast United States and Canada have decreased slightly throughout the century, but the decrease in reconstructed N-NH4+ deposition rates does not parallel emissions estimates. The trend in reconstructed total nitrogen deposition suggests an overall increase through the century at a rate of 0.26 kg N ha−1 per decade. This overall increase in deposition may expose coastal forests to rates of nitrogen addition that, if exceeded, could induce nitrogen saturation and increase nitrogen loads to adjoining estuaries.  相似文献   

18.
Dry deposition modelling typically assumes that canopy resistance (Rc) is independent of ammonia (NH3) concentration. An innovative flux chamber system was used to provide accurate continuous measurements of NH3 deposition to a moorland composed of a mixture of Calluna vulgaris (L.) Hull, Eriophorum vaginatum L. and Sphagnum spp. Ammonia was applied at a wide range of concentrations (1–100 μg m−3). The physical and environmental properties and the testing of the chamber are described, as well as results for the moorland vegetation using the ‘canopy resistance’ and ‘canopy compensation point’ interpretations of the data.Results for moorland plant species demonstrate that NH3 concentration directly affects the rate of NH3 deposition to the vegetation canopy, with Rc and cuticular resistance (Rw) increasing with increasing NH3 concentrations. Differences in Rc were found between night and day: during the night Rc increases from 17 s m−1 at 10 μg m−3 to 95 s m−1 at 80 μg m−3, whereas during the day Rc increases from 17 s m−1 at 10 μg m−3 to 48 s m−1 at 80 μg m−3. The lower resistance during the day is caused by the stomata being open and available as a deposition route to the plant. Rw increased with increasing NH3 concentrations and was not significantly different between day and night (at 80 μg m−3 NH3 day Rw=88 s m−1 and night Rw=95 s m−1). The results demonstrate that assessments using fixed Rc will over-estimate NH3 deposition at high concentrations (over ∼15 μg m−3).  相似文献   

19.
The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σsp) at 525 nm, PM10, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m−1, 157.6±270.0 μg m−3, and 2.30±3.41 m2 g−1, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m−1, 119.0±112.9 μg m−3, and 1.87±1.41 m2 g−1. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM10, σsp, and α were 184.1±211.548 μg m−3, 126.3±89.6 M m−1, and 1.05±0.97 m2 g−1, respectively, and these values at Dongsheng were 146.4±142.1 μg m−3, 183.4±81.7 M m−1, and 1.98±1.52 m2 g−1, respectively. However, in winter at Dunhuang PM10, σsp, and α were 158.1±261.4 μg m−3, 303.3±165.2 M m−1, and 3.17±1.93 m2 g−1, respectively, and these values at Dongsheng were 155.7±170.1 μg m−3, 304.4±158.1 M m−1, and 2.90±1.72 m2 g−1, respectively. σsp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.  相似文献   

20.
In an effort to reduce uncertainties in the quantification of aerosol direct radiative forcing (ADRF) in the southeastern United States (US), a field column experiment was conducted to measure aerosol radiative properties and effects at Mt. Mitchell, North Carolina, and at an adjacent valley site. The experimental period was from June 1995 to mid-December 1995. The aerosol optical properties (single scattering albedo and asymmetry factor) needed to compute ADRF were obtained on the basis of a procedure involving a Mie code and a radiative transfer code in conjunction with the retrieved aerosol size distribution, aerosol optical depth, and diffuse-to-direct solar irradiance ratio. The regional values of ADRF at the surface and top of atmosphere (TOA), and atmospheric aerosol absorption are derived using the obtained aerosol optical properties as inputs to the column radiation model (CRM) of the community climate model (CCM3). The cloud-free instantaneous TOA ADRFs for highly polluted (HP), marine (M) and continental (C) air masses range from 20.3 to −24.8, 1.3 to −10.4, and 1.9 to −13.4 W m−2, respectively. The mean cloud-free 24-h ADRFs at the TOA (at the surface) for HP, M, and C air masses are estimated to be −8±4 (−33±16), −7±4 (−13±8), and −0.14±0.05 (−8±3) W m−2, respectively. On the assumption that the fractional coverage of clouds is 0.61, the annual mean ADRFs at the TOA and the surface are −2±1, and −7±2 W m−2, respectively. This also implies that aerosols currently heat the atmosphere over the southeastern US by 5±3 W m−2 on annual timescales due to the aerosol absorption in the troposphere.  相似文献   

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