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1.
Both aerosol and rainwater samples were collected and analyzed for ionic species at a coastal site in Southeast Asia over a period of 9 months (January–September 2006) covering different monsoons. In general, the occurrence and distribution of ionic species showed a distinct seasonal variation in response to changes in air mass origins. Real-time physical characterization of aerosol particles during rain events showed changes in particle number distributions which were used to assess particle removal processes associated with precipitation, or scavenging. The mean scavenging coefficients for particles in the range 10–500 nm and 500–10 μm were 7.0 × 10−5 ± 2.8 × 10−5 s−1 and 1.9 × 10−4 ± 1.6 × 10−5 s−1, respectively. A critical analysis of the scavenging coefficients obtained from this study suggested that the wet removal of aerosol particles was greatly influenced by rain intensity, and was particle size-dependent as well. The scavenging ratios, another parameter used to characterize particle removal processes by precipitation, for NH4 +, Cl−, SO4 2−, and NO3 − were found to be higher than those of Na+, K+, and Ca2+ of oceanic and crustal origins. This enrichment implied that gaseous species NH3, HCl, and HNO3 could also be washed out readily. These additional sources of ions in precipitation presumably counter-balanced the dilution effect caused by high total precipitation volume in the marine and tropical area.  相似文献   

2.
A time series of microwave radiometric profiles over Arctic Canada’s Cape Bathurst (70°N, 124.5°W) flaw lead polynya region from 1 January to 30 June, 2008 was examined to determine the general characteristics of the atmospheric boundary layer in winter and spring. A surface based or elevated inversion was present on 97% of winter (January–March) days, and on 77% of spring (April–June) days. The inversion was the deepest in the first week of March (≈1100 m), and the shallowest in June (≈250 m). The mean temperature and absolute humidity from the surface to the top of the inversion averaged 250.1 K (−23.1°C), and 0.56 × 10−3 kg m−3 in winter, and in spring averaged 267.5 K (−5.6°C), and 2.77 × 10−3 kg m−3. The median winter atmospheric boundary-layer (ABL) potential temperature profile provided evidence of a shallow, weakly stable internal boundary layer (surface to 350 m) topped by an inversion (350–1,000 m). The median spring profile showed a shallow, near-neutral internal boundary layer (surface to 350 m) under an elevated inversion (600–800 m). The median ABL absolute humidity profiles were weakly positive in winter and negative in spring. Estimates of the convergence of sensible heat and water vapour from the surface that could have produced the turbulent internal boundary layers of the median profiles were 0.67 MJ m−2 and 13.1 × 10−3 kg m−2 for the winter season, and 0.66 MJ m−2 and 33.4 × 10−3 kg m−2 for the spring season. With fetches of 10–100 km, these accumulations may have resulted from a surface sensible heat flux of 15–185 W m−2, plus a surface moisture flux of 0.001–0.013 mm h−1 (or a latent heat flux of 0.7–8.8 W m−2) in winter, and 0.003–0.033 mm h−1 (or a latent heat flux of 2–22 W m−2) in spring.  相似文献   

3.
Aerosol and rain samples were collected between 48°N and 55°S during the KH-08-2 and MR08-06 cruises conducted over the North and South Pacific Ocean in 2008 and 2009, to estimate dry and wet deposition fluxes of atmospheric inorganic nitrogen (N). Inorganic N in aerosols was composed of ~68% NH4+ and ~32% NO3– (median values for all data), with ~81% and ~45% of each species being present on fine mode aerosol, respectively. Concentrations of NH4+ and NO3− in rainwater ranged from 1.7–55 μmol L−1 and 0.16–18 μmol L−1, respectively, accounting for ~87% by NH4+ and ~13% by NO3− of total inorganic N (median values for all data). A significant correlation (r = 0.74, p < 0.05, n = 10) between NH4+ and methanesulfonic acid (MSA) was found in rainwater samples collected over the South Pacific, whereas no significant correlations were found between NH4+ and MSA in rainwater collected over the subarctic (r = 0.42, p > 0.1, n = 6) and subtropical (r = 0.33, p > 0.5, n = 6) western North Pacific, suggesting that emissions of ammonia (NH3) by marine biological activity from the ocean could become a significant source of NH4+ over the South Pacific. While NO3− was the dominant inorganic N species in dry deposition, inorganic N supplied to surface waters by wet deposition was predominantly by NH4+ (42–99% of the wet deposition fluxes for total inorganic N). We estimated mean total (dry + wet) deposition fluxes of atmospheric total inorganic N in the Pacific Ocean to be 32–64 μmol m−2 d−1, with 66–99% of this by wet deposition, indicating that wet deposition plays a more important role in the supply of atmospheric inorganic N than dry deposition.  相似文献   

4.
The results of one year’s monitoring in Srednja Bijambarska Cave (Bosnia and Herzegovina) are presented and discussed. Temporal variations of the carbon dioxide (CO2) concentration are controlled by the switching between two ventilation regimes driven by outside temperature changes. A regression model with a simple perfectly mixed volume applied to a cave sector (“Music hall”) resulted in an estimate of ventilation rates between 0.02 h−1 and 0.54 h−1. Carbon dioxide input per plan surface unit is estimated by the model at around 50 × 10−6 mh−1 during the winter season and up to more than 1000 × 10−6 mh−1 during the first temperature falls at the end of summer (0.62 μmoles m−2 s−1 and 12.40 μmoles m−2 s−1 for normal conditions respectively). These values have been found to be related to the cave ventilation rate and dependent on the availability of CO2 in the surrounding environment. For airflow close to zero the values of CO2 input per plan surface have a range in the order of magnitude of a few units × 10−6 mh−1. Based on two experiments, the anthropogenic contribution from cave visitors has been calculated, at between 0.35 lCO2 min−1 person−1 and 0.45 lCO2min−1person−1.  相似文献   

5.
To understand the response of the Greenland ice sheet to climate change the so-called ablation zone is of particular importance, since it accommodates the yearly net surface ice loss. In numerical models and for data analysis, the bulk aerodynamic method is often used to calculate the turbulent surface fluxes, for which the aerodynamic roughness length (z 0) is a key parameter. We present, for the first time, spatial and temporal variations of z 0 in the ablation area of the Greenland ice sheet using year-round data from three automatic weather stations and one eddy-correlation mast. The temporal variation of z 0 is found to be very high in the lower ablation area (factor 500) with, at the end of the summer melt, a maximum in spatial variation for the whole ablation area of a factor 1000. The variation in time matches the onset of the accumulation and ablation season as recovered by sonic height rangers. During winter, snow accumulation and redistribution by snow drift lead to a uniform value of z 0≈ 10−4 m throughout the ablation area. At the beginning of summer, snow melt uncovers ice hummocks and z 0 quickly increases well above 10−2 m in the lower ablation area. At the end of summer melt, hummocky ice dominates the surface with z 0 > 5  ×  10−3 m up to 60 km from the ice edge. At the same time, the area close to the equilibrium line (about 90 km from the ice edge) remains very smooth with z 0 = 10−5 m. At the beginning of winter, we observed that single snow events have the potential to lower z 0 for a very rough ice surface by a factor of 20 to 50. The total surface drag of the abundant small-scale ice hummocks apparently dominates over the less frequent large domes and deep gullies. The latter results are verified by studying the individual drag contributions of hummocks and domes with a drag partition model.  相似文献   

6.
The uptake of water vapor on MgCl2×6H2O and NaCl salt dry solid films was studied over the temperature range 240 to 340 K and at 1 Torr pressure of helium using a flow reactor coupled to a modulated molecular beam mass spectrometer. The H2O to salt uptake data were obtained from the kinetics of H2O loss on salt coated Pyrex rods. The following Arrhenius expression was obtained for the initial uptake coefficient of H2O on MgCl2×6H2O films: γ 0 (MgCl2) = (6.5 ± 1.0) × 10−6 exp[(470 ± 40)/T] (calculated with specific BET surface area, quoted uncertainties are 1σ statistical). The rate of H2O adsorption on NaCl was found to be much lower than on MgCl2×6H2O, and only an upper limit was determined for the corresponding uptake coefficient: γ (NaCl) ≤ 5.6 × 10−6 at T = 300 K. The results show that the rate of H2O adsorption to salt surfaces is drastically dependent on the salt sample composition.  相似文献   

7.
Sonic anemometer and profile mast measurements made in Wahlenbergfjorden, Svalbard Arctic archipelago, in May 2006 and April 2007 were employed to study the atmospheric boundary layer over sea-ice. The turbulent surface fluxes of momentum and sensible heat were calculated using eddy correlation and gradient methods. The results showed that the literature-based universal functions underestimated turbulent mixing in strongly stable conditions. The validity of the Monin-Obukhov similarity theory was questionable for cross-fjord flow directions and in the presence of mesoscale variability or topographic effects. The aerodynamic roughness length showed a dependence on the wind direction. The mean roughness length for along-fjord wind directions was (2.4 ± 2.6) × 10−4 m, whereas that for cross-fjord directions was (5.4 ± 2.8) × 10−3 m. The thermal stratification and turbulent fluxes were affected by the synoptic situation with large differences between the 2 years. Channelling effects and drainage flows occurred especially during a weak large-scale flow. The study periods were simulated applying the Weather Research and Forecasting (WRF) model with 1-km horizontal resolution in the finest domain. The results for the 2-m air temperature and friction velocity were good, but the model failed to reproduce the spatial variability in wind direction between measurement sites 3 km apart. The model suggested that wind shear above the stable boundary layer provided a non-local source for the turbulence observed.  相似文献   

8.
Ambient respirable particles (PM10; aerodynamic diameter ≤10 μm) collected in a tropical urban environment (Delhi, India) during December 2008-November 2009 were characterized with respect to 16 US EPA priority polycyclic aromatic hydrocarbons (PAHs) and 8 major and trace metals (Fe, Mn, Cd, Cu, Ni, Pb, Zn and Cr). Concentrations of Σ16PAHs (annual mean: 74.7 ± 50.7 ng m−3, range 22.1–258.4 ng m−3) and most metallic species were at least an order of magnitude greater than values reported from similar locations worldwide. Seasonal variations in Σ16PAHs were significant (p < 0.001) with highest levels in winter while crustal and anthropogenic metals showed significant but mutually opposite seasonal dependence. Statistically significant associations were observed between chemical species and various meteorological parameters. The PAH profile was dominated by combustion-derived large-ring species (~85%) that were essentially local in origin. Principal component analysis–multiple linear regression (PCA-MLR) apportioned four sources: crustal dust (73%), vehicular emission (21%), coal combustion (4%) and industrial emission (2%) that was further validated by hierarchical cluster analysis (HCA). Temporal trend analysis showed that crustal sources were predominant in summer (p < 0.05) while the remaining sources were most active in winter. Summertime intrusions of Saharan dust were identified with the help of aerosol maps and air parcel backward trajectories. Inhalation cancer risk assessment showed that up to 3,907 excess cancer cases (357 for PAHs, 122 for Cd, 2040 for Cr (VI) and 1387 for Ni) are likely in Delhi considering lifetime inhalation exposure to these chemicals at their current concentrations.  相似文献   

9.
The kinetics of heterogeneous reactions of NO2 with 17 polycyclic aromatic hydrocarbons (PAHs) adsorbed on laboratory generated kerosene soot surface was studied over the temperature range (255–330) K in a low pressure flow reactor combined with an electron-impact mass spectrometer. The kinetics of soot-bound PAH consumption due to their desorption and reaction with NO2 were monitored using off-line HPLC measurements of their concentrations in soot samples as a function of reaction time, NO2 concentrations in the gas phase being analyzed by mass spectrometer. No measurable decay of PAHs due to the reaction with NO2 was observed under experimental conditions of the study (maximum NO2 concentration of 5.5 × 1014 molecule cm−3 and reaction time of 45 min), which allowed to determine the upper limits of the first-order rate constants for the heterogeneous reactions of 17 soot-bound PAHs with NO2: k < 5.0 × 10−5 s−1 (for most PAHs studied). Comparison of these results to previous studies carried on different carbonaceous substrates, showed that heterogeneous reactivity of PAHs towards NO2 is, probably, dependent on the substrate nature even for resembling, although different carbonaceous materials. Results show that particulate PAHs degradation by NO2 alone is of minor importance in the atmosphere  相似文献   

10.
The concentrations of PM10, PM2.5 and their water-soluble ionic species were determined for the samples collected during January to December, 2007 at New Delhi (28.63° N, 77.18° E), India. The annual mean PM10 and PM2.5 concentrations (± standard deviation) were about 219 (± 84) and 97 (±56) μgm−3 respectively, about twice the prescribed Indian National Ambient Air Quality Standards values. The monthly average ratio of PM2.5/PM10 varied between 0.18 (June) and 0.86 (February) with an annual mean of ∼0.48 (±0.2), suggesting the dominance of coarser in summer and fine size particles in winter. The difference between the concentrations of PM10 and PM2.5, is deemed as the contribution of the coarse fraction (PM10−2.5). The analyzed coarse fractions mainly composed of secondary inorganic aerosols species (16.0 μgm−3, 13.07%), mineral matter (12.32 μgm−3, 10.06%) and salt particles (4.92 μgm−3, 4.02%). PM2.5 are mainly made up of undetermined fractions (39.46 μgm−3, 40.9%), secondary inorganic aerosols (26.15 μgm−3, 27.1%), salt aerosols (22.48 μgm−3, 23.3%) and mineral matter (8.41 μgm−3, 8.7%). The black carbon aerosols concentrations measured at a nearby (∼300 m) location to aerosol sampling site, registered an annual mean of ∼14 (±12) μgm−3, which is significantly large compared to those observed at other locations in India. The source identifications are made for the ionic species in PM10 and PM2.5. The results are discussed by way of correlations and factor analyses. The significant correlations of Cl−, SO42−, K+, Na+, Ca2+, NO3− and Mg2+ with PM2.5 on one hand and Mg2+ with PM10 on the other suggest the dominance of anthropogenic and soil origin aerosols in Delhi.  相似文献   

11.
A study of the oxidation mechanism of N-methyl pyrrolidinone (C5H9NO, NMP) initiated by hydroxyl radicals was made at EUPHORE at atmospheric pressure (1000 ± 10) mbar of air and ambient temperature (T = 300 ± 5 K). The main products were N-methyl succinimide (NMS) (52 ± 4)% and N-formyl pyrrolidinone (FP) (23 ± 9)%. The relative rate technique was used to determine the rate constants of OH with NMP, NMS and FP, the measured values were (in units of cm3 molecule − 1 s− 1): kNMP = (2.2 ± 0.4) × 10− 11, kNMS = (1.4 ± 0.3) × 10− 12 and kFP = (6 ± 1) × 10− 12. The results are presented and discussed in terms of the atmospheric impact.  相似文献   

12.
In this experimental study, rate constants were measured for the reactions of ozone with 13 polycyclic aromatic hydrocarbons (PAHs) adsorbed on different types of particles. Graphite and silica were chosen to model, respectively, carbonaceous and mineral atmospheric particles. The pseudo-first order rate constants were obtained from the fit of the experimental decay of particulate PAH concentrations versus time. Second order rate constants were calculated considering the ozone gaseous concentration. At room temperature, rate constants varied, in the case of graphite particles, between (1.5 ± 0.5) × 10−17 and (1.3 ± 0.7) × 10−16 cm3 molecule−1 s−1 for chrysene and dibenzo[a,l]pyrene, respectively, and, in the case of silica particles, between (1.5 ± 0.3) × 10−17 and (1.4 ± 0.3) × 10−16 cm3 molecule−1 s−1 for fluoranthene and benzo[a]pyrene, respectively. Different granulometric parameters (particle size, pore size) and different PAH concentrations were tested in the case of silica particles. Heterogeneous reactions of ozone with particulate PAHs are shown to be more rapid than those occurring in the gas-phase, and may be competitive with atmospheric photodegradation.  相似文献   

13.
For the measurement of atmospheric NO2 vertical column density (VCD), Kitt Peak Solar Flux Atlas can be substituted as an extraterrestrial solar radiation. Compared with differential analysis method, the Taylor expansion of integrated transfer equation underestimates the VCD. This underestimation is as large as 35% when the amount of NO2 is 1 × 1017 cm－2 and observation is conducted with an air mass factor of 10. Even when the VCD is 2 × 1016 cm－2 and the air mass factor is 4, the relative error of the retrieved VCD is still no less than 3%. If the observation is restricted under the small air mass factor condition (≤4), with Kitt Peak Solar spectrum as an extraterrestrial solar radiation, only an atmospheric layer of 2 km thick from ground can be studied, which will make the absorption too weak to be detected by normal instruments.The VCD in winter Tokyo area was observed and analyzed by differential method, which shows a good precision even when the absorption is as low as 3%. The largest average VCD was about 1.3 × 1017 cm－2, and the lowest was about 1.3 × 1016 cm－2. The trend of its variation was almost the same as the ground level observation by Saltzman reagent method.  相似文献   

14.
In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM10 (particles with aerodynamic diameter ≤10 μm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (～1000 μg m-3), the Gobi Desert (～400 μg m-3), and the Huabei Plain (～300 μm-3) of China. Vertically, high PM10 concentrations ranging from 100 μg m-3 to 250 μg m-3 occurred from the surface to an altitude of 6000 m at 30o--45oN in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ～42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.  相似文献   

15.
This paper deals with the atmospheric concentrations of PM5 and PM2.5 particulate matter and its water soluble constituents along with the size distribution of ions and spatial variation at three different residential environments in a semiarid region in India. Samples were collected from the indoors and outdoors of urban, rural and roadside sites of Agra during October 2007–March 2008. The mean concentrations of PM2.5 indoors and outdoors were 178 μgm−3 and 195 μgm−3 while the mean concentrations of PM5 indoors and outdoors were 231.8 μgm−3 and 265.2 μgm−3 respectively. Out of the total aerosol mass, water soluble constituents contributed an average of 80% (33% anions, 50% cations) in PM5 and 70% (29% anions, 43% cations) in PM2.5. The indoor–outdoor ratio of water soluble components suggested additional aerosol indoor sources at rural and roadside sites. Indoor–outdoor correlations were also determined which show poor relationships among concentrations of aerosol ions at all three sites. Univariate Pearson correlation coefficients among water soluble aerosols were determined to evaluate the relationship between aerosol ions in indoor and outdoor air.  相似文献   

16.

Size-segregated aerosol particles were collected using a high volume MOUDI sampler at a coastal urban site in Xiamen Bay, China, from March 2018 to June 2020 to examine the seasonal characteristics of aerosol and water-soluble inorganic ions (WSIIs) and the dry deposition of nitrogen species. During the study period, the annual average concentrations of PM1, PM2.5, PM10, and TSP were 14.8?±?5.6, 21.1?±?9.0, 35.4?±?14.2 μg m?3, and 45.2?±?21.3 μg m?3, respectively. The seasonal variations of aerosol concentrations were impacted by the monsoon with the lowest value in summer and the higher values in other seasons. For WSIIs, the annual average concentrations were 6.3?±?3.3, 2.1?±?1.2, 3.3?±?1.5, and 1.6?±?0.8 μg m?3 in PM1, PM1-2.5, PM2.5–10, and PM>10, respectively. In addition, pronounced seasonal variations of WSIIs in PM1 and PM1-2.5 were observed, with the highest concentration in spring-winter and the lowest in summer. The size distribution showed that SO42?, NH4+ and K+ were consistently present in the submicron particles while Ca2+, Mg2+, Na+ and Cl? mainly accumulated in the size range of 2.5–10 μm, reflecting their different dominant sources. In spring, fall and winter, a bimodal distribution of NO3? was observed with one peak at 2.5–10 μm and another peak at 0.44–1 μm. In summer, however, the fine mode peak disappeared, likely due to the unfavorable conditions for the formation of NH4NO3. For NH4+ and SO42?, their dominant peak at 0.25–0.44 μm in summer and fall shifted to 0.44–1 μm in spring and winter. Although the concentration of NO3–N was lower than NH4–N, the dry deposition flux of NO3–N (35.77?±?24.49 μmol N m?2 d?1) was much higher than that of NH4–N (10.95?±?11.89 μmol N m?2 d?1), mainly due to the larger deposition velocities of NO3–N. The contribution of sea-salt particles to the total particulate inorganic N deposition was estimated to be 23.9—52.8%. Dry deposition of particulate inorganic N accounted for 0.95% of other terrestrial N influxes. The annual total N deposition can create a new productivity of 3.55 mgC m?2 d?1, accounting for 1.3–4.7% of the primary productivity in Xiamen Bay. In light of these results, atmospheric N deposition could have a significant influence on biogeochemistry cycle of nutrients with respect to projected increase of anthropogenic emissions from mobile sources in coastal region.

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17.
Summary One of the great unknowns in climate research is the contribution of aerosols to climate forcing and climate perturbation. In this study, retrievals from AERONET are used to estimate the direct clear-sky aerosol top-of-atmosphere and surface radiative forcing effects for 12 multi-site observing stations in Europe. The radiative transfer code sdisort in the libRadtran environment is applied to accomplish these estimations. Most of the calculations in this study rely on observations which have been made for the years 1999, 2000, and 2001. Some stations do have observations dating back to the year of 1995. The calculations rely on a pre-compiled aerosol optical properties database for Europe. Aerosol radiative forcing effects are calculated with monthly mean aerosol optical properties retrievals and calculations are presented for three different surface albedo scenarios. Two of the surface albedo scenarios are generic by nature bare soil and green vegetation and the third relies on the ISCCP (International Satellite Cloud Climatology Project) data product. The ISCCP database has also been used to obtain clear-sky weighting fractions over AERONET stations. The AERONET stations cover the area 0° to 30° E and 42° to 52° N. AERONET retrievals are column integrated and this study does not make any seperation between the contribution of natural and anthropogenic components. For the 12 AERONET stations, median clear-sky top-of-atmosphere aerosol radiative forcing effect values for different surface albedo scenarios are calculated to be in the range of −4 to −2 W/m2. High median radiative forcing effect values of about −6 W/m2 were found to occur mainly in the summer months while lower values of about −1 W/m2 occur in the winter months. The aerosol surface forcing also increases in summer months and can reach values of −8 W/m2. Individual stations often have much higher values by a factor of 2. The median top-of-atmosphere aerosol radiative forcing effect efficiency is estimated to be about −25 W/m2 and their respective surface efficiency is around −35 W/m2. The fractional absorption coefficient is estimated to be 1.7, but deviates significantly from station to station. In addition, it is found that the well known peak of the aerosol radiative forcing effect at a solar zenith angle of about 75° is in fact the average of the peaks occurring at shorter and longer wavelengths. According to estimations for Central Europe, based on mean aerosol optical properties retrievals from 12 stations, the critical threshold of the aerosol single scattering albedo, between cooling and heating in the presence of an aerosol layer, is close between 0.6 and 0.76.  相似文献   

18.
Ozone tendencies due to chemistry and transport are calculated by a mesoscale model using a fine horizontal resolution (3 km × 3 km), over South-Eastern France. Over that region where the anthropogenic emissions are very strong, ozone pollution is highlighted during two intensive observations periods of the ESCOMPTE campaign, when the sea breeze penetrates far into the Durance and Rhone valleys and the up-slope breezes are developed. From a fine analysis of time series of ozone concentration at different ground stations along these valleys and from numerical results, it is possible to discriminate the tendency due to chemistry from the tendency due to dynamical processes. We can distinguish both processes, either local chemical production/loss or dynamical increase/decrease (transport, deposition) on maps of ozone budget according to the meteorological conditions. In particular, we show that the variations due to transport can be have the same order of magnitude than those due to chemistry, reaching 20 ppbv h−1, whereas those due to chemistry are around 30 ppbv h−1.  相似文献   

19.
Concentrations of manganese in 56 rain events in Wilmington, NC, USA rainwater from April 1, 2005 to March 31, 2006 were 11 ± 3 nM for dissolved Mn and 1.2 ± 0.4 nM for particulate Mn. Concentrations of both forms of Mn were higher in terrestrial storms relative to marine events. This observation along with the positive correlation of Mn with pollutant indicators suggests anthropogenic inputs to rain at this location, as has been observed at other locations. The ratio of Mnpart/Mndiss was threefold larger in summer relative to winter rain, which matched the increase of particulate to dissolved Fe in rainwater suggesting influence of Saharan dust during the summer. Like Fe in rain, Mn undergoes photoreduction in rainwater, which has also been shown to be important in Mn cycling in seawater. The flux of Mn removed from the atmosphere via wet deposition is 1.5 × 10−5 moles m−2 yr−1 at this location, which is approximately twice the flux reported from two rainwater studies conducted in the early 1980s on Bermuda. Atmospheric input of Mn to the oceans is important because Mn like Fe is an essential and potentially limiting nutrient. Experiments mixing authentic rainwater and seawater demonstrate that rainwater dissolved Mn does not rapidly precipitate in seawater suggesting wet deposition is an important source of soluble, stable Mn to surface seawater.  相似文献   

20.
The atmospheric processing by ozone of peptide-containing mixed particles was investigated as proxies for biogenic and sea spray primary organic aerosol. Reactions were performed in a flow reactor and particle composition was monitored by photoelectron resonance capture ionization aerosol mass spectrometry. Mixed particles containing dipeptides in a saturated organic matrix of stearic and palmitic acids showed no reaction under ozonolysis at exposure levels of 2.5 × 10−4 atm s O3. However reactions of mixed particles of a dipeptide (Leu-Leu) in an unsaturated matrix (oleic acid) under the same conditions resulted in a rapid loss of the peptide ion signal, as well as the carrier matrix, and appearance of a number of ion signals corresponding to secondary products. High molecular weight imides and amides have been identified corresponding to possible reactions of ozonolysis products and reactive intermediates (i.e. aldehydes, stabilized Criegee intermediates). Additionally, tautomerisation of the imides to enamines in the particle phase is postulated, with ozonolysis of the enamine followed by regioselective decomposition of the primary ozonide to form an amide whereby the peptide incorporates an aldehydic group at the N-terminus. The same general reactivity pattern was observed for mixed particles of diglycine and oleic acid. This behavior was not observed in solution phase experiments, where the tautomerisation favors the more stable imine form, indicating that particulate phase reactions of this nature may be dependent on the specific particle physical properties. The implications of this chemistry with respect the atmospheric aging of cell-derived organic aerosol are discussed.  相似文献   

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