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1.
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   

2.
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   

3.
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   

4.
We use a global atmospheric chemistry transport model to study the possible influence of aqueous phase reactions of peroxynitric acid (HNO4) on the concentrations and budgets of NOx, SOx, O3 and H2O2. Laboratory studies have shown that the aqueous reaction of HNO4aq withHSO 3aq, and the uni-molecular decomposition of the NO4 anion to form NO2 (nitrite) occur on a time scale of about a second. Despite a substantial contribution of the reaction of HSO 3aq with HNO4aq to the overall in-cloud conversion of SO2 to SO4 2–, a simultaneous decrease of other oxidants (most notably H2O2) more than compensated the increase in SO4 2– production. The strongest influence of heterogeneous HNO4 chemistry was found in the boundary layer, where calculated monthly average ozone concentrations were reduced between 2% to 10% andchanges of H2O2 between –20% to +10%compared to a simulation which ignores this reaction. Furthermore, SO2 was increased by 10% to 20% and SO4 2–depleted by up to 10%. Since the resolution of our global model does not enable a detailed comparison with measurements in polluted regions, it is not possible to verify whether considering heterogeneous HNO4 reactions results in a substantial improvement of atmospheric chemistry transport models. However, the conversion of HNO4 in the aqueous phase seems to be efficient enough to warrant further laboratory investigations and more detailed model studies on this topic.  相似文献   

5.
This study reports comparisonsbetween model simulations, based on current sulfurmechanisms, with the DMS, SO2 and DMSOobservational data reported by Bandy et al.(1996) in their 1994 Christmas Island field study. For both DMS and SO2, the model results werefound to be in excellent agreement with theobservations when the observations were filtered so asto establish a common meteorological environment. Thisfiltered DMS and SO2 data encompassedapproximately half of the total sampled days. Basedon these composite profiles, it was shown thatoxidation of DMS via OH was the dominant pathway withno more than 5 to 15% proceeding through Cl atoms andless than 3% through NO3. This analysis wasbased on an estimated DMS sea-to-air flux of 3.4 ×109 molecs cm-2 s-1. The dominant sourceof BL SO2 was oxidation of DMS, the overallconversion efficiency being evaluated at 0.65 ± 0.15. The major loss of SO2 was deposition to theocean's surface and scavenging by aerosol. Theresulting combined first order k value was estimated at 1.6 × 10-5 s-1. In contrast to the DMSand SO2 simulations, the model under-predictedthe observed DMSO levels by nearly a factor of 50. Although DMSO instrument measurement problems can notbe totally ruled out, the possibility of DMSO sourcesother than gas phase oxidation of DMS must beseriously considered and should be explored in futurestudies.  相似文献   

6.
Kinetics and products of the gas-phase reactions of dimethylsulphide (DMS), dimethylsulphoxide (DMSO) and dimethylsulphone (DMSO2) with Br atoms and BrO radicals in air have beeninvestigated using on-line Fourier Transform Infrared Spectroscopy (FT-IR) as analytical technique at 740 ± 5 Torr total pressure and at 296 ± 3 K in a480 L reaction chamber. Using a relative rate method for determining the rate constants; the following values (expressed in cm3molecule–1 s–1) were found: kDMS+Br = (4.9 ±1.0) ×10–14, kDMSO + Br < 6 × 10–14,kDMSO 2 + Br 1 × 10–15,kDMSO + BrO = (1.0 ± 0.3) × 10–14 andkDMSO 2 + BrO 3 × 10–15 (allvalues are given with one on the experimental data). DMSO, SO2, COS, CH3SBr andCH3SO2Br were identified as the main sulphur containing products of the oxidation of DMS by Br atoms. From the reaction between DMSO and Br atoms, DMSO2and CH3SO2Br were the only sulphur containing products thatwere identified. DMSO, DMSO2 and SO2 were identified as themain sulphur containing products of the reaction between DMS and BrO.DMSO2 was found to be the only product of the reaction between DMSO and BrO. For the reactions of DMSO2 with Br and BrO no products were identified because the reactions were too slow.The implications of these results for atmospheric chemistry are discussed.  相似文献   

7.
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   

8.
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   

9.
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   

10.
A photochemical box model is used to simulate seasonal variations in concentrations of sulfur compounds at latitude 40° S. It is assumed that the hydroxyl radical (OH) addition reaction to sulfur in the dimethyl sulfide (DMS) molecule is the predominant pathway for methanesulfonic acid (MSA) production, and that the rate constant increases as the air temperature decreases. Concentration of the nitrate radical (NO3) is a function of the DMS flux, because the reaction of DMS with NO3 is the most important loss mechanism of NO3. While the diurnally averaged concentration of OH in winter is a factor of about 8 smaller than in summer, due to the weak photolysis process, the diurnally averaged concentration of NO3 in winter is a factor of about 4–5 larger than in summer, due to the decrease of DMS flux. Therefore, at middle and high latitudes in winter, atmospheric DMS is mainly oxidized by the reaction with NO3. The calculated ratio of the MSA to SO2 production rates is smaller in winter than in summer, and the MSA to non-sea-salt sulfate (nssSO4 2-) molar ratio varies seasonally. This result agrees with data on the seasonal variation of the MSA/nssSO4 2- molar ratio obtained at middle and high latitudes. The calculations indicate that during winter the reaction of DMS with NO3 is likely to be a more important sink of NOx (NO+NO2) than the reaction of NO2 with OH, and to serve as a significant pathway of the HNO3 production. If dimethyl sulfoxide (DMSO) is produced through the OH addition reaction and is heterogeneously oxidized in aqueous solutions, half of the nssSO4 2- produced in summer may be through the oxidation process of DMSO. It is necessary to further investigate the oxidation products by the reaction of DMS with OH, and the possibility of the reaction of DMS with NO3 during winter.  相似文献   

11.
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   

12.
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   

13.
Dimethyl sulfide (DMS) and sulfur dioxide (SO2) mixing ratios were measured in the boundary layer on Oahu, Hawaii in April and May 2000. Average DMS and SO2 levels were 22 ± 7 (n = 488) pmol/mol and 23 ± 7 (n = 471) pmol/mol respectively. Anti-correlated DMS and SO2 diurnal cycles, consistent with DMS + OH oxidation were observed on most days. Photochemical box model simulations suggest that the yield of SO2 and total SO2 sink are ∼85% and ∼2 × 104 molec cm− 3 s− 1 respectively. On several days the rate of decrease in DMS and increase in SO2 levels in the early morning were larger that predicted by the model. Dynamical and chemical causes for the anomalous early morning data are explored.  相似文献   

14.
Using a filter radiometer, the meridional profile of the NO2 photolysis frequency, J(NO2), was measured between 50° N and 30° S during the cruise ANTVII/1 September/October 1988 of the research vessel Polarstern on the Atlantic Ocean. Simultaneously, global broadband irradiance and acrosol were monitored. Clean marine background air with low aerosol loads (b sp=(1–2)×10-5 m-1) was encountered at the latitudes 25° N–30° N and 18° S–27° S, respectively. Under these conditions and an almost cloudless sky J(NO2) reached 7.3×10-3 s-1 (2 sr) for a zenith angle of 30°. Between 30° N and 30° S, the latitudinal variation of the J(NO2) noontime maxima was less than ± 10%, while the mean value at noon was 7.8×10-3 s-1. For the set of all data between 50° N and 30° S, a nearly linear correlation of J(NO2) vs. global broadland irradiance was found. The slope of (8.24±0.03)×10-5 s-1/mW cm-2 agrees within 10% with observations in Jülich (51° N, 6.2° E).  相似文献   

15.
The Pacific Atmospheric Sulfur Experiment (PASE) is the first sulfur-budget field experiment to feature simultaneous flux measurements of DMS marine emissions and SO2 deposition to the ocean surface. We make use of these data to constrain a 1-D chemical transport model to study the production and loss pathways for DMS and SO2 over the equatorial Pacific. Model results suggest that OH is the main sink for DMS in the boundary layer (BL), and the average DMS-to-SO2 conversion efficiency is ~73%. In an exploratory run involving the addition of 1 pptv of BrO as a second oxidant, a 14% increase in the DMS flux is needed beyond that based on OH oxidation alone. This BrO addition also reduces the DMS-to-SO2 conversion efficiency from 73% to 60%. The possibility of non-DMS sources of marine sulfur influencing the estimated conversion efficiency was explored and found to be unconvincing. For BL conditions, SO2 losses consist of 48% dry deposition, while transport loss to the BuL and aerosol scavenging each account for another 19%. The conversion of SO2 to H2SO4 consumes the final 14%. In the BuL, cloud scavenging removes 85% of the SO2, thus resulting in a decreasing vertical profile for SO2. The average SO2 dry deposition velocity from direct measurements (i.e., 0.36 cm sec−1) is approximately 50% of what is calculated from the 1-D model and the global GEOS-Chem model. This suggests that the current generation of global models may be significantly overestimating SO2 deposition rates over some tropical marine areas. Although the specific mechanism cannot be determined, speculation here is that the dry deposition anomalous results may point to the presence of a micro-surface chemical phenomenon involving partial saturation with either S(IV) and/or S(VI) DMS oxidation products. This could also appear as a pH drop in the ocean’s surface microfilm layer in this region. Finally, we propose that the enhanced SO2 level observed in the lower free troposphere versus that in the upper BuL during PASE is most likely the result of transported DMS/SO2-rich free-tropospheric air parcels from the east of the PASE sampling area, rather than an inadequate representation in the model of local convection.  相似文献   

16.
A three-dimensional model of the global ammonia cycle   总被引:16,自引:0,他引:16  
Using a three-dimensional (3-D) transport model of the troposphere, we calculated the global distributions of ammonia (NH3) and ammonium (NH 4 + ), taking into account removal of NH3 on acidic aerosols, in liquid water clouds and by reaction with OH. Our estimated global 10°×10° NH3 emission inventory of 45 Tg N-NH3 yr provides a reasonable agreement between calculated wet NH 4 + deposition and measurements and of measured and modeled NH 4 + in aerosols, although in Africa and Asia especially discrepancies exist.NH3 emissions from natural continental ecosystems were calculated applying a canopy compensation point and oceanic NH3 emissions were related to those of DMS (dimethylsulfide). In many regions of the earth, the pH found in rain and cloud water can be attributed to acidity derived from NO, SO2 and DMS emissions and alkalinity from NH3. In the remote lower troposphere, sulfate aerosols are calculated to be almost neutralized to ammonium sulfate (NH4)2SO4, whereas in the middle and upper troposphere, according to our calculations, the aerosol should be more acidic, as a result of the oxidation of DMS and SO2 throughout the troposphere and removal of NH3 on acidic aerosols at lower heights. Although the removal of NH3 by reaction with the OH radical is relatively slow, the intermediate NH2 radical can provide a substantial annual N2O source of 0.9 –0.4 +0.9 Tg, thus contributing byca. 5% to estimated global N2O production. The oxidation by OH of NH3 from anthropogenic sources accounts for 10% of the estimated total anthropogenic sources of N2O. This source was not accounted for in previous studies, and is mainly located in the tropics, which have high NH3 and OH concentrations. Biomass burning plumes, containing high NO x and NH3 concentrations provide favourable conditions for gas phase N2O production. This source is probably underestimated in this model study, due to the coarse resolution of the 3-D model, and the rather low biomass burning NH3 and NO x emissions adopted. The estimate depends heavily on poorly known concentrations of NH3 (and NO x ) in the tropics, and uncertainties in the rate constants of the reactions NH2 + NO2 N2O + H2O (R4), and NH2 + O3 NH2O + O2 (R7).  相似文献   

17.
The photochemical oxidation of SO2 in the presence of NO and C3H6 was studied in a 18.2 liter pyrex reactor. When light intensity, irradiation time and SO2 concentration were constant, SO4 2- concentration, derived from the total volume of aerosol produced, peaked when [C3H6]/[NO] was approximately 6.0. Another increase im SO4 2- formation was reached at very high ratios (>50). The experimental observations are consistent with the two SO2 oxidation mechanisms. At low [C3H6]/[NO] ratios, the processes proceed via the HO–SO2 reaction, while at high ratios the O3–C3H6 adduct is assumed to oxidize SO2 to produce SO4 2- aerosols.  相似文献   

18.
Lightning is thought to represent an important source of tropospheric reactive nitrogen species NOx (NO + NO2),but estimates of global production of NOx by lightning varyconsiderably. We evaluate the production of NOx by lightning using a global chemical/transport model, satellite lightning observations, and airborne NOx measurements. Various model calculations are conducted toassess the global NOx production rate of lightning by comparing the model calculations with airborne measurements. The results show that the simulated NOx in the tropical middle and upper troposphere are very sensitiveto the amount and altitude of the lightning NOx used in the model. A global lightning NOx production of 7 Tg N yr–1uniformly distributed in convective clouds or 3.5 Tg N yr–1 distributedin the upper cloud regions produces good agreement between calculated and measured NOx concentrations in the tropics.  相似文献   

19.
We present here experimental determinations of mass accommodation coefficients using a low pressure tube reactor in which monodispersed droplets, generated by a vibrating orifice, are brought into contact with known amounts of trace gases. The uptake of the gases and the accommodation coefficient are determined by chemical analysis of the aqueous phase.We report in this article measurements of exp=(6.0±0.8)×10–2 at 298 K and with a total pressure of 38 Torr for SO2, (5.0±1.0)×10–2 at 297 K and total pressure of 52 Torr for HNO3, (1.5±0.6)×10–3 at 298 K and total pressure of 50 Torr for NO2, (2.4±1.0)×10–2 at 290 K and total pressure of 70 Torr for NH3.These values are corrected for mass transport limitations in the gas phase leading to =(1.3±0.1)×10–1 (298 K) for SO2, (1.1±0.1)×10–1 (298 K) for HNO3, (9.7±0.9)×10–2 (290 K) for NH3, (1.5±0.8)×10–3 (298 K) for NO2 but this last value should not be considered as the true value of for NO2 because of possible chemical interferences.Results are discussed in terms of experimental conditions which determine the presence of limitations on the mass transport rates of gaseous species into an aqueous phase, which permits the correction of the experimental values.  相似文献   

20.
A global data set on the geographic distribution and seasonality of freshwater wetlands and rice paddies has been compiled, comprising information at a spatial resolution of 2.5° by latitude and 5° by longitude. Global coverage of these wetlands total 5.7×106 km2 and 1.3×106 km2, respectively. Natural wetlands have been grouped into six categories following common terminology, i.e. bog, fen, swamp, marsh, floodplain, and shallow lake. Net primary productivity (NPP) of natural wetlands is estimated to be in the range of 4–9×1015 g dry matter per year. Rice paddies have an NPP of about 1.4×1015 g y–1. Extrapolation of measured CH4 emissions in individual ecosystems lead to global methane emission estimates of 40–160 Teragram (1 Tg=1012 g) from natural wetlands and 60–140 Tg from rice paddies per year. The mean emission of 170–200 Tg may come in about equal proportions from natural wetlands and paddies. Major source regions are located in the subtropics between 20 and 30° N, the tropics between 0 and 10° S, and the temperate-boreal region between 50 and 70° N. Emissions are highly seasonal, maximizing during summer in both hemispheres. The wide range of possible CH4 emissions shows the large uncertainties associated with the extrapolation of measured flux rates to global scale. More investigations into ecophysiological principals of methane emissions is warranted to arrive at better source estimates.  相似文献   

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