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1.
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO4 2–), sodium (Na+), ammonium (NH4 +), and nitrate (NO3 –) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO4 2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO4 2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3 –, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.  相似文献   

2.
Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO2), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2-) were monitored during the period June 9–26, 1989 at a coastal site in Brittany. As indicated by the radon (Rn-222) activities and the high concentrations of NOx the air masses, for most of the experiment, were continental in origin. The observed concentrations range from 1.9 to 65 nmol/m3 for DMS (n=157), 0.6 to 94.2 nmol/m3 for SO2 (n=50), 0.6 to 11.6 nmol/m3 for MSA (n=44) and 42 to 350 nmol/m3 for nss-SO4 2- (n=44). Aitken nuclei reached values as high as 4.5 × 105 particles/m3. When continental conditions predominated, the measured SO2 concentrations were lower than those expected from a consideration of the observed DMS concentrations and the existence of SO2 background of the continental air masses. Similarly, compared to the MSA/DMS ratio in the marine atmosphere, higher concentrations of MSA were observed than those expected from the measured levels of DMS. The presence of enhanced levels of MSA was also endorsed by the observation that the measured mean MSA/nss-SO4 2- ratio of 6±3% was similar to the mean value of 6.9% observed in the marine atmosphere. These above observations are in line with recent laboratory findings by Barnes et al. (1988), which show an increase of the MSA/DMS yield with a simultaneous decrease of the SO2/DMS yield in the presence of NOx.  相似文献   

3.
A global three-dimensional model of the tropospheric sulfur cycle   总被引：9，自引：0，他引：9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

4.
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO4 2-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO4 2- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO4 2- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO4 2- values decreased significantly in the middle FT. NH4 +/nss-SO4 2- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium.  相似文献   

5.
Simultaneous shipboard measurements of atmospheric dimethylsulfide and hydrogen sulfide were made on three cruises in the Gulf of Mexico and the Caribbean. The cruise tracks include both oligotrophic and coastal waters and the air masses sampled include both remote marine air and air masses heavily influenced by terrestrial or coastal inputs. Using samples from two north-south Caribbean transects which are thought to represent remote subtropical Atlantic air, mean concentrations of DMS and H2S were found to be 57 pptv (74 ng S m-3, =29 pptv, n=48) and 8.5 pptv (11 ng S m-3, =5.3 pptv, n=36), respectively. The ranges of measured concentrations for all samples were 0–800 pptv DMS and 0–260 pptv H2S. Elevated concentrations were found in coastal regions and over some shallow waters. Statistical analysis reveals slight nighttime maxima in the concentrations of both DMS and H2S in the remote marine atmosphere. The diurnal nature of the H2S data is only apparent after correcting the measurements for interference due to carbonyl sulfide. Calculations using the measured ratio of H2S to DMS in remote marine air suggest that the oxidation of H2S contributes only about 11% to the excess (non-seasalt) sulfate in the marine boundary layer.  相似文献   

6.
Daily measurements of atmospheric sulfur dioxide (SO2) concentrations were performed from March 1989 to January 1991 at Amsterdam Island (37°50 S–77°30 E), a remote site located in the southern Indian Ocean. Long-range transport of continental air masses was studied using Radon (222Rn) as continental tracer. Average monthly SO2 concentrations range from less than 0.2 to 3.9 nmol m-3 (annual average = 0.7 nmol m-3) and present a seasonal cycle with a minimum in winter and a maximum in summer, similar to that described for atmospheric DMS concentrations measured during the same period. Clear diel correlation between atmospheric DMS and SO2 concentrations is also observed during summer. A photochemical box model using measured atmospheric DMS concentrations as input data reproduces the seasonal variations in the measured atmospheric SO2 concentrations within ±30%. Comparing between computed and measured SO2 concentrations allowed us to estimate a yield of SO2 from DMS oxidation of about 70%.  相似文献   

7.
Dimethylsulfide (DMS) in surface seawater and the air, methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2–) in aerosol, and radon-222 (Rn-222) were measured in the northern North Pacific, including the Bering Sea, during summer (13 July – 6 September 1997). The mean atmospheric DMS concentrations in the eastern region (21.0 ± 5.8 nmole/m3 (mean ± S.D.), n=30) and Bering Sea (19.9 ± 9.8 nmole/m3, n=10) were higher than that in the western region (11.1 ± 6.4 nmole/m3, n=31) (p<0.05), although these regions did not significantly differ in the mean DMS concentration in surface seawater. Mean sea-to-air DMS flux in the eastern region (21.0 ± 10.4 mole/m2/day, n=19) was larger than those in the western region (11.3 ± 16.9 mole /m2/day, n=22) and Bering Sea (11.2 ± 7.8 mole/m2/day, n=7) (p<0.05). This suggests that the longitudinal difference in atmospheric DMS was produced by that in DMS flux owing to wind speed, while the possible causes of the higher DMS concentrations in the Bering Sea include (1) later DMS oxidation rates, (2) lower heights of the marine boundary layer, and (3) more inactive convection. The mean MSA concentrations in the eastern region (1.18 ± 0.84 nmole/m3, n=35) and Bering Sea (1.17 ± 0.87 nmole/m3, n=13) were higher than that in the western region (0.49 ± 0.25 nmole/m3, n=28) (p < 0.05). Thus the distribution of MSA was similar to that of DMS, while the nss-SO4 2– concentrations were higher near the continent. This suggests that nss-SO4 2– concentrations were regionally influenced by anthropogenic sulfur input, because the distribution of nss-SO4 2– was similar to that of Rn-222 used as a tracer of continental air masses.  相似文献   

8.
Developments allowing the direct determination of sulfur dioxide and dimethyl sulfide in grab samples by gas chromatography/mass spectrometry with isotopically labeled standards (GC/MS/ILS) are reported. Isotopomers of DMS and SO2 are used as internal standards. Spiked air samples are dried to a dew point of <–60 °C and trapped cryogenically in loops of Teflon tubing. Sealed samples are transported to the laboratory under liquid nitrogen and later subjected to GC/MS analysis. Holding times of up to one month do not result in significant sample loss. For samples collected in a clean marine environment, concentrations of SO2 and DMS greater than 5 and 8 pptv, respectively, are significantly different from blanks at the 95% confidence level. Average measurement precision derived from a propagation of errors are 9% for SO2 and 42% for DMS at concentrations from 5–15 pptv.Improvements are outlined which should provide sensitivity and precision comparable to that of on-site GC/MS. The technique will allow increased flexibility for the determination of trace sulfur species in the field under conditions where deployment of a mass spectrometer is not possible.  相似文献   

9.
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10.
A box model, involving simple heterogeneous reaction processes associated with the production of non-sea-salt sulfate (nss-SO 4 2– ) particles, is used to investigate the oxidation processes of dimethylsulfide (DMS or CH3SCH3) in the marine atmosphere. The model is applied to chemical reactions in the atmospheric surface mixing layer, at intervals of 15 degrees latitude between 60° N and 60° S. Given that the addition reaction of the hydroxyl radical (OH) to the sulfur atom in the DMS molecule is faster at lower temperature than at higher temperature and that it is the predominant pathway for the production of methanesulfonic acid (MSA or CH3SO3H), the results can well explain both the increasing tendency of the molar ratio of MSA to nss-SO 4 2– toward higher latitudes and the uniform distribution with latitude of sulfur dioxide (SO2). The predicted production rate of MSA increases with increasing latitude due to the elevated rate constant of the addition reaction at lower temperature. Since latitudinal distributions of OH concentration and DMS reaction rate with OH are opposite, a uniform production rate of SO2 is realized over the globe. The primary sink of DMS in unpolluted air is caused by the reaction with OH. Reaction of DMS with the nitrate radical (NO3) also reduces DMS concentration but it is less important compared with that of OH. Concentrations of SO2, MSA, and nss-SO 4 2– are almost independent of NO x concentration and radiation field. If dimethylsulfoxide (DMSO or CH3S(O)CH3) is produced by the addition reaction and further converted to sulfuric acid (H2SO4) in an aqueous solution of cloud droplets, the oxidation process of DMSO might be important for the production of aerosol particles containing nss-SO 4 2– at high latitudes.  相似文献   

11.
Emissions of marine biogenic sulfur to the atmosphere of northern Europe   总被引：1，自引：0，他引：1  
Measurements of DMS and other reduced sulfur compounds in surface waters have been carried out from a helicopter in the seas surrounding Scandinavia. Average summer time concentrations of DMS ranged from 70 to 150 ngS L-1. Simultaneous measurements of biological and physical parameters revealed no correlation between DMS and phytoplankton species, species assemblages, total phytoplankton biomass, chlorophyll a, temperature, and salinity. The only exception was a correlation between DMS concentration, Chrysochromulina spp. belonging to the Prymnesiophyceae, and salinity over a narrow range of salinity in the Baltic Sea.The flux of reduced sulfur to the atmosphere in July in this region is estimated to be 120–170 gS m-2 d-1 from the Baltic, 240–810 in the Kattegat/Skagerrak, and 120–690 in the North Sea. Annual fluxes are roughly 100 times higher than these daily fluxes. On an annual basis, biogenic sulfur emissions from the coastal seas are negligible (<1%) compared to the anthropogenic emissions in northern Europe. However, during the summer months, the biogenic sulfur emissions from the seas surrounding the Scandinavian peninsula are estimated to be as high as 20–70% of the anthropogenic emissions in Scandinavia. This makes it of interest to incorporate the biogenic emissions in calculations of long-range transport and deposition of sulfur within the region.Other volatile sulfur species, mainly methyl mercaptan, contribute about 10% of the total flux of reduced sulfur. Estimated fluxes of CS2 to the atmosphere ranged from 1 gS m-2 d-1 in the Baltic Sea to 6 gS m-2 d-1 in the North Sea. No emissions for H2S or COS were detected.  相似文献   

12.
A one-month experiment was performed at Amsterdam Island in January 1998, to investigate the factors controlling the short-term variations of atmospheric dimethylsulfide (DMS) and its oxidation products in the mid-latitudes remote marine atmosphere. High mixing ratios of DMS, sulfur dioxide (SO2) and dimethylsulfoxide (DMSO) have been observed during this experiment, with mean concentrations of 395 parts per trillion by volume (pptv) (standard deviation, = 285, n = 500), 114 pptv ( = 125, n = 12) and 3 pptv ( = 1.2, n = 167), respectively. Wind speed and direction were identified as the major factors controlling atmospheric DMS levels. Changes in air temperature/air masses origin were found to strongly influence the dimethylsulfoxide (DMSO)/DMS and SO2/DMS molar ratios, in line with recent laboratory data. Methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2–) mean concentrations in aerosols during this experiment were 12.2± 6.5 pptv (1, n=47) and 59 ± 33 pptv (1, n=47), respectively. Evidence of vertical entrainment was reported following frontal passages, with injection of moisture-poor, ozone-rich air. High MSA/ nss-SO4 2– molar ratios (mean 0.44) were calculated during these events. Finally following frontal passages, few spots in condensation nuclei (CN) concentration were also observed.  相似文献   

13.
Methanesulfonate (MS–) and non-sea-salt sulfate (nss-SO 4 2– ), two of the major oxidation products of atmospheric dimethylsulfide (DMS), have been continuously measured in rainwater at three remote islands in the Southern Indian Ocean: Amsterdam since 1991, Crozet since 1992, and Kerguelen since 1993. The annual volume weighted mean (VWM) concentrations of nss-SO 4 2– in rainwater were 3.19, 3.04 and 4.57 eq l–1 at Amsterdam, Crozet, and Kerguelen, respectively while the VWM of MS– were 0.24, 0.15 and 0.30 eq l–1, respectively. At all three islands, MS– presented a well-distinguished seasonal variation with a maximum during summer whereas the seasonal variation of nss-SO 4 2– was less pronounced, possibly due to the increased anthropogenic influence during the winter period. Furthermore, MS– presented significant interannual variations, in particular at Amsterdam and Crozet, which is closely related to the sea-surface temperature (SST) anomalies). Finally, the nss-SO 4 2– deposition at Crozet Island presented a decreasing interannual trend, reflecting probably reductions in sulfur emissions from Southern Africa. On the contrary no interannual tendency was observed in the nss-SO 4 2– concentrations at Amsterdam Island, indicating that the biogeochemical sulfur cycle at this area is mainly influenced by biogenic emissions.  相似文献   

14.
Daily measurements of atmospheric concentrations of dimethylsulfide (DMS) were carried out for two years in a marine site at remote area: the Amsterdam Island (37°50S–77°31E) located in the southern Indian Ocean. DMS concentrations were also measured in seawater. A seasonal variation is observed for both DMS in the atmosphere and in the sea-surface. The monthly averages of DMS concentrations in the surface coastal seawater and in the atmosphere ranged, respectively, from 0.3 to 2.0 nmol l-1 and from 1.4 to 11.3 nmol m-3 (34 to 274 pptv), with the highest values in summer. The monthly variation of sea-to-air flux of DMS from the southern Indian Ocean ranges from 0.7 to 4.4 mol m-2 d-1. A factor of 2.3 is observed between summer and winter with mean DMS fluxes of 3.0 and 1.3 mol m-2 d-1, respectively.  相似文献   

15.
Atmospheric dimethyl sulfide (DMS) and sulfur dioxide (SO2) concentrations were measured at Baring Head, New Zealandduring February and March 2000. Anti-correlated DMS and SO2 diurnalcycles, consistent with the photochemical production of SO2 from DMS, were observed in clean southerly air off the ocean. The data is used to infer a yield of SO2 from DMS oxidation. The estimated yields are highly dependent on assumptions about the DMS oxidation rate. Fitting the measured data in a photochemical box model using model-generated OH levels and the Hynes et al. (1986) DMS + OH rate constant suggests that theSO2 yield is 50–100%, similar to current estimates for the tropical Pacific.However, the observed amplitude of the DMS diurnal cycle suggests that the oxidation rate is higher than that used by the model, and therefore, that theSO2 yield is lower in the range of 20–40%.  相似文献   

16.
DMS emissions and fluxes from the Australasian sector of the Antarctic and Subantarctic Oceans, bound by 46–68° S and 65.5–142.6° E, were determined from a limited number of samples (n=32) collected during three summer resupply voyages to Australian Antarctic continental research bases between November 1988 and January 1989 (a 92 day period). The maximum DMS emission from this sector of the Antarctic Ocean was in an area near the Antarctic Divergence (60–63° S) and the minimum DMS emission was from the Antarctic coastal and offshelf waters. The greatest emission of DMS from this sector of the Southern Ocean was from the Subantarctic waters. DMS flux from the Australasian Antarctic Ocean was 64.3×106 (±115) mol d–1 or 5.9 (±10.6)×109 mol based on an emission of 10.9 (±19.5) µmol m–2 d–1 (n=26). The flux of DMS from the Australasian sector of the Subantarctic Ocean was probably twice the flux of DMS from the adjacent Antarctic Ocean.  相似文献   

17.
Analyses of cloud condensation nuclei (CCN) number concentrations (cm− 3) measured at the Mace Head Atmospheric Research Station, near Carna, County Galway, Ireland, using a DH Associates Model M1 static thermal diffusion cloud chamber over the period from March 1994 to September 2002 are presented in this work. Air masses are defined as being ‘marine’ if they originate from a wind direction of 180–300° and ‘continental’ air masses are defined as originating from a wind direction of 45–135°. Air masses without such filtering were classified as ‘undefined’ air masses. Air masses were found to be dominated by marine sector air, re-affirming Mace Head as a baseline atmospheric research station. CCN levels for specific air masses at Mace Head were found to be comparable with earlier studies both at Mace Head and elsewhere. Monthly averaged clean marine (wind direction of 180–300° and black carbon absorption coefficient < 1.425 Mm− 1) CCN and marine CCN varied between 15–247 cm− 3 and 54–670 cm− 3, respectively. As expected, significant increases in number concentration were found in continentally sourced CCN over that of marine CCN and were found to follow a log-normal distribution significantly tighter than that of clean marine air masses. No significant trend was found for CCN over the 9-year period. While polluted continental air masses showed a slight increase in CCN concentrations over the winter months, most likely due to increased fuel usage and a lower mixed boundary layer, the dominance of marine sector air arriving at Mace Head, which generally consists of background CCN concentrations, reduced seasonal differences for polluted air. Marine air showed a distinct seasonal pattern, with elevated values occurring over the spring and summer seasons. This is thought to be due to enhanced biogenic aerosol production as a result of phytoplankton bloom activity in the North Atlantic.  相似文献   

18.
A box model was constructed to investigate connections between the particulate MSA to non-sea-salt sulfate ratio, R, and DMS chemistry in a clean marine boundary layer. The simulations demonstrated that R varies widely with particle size, which must be taken into account when interpreting field measurements or comparing them with each other. In addition to DMS gas-phase chemistry, R in the submicron size range was shown to be sensitive to the factors dictating sulfate production via cloud processing, to the removal of SO2 from the boundary layer by dry deposition and sea-salt oxidation, to the entrainment of SO2 from the free troposphere, to the relative concentration of sub- and supermicron particles, and to meteorology. Three potential explanations for the increase of R toward high-latitudes during the summer were found: larger MSA yields from DMS oxidation at high latitudes, larger DMSO yields from DMS oxidation followed by the conversion of DMSO to MSA at high latitudes, or lower ambient H2O2 concentrations at high latitudes leading to less efficient sulfate production in clouds. Possible reasons for the large seasonal amplitude of R at mid and high latitudes include seasonal changes in the partitioning of DMS oxidation to the OH and NO3 initiated pathways, seasonal changes in the concentration of species participating the DMS-OH reaction pathway, or the existence of a SO2 source other than DMS oxidation in the marine boundary layer. Even small anthropogenic perturbations were shown to have a potential to alter the MSA to non-sea-salt sulfate ratio.  相似文献   

19.
Airborne measurements of volatile organic compounds (VOC) were performed overthe tropical rainforest in Surinam (0–12 km altitude,2°–7° N, 54°–58° W) using the proton transferreaction mass spectrometry (PTR-MS) technique, which allows online monitoringof compounds like isoprene, its oxidation products methyl vinyl ketone,methacrolein, tentatively identified hydroxy-isoprene-hydroperoxides, andseveral other organic compounds. Isoprene volume mixing ratios (VMR) variedfrom below the detection limit at the highest altitudes to about 7 nmol/molin the planetary boundary layer shortly before sunset. Correlations betweenisoprene and its product compounds were made for different times of day andaltitudes, with the isoprene-hydroperoxides showing the highest correlation.Model calculated mixing ratios of the isoprene oxidation products using adetailed hydrocarbon oxidation mechanism, as well as the intercomparisonmeasurement with air samples collected during the flights in canisters andlater analysed with a GC-FID, showed good agreement with the PTR-MSmeasurements, in particular at the higher mixing ratios.Low OH concentrations in the range of 1–3 × 105molecules cm-3 averaged over 24 hours were calculated due to lossof OH and HO2 in the isoprene oxidation chain, thereby stronglyenhancing the lifetime of gases in the forest boundary layer.  相似文献   

20.
本文利用一维光化学模式，以二甲硫醚（ＤｉｍｅｔｈｙｌＳｕｌｆｉｄｅ，简称ＤＭＳ）为源模拟了西太平洋对流层的硫化物循环。ＤＭＳ海－气通量由“ｓｔａｇｎａｎｔ－ｆｉｌｍ”模式进行计算。尽管海洋大气中ＯＣＳ浓度比ＤＭＳ大一个量级，但它对ＳＯ２的贡献很小，ＤＭＳ仍是海洋大气中ＳＯ２的主要源。在大气垂直湍流输送过程中，ＤＭＳ白天与ＯＨ反应，夜间与ＮＯ３反应被氧化成ＳＯ２，ＳＯ２大部分通过非均相转化形成Ｈ２ＳＯ４。模拟结果与ＰＥＭ－ＷＥＳＴ－Ａ观测资料对比，取得了较好的一致性。  相似文献   

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