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1.
Measurements of various sulphur gases in a coastal marine environment   总被引：4，自引：0，他引：4  
Measurements of several sulphur gases have been made in coastal seawaters (including microlayers) and marine air off Great Yarmouth, U.K., and in a freshwater lake. The results show dimethyl sulphide to be the dominant sulphur gas in all the waters examined, with lesser amounts of carbonyl sulphide and carbon disulphide. For the marine air and water samples carbonyl sulphide showed no significant seasonal variation in concentration. The seawater was always supersaturated with respect to the carbonyl sulphide concentration in the air; the mean saturation value being 4.6. Likewise the seawater was always supersaturated with dimethyl sulphide, but for this gas the concentrations in the water showed substantial seasonal variation (× 40), with a maximum value of about 500 ng(S) l-1 in late June, approximately contemporaneous with the second plankton bloom in the region.Sea surface microlayers harvested cryogenically showed a mean enrichment of 2.4 relative to subsurface water for carbonyl sulphide. Some part of the observed microlayer enrichment for this gas may be due to freezing-on of atmospheric carbonyl sulphide onto the frozen microlayer sample. In general, microlayer samples did not exhibit a significant enrichment for dimethyl sulphide. However, under conditions of high biological production, enrichments of several-fold were found, but may be attributable, at least in part, to biological production of dimethyl sulphide in the microlayer water in the period between collection and analysis.  相似文献   

2.
Release and uptake of carbonyl sulfide (OCS) were measured at 25°C in samples of three forest soils (BL, BW, PBE) and one soil from a rape field (RA). The soil samples were flushed with a constant flow of either air (oxic conditions) or nitrogen (anoxic conditions) containing defined concentrations of OCS. A cryogenic trapping technique with liquid argon (-186 °C) was used to collect gas samples for analysis in a gas chromatograph equipped with a flame-photometric detector. The dependence of net OCS fluxes between soil and atmosphere could be described by a simple model of simultaneous OCS production and OCS uptake. By using this model, production rates (P), uptake rate constants (k) and compensation concentrations (m c ) of OCS could be determined as function of the soil type and the incubation conditions. Under oxic conditions, OCS production (P) and uptake were observed in all soils tested. However, the compensation concentrations (<166 ng l-1; 1 ng OCS l-1=0.41 ppbv) that were calculated from the model were high relative to the ambient OCS concentration (ca. 0.5 ppbv). The production rates (0.16–1.9 ng h-1 g-1 dw) that were actually measured when flushing the soil samples with air containing zero OCS were smaller than those (17–114 ng h-1 g-1 dw) calculated from the model. This observation was explained by two different concepts: one assuming the existence of a threshold concentration (m t ) below which OCS was no longer consumed in the soil; the other assuming the existence of two different OCS consumption processes, of which only the process active at elevated OCS concentrations was covered by the experiments. The latter concept allowed the estimation of OCS compensation concentrations that were partially low enough to allow the uptake of atmospheric OCS by soil. Both OCS production and uptake in PBE soil were dependent on soil temperature (optimum 20 °C) indicating a microbial process. However, both production and consumption of OCS were not consistently inhibited by sterilization of the soil, suggesting that they were not exclusively due to microbiological processes. Under anoxic conditions, OCS was also produced, but was not consumed except in one soil (RA). Production of OCS in the soils was stimulated after addition of thiocyanate, but not thiourea, thiosulfate, thioglycolate, tetrathionate, sulfate, elemental sulfur, cysteine and methionine.  相似文献   

3.
A two-dimensional model of global atmospheric transport is used to relate estimated air-to-surface exchanges of carbon dioxide (CO2) to spatial and temporal variations of atmospheric CO2 concentrations and isotopic composition. The atmospheric model coupled with models of the biosphere and mixed layer of the ocean describes the gross features of the global carbon cycle. In particular this paper considers the change in isotopic composition due to interreservoir exchanges and thus the potential application and measurement requirements of new isotopic observational programs.A comparison is made between the model-generated CO2 concentration variation and those observed on secular, interannual and seasonal time scales and spatially through the depth of the troposphere and meridionally from pole-to-pole.The relationship between isotopic and concentration variation on a seasonal time-scale is discussed and it is shown how this can be used to quantitatively estimate relative contributions of biospheric and oceanic CO2 exchange. Further, it is shown that the interhemispheric gradient of concentration and isotopic ratio results primarily from the redistribution of fossil fuel CO2. Both isotopic and concentration data indicate that tropical deforestation contributes less than 2 Gt yr-1 of carbon to the atmosphere.The study suggests that changes in the rate of change of the ratio of 13C to 12C in the atmosphere of less than 0.03 yr-1 might be expected if net exchanges with the biosphere are the cause of interannual variations of CO2 concentrations.  相似文献   

4.
In the current study, we quantified changes in the growth and alkaloid content of wild poppy, (Papaver setigerum) as a function of recent and projected changes in global atmospheric carbon dioxide concentration, [CO2]. The experimental [CO2] values (300, 400, 500 and 600μmol mol?1) correspond roughly to the concentrations that existed during the middle of the twentieth century, the current concentration, and near and long-term projections for the current century (2050 and 2090), respectively. Additional carbon dioxide resulted in significant increases in leaf area and above ground biomass for P. setigerum at all [CO2] relative to the 300μmol mol?1 baseline. Reproductively, increasing [CO2] from 300 to 600μmol mol?1 increased the number of capsules, capsule weight and latex production by 3.6, 3.0 and 3.7×, respectively, on a per plant basis. Quantification of secondary compounds (i.e. those not involved in primary metabolism) included the alkaloids morphine, codeine, papaverine and noscapine. The amount of all alkaloids increased significantly on a per plant basis, with the greatest relative increase occurring with recent increases in atmospheric carbon dioxide (e.g. from 300 to 400μmol mol?1). Overall, these data suggest that as atmospheric [CO2] continues to increase, significant effects on the production of secondary plant compounds of pharmacological interest (i.e. opiates) could be expected.  相似文献   

5.
Extensive ambient concentration and flux measurements have been performed in the heavily polluted region of Cubatão/Brazil. Substantial contribution of anthropogenic sources to the local reduced sulfur burden has been observed. As a result of this atmospheric sulfur burden average gas exchange between vegetated soils and the atmosphere shows net deposition. Based mainly on own field measurements a local budget for H2S, COS, and CS2 has been made up in order to calculate anthropogenic emissions. All major sources and sinks in the chosen atmospheric reservoir (24×20×1 km) have been taken into account. Due to the small reservoir size fluxes across its boundaries are dominant sources and sinks. The differences between outflux and influx therefore account for the unknown anthropogenic emissions which have been determined to be 80±10 (H2S), 66±15 (COS), and 29±6 Mmol year-1 (CS2). Other sources and sinks like natural emissions, chemical conversion, and dry deposition turned out to be of minor importance on a local scale. In fact, inside the investigated reservoir natural emissions were below 0.5% of anthropogenic emissions. Anthropogenic emissions of H2S, COS, and CS2 quantified in this work have been compared with global emission estimates for these compounds made by other authors. We conclude that global anthropogenic emissions of reduced sulfur compounds especially of COS and CS2 are currently under-estimated.  相似文献   

6.
During the hydrological survey from November 4 to 9, 2009, the underway measurements of pH, temperature, and salinity of the surface water in the Peter the Great Bay were carried out using the cell without the liquid junction in the running system. Using the measurement data, the partial pressure of carbon dioxide (pCO2) was computed which was below its atmospheric value and varied from 290 to 360μatm. Thus, during the period under study, the surface water of the bay forms the runoff for the atmospheric carbon dioxide. The minimum values of pCO2 are associated with the warm stream entering the bay from the southwestern part of the open sea. The maximum values of pCO2 are associated with the local upwelling of bottom waters. It is suggested that the horizontal convection caused by the nonuniform cooling of coastal water in the autumn forms the revealed mesoscale dynamic structures.  相似文献   

7.
A coupled climate–carbon cycle model composed of a process-based terrestrial carbon cycle model, Sim-CYCLE, and the CCSR/NIES/FRCGC atmospheric general circulation model was developed. We examined the multiple temporal scale functions of terrestrial ecosystem carbon dynamics induced by human activities and natural processes and evaluated their contribution to fluctuations in the global carbon budget during the twentieth century. Global annual net primary production (NPP) and heterotrophic respiration (HR) increased gradually by 6.7 and 4.7%, respectively, from the 1900s to the 1990s. The difference between NPP and HR was the net carbon uptake by natural ecosystems, which was 0.6 Pg C year?1 in the 1980s, whereas the carbon emission induced by human land-use changes was 0.5 Pg C year?1, largely offsetting the natural terrestrial carbon sequestration. Our results indicate that monthly to interannual variation in atmospheric CO2 growth rate anomalies show 2- and 6-month time lags behind anomalies in temperature and the NiNO3 index, respectively. The simulated anomaly amplitude in monthly net carbon flux from terrestrial ecosystems to the atmosphere was much larger than in the prescribed air-to-sea carbon flux. Fluctuations in the global atmospheric CO2 time series were dominated by the activity of terrestrial vegetation. These results suggest that terrestrial ecosystems have acted as a net neutral reservoir for atmospheric CO2 concentrations during the twentieth century on an interdecadal timescale, but as the dominant driver for atmospheric CO2 fluctuations on a monthly to interannual timescale.  相似文献   

8.
The concept of global warming potential was developed as a relative measure of the potential effects on climate of a greenhouse gas as compared to CO2. In this paper a series of sensitivity studies examines several uncertainties in determination of Global Warming Potentials (GWPs). For example, the original evaluation of GWPs for the Intergovernmental Panel on Climate Change (IPCC, 1990) did not attempt to account for the possible sinks of carbon dioxide (CO2) that could balance the carbon cycle and produce atmospheric concentrations of CO2 that match observations. In this study, a balanced carbon cycle model is applied in calculation of the radiative forcing from CO2. Use of the balanced model produces up to 21% enhancement of the GWPs for most trace gases compared with the IPCC (1990) values for time horizons up to 100 years, but a decreasing enhancement with longer time horizons. Uncertainty limits of the fertilization feedback parameter contribute a 20% range in GWP values. Another systematic uncertainty in GWPs is the assumption of an equilibrium atmosphere (one in which the concentration of trace gases remains constant) versus a disequilibrium atmosphere (one in which the concentration of trace gases varies with time). The latter gives GWPs that are 19 to 32% greater than the former for a 100 year time horizons, depending upon the carbon dioxide emission scenario chosen. Five scenarios are employed: constant-concentration, constant-emission past 1990 and the three IPCC (1992) emission scenarios. For the analysis of uncertainties in atmospheric lifetime (τ) the GWP changes in direct proportion toτ for short-lived gases, but to a lesser extent for gases withτ greater than the time horizontal for the GWP calculation.  相似文献   

9.
We use recent advances in time series econometrics to estimate the relation among emissions of CO2 and CH4, the concentration of these gases, and global surface temperature. These models are estimated and specified to answer two questions; (1) does human activity affect global surface temperature and; (2) does global surface temperature affect the atmospheric concentration of carbon dioxide and/or methane. Regression results provide direct evidence for a statistically meaningful relation between radiative forcing and global surface temperature. A simple model based on these results indicates that greenhouse gases and anthropogenic sulfur emissions are largely responsible for the change in temperature over the last 130 years. The regression results also indicate that increases in surface temperature since 1870 have changed the flow of carbon dioxide to and from the atmosphere in a way that increases its atmospheric concentration. Finally, the regression results for methane hint that higher temperatures may increase its atmospheric concentration, but this effect is not estimated precisely.  相似文献   

10.
Atmospheric concentrations of several reduced sulphur compounds (H2S, COS, CH3SH, CH3SCH3, CS2) originating from both natural and anthropogenic sources were measured at a number of locations in the All Saints Bay area and Reconcavo Baiano, Brazil.The volatile reduced sulphur compounds were collected by pre-concentration using cryo-tubes. Analysis of these compounds was carried out at a later date using gas chromatography with a flame photometric detector. In areas dominated by biogenic sources, the COS concentration varied between 0.5 and 1.0 ppbv, consistent with its normal global distribution in the atmosphere.Areas without direct industrial influence showed low atmospheric concentrations for all volatile sulphur compounds ( 0.25 ppbv).The anthropogenic influence of the Petrochemical Complex in Camaçari resulted in relatively high levels of some reduced sulphur compounds, such as COS (8 ppbv), CH3SH (1.50 ppbv), H2S (1.35 ppbv) and CS2 (0.3 ppbv). In mangrove areas, the H2S concentrations (0.2 ppbv) were almost twice as high as those in the air masses arriving from the Atlantic Ocean. The maximum H2S concentrations were found in the industrial area of the Petrochemical Complex in Camaçari, but did not reach the limit of human perception (0.14 ppbv) and rarely reached the typical recognizable smelling level (0.40 ppbv). Industrial emissions from the Landulfo Alves Refinery increased the COS, DMS and CS2 concentrations to 2.0, 0.55 and 0.2 ppbv, respectively.  相似文献   

11.
The diurnal-to-monthly behavior of the fluxes of OCS, H2S, and CS2 from a mixed-Spartina grass-covered site in a Wallops Island salt water marsh was determined through a series of experiments in August and September, 1982. Absolute flux values were determined for OCS and H2S, while only relative values were determined for CS2. The rates of emission of OCS and H2S were observed to vary diurnally and to be strongly influenced by tides. The time-averaged flux values show that such mixed-Spartina stands are insignificant ( 1%) global sources of H2S or CS2 and insignificant contributors to the global OCS cycle (< 1%). These results demonstrate that some marsh regions play a minor role in the global sulfur budget and, consequently, that the inclusion of such areas in extrapolations of measurements of more productive regions could lead to an overestimate of the role of salt water marshes in the global sulfur budget.  相似文献   

12.
The net fluxes of carbonyl sulfide (COS) and carbon disulfide (CS2) to the atmosphere from nitrogen amended and unamended deciduous and coniferous forest soils were measured during the spring of 1986. We found that emissions of these gases from acidic forest soils were substantially increased after nitrogen fertilization. The total (COS+CS2) emissions were increased by nearly a factor of three in the hardwood stand and were more than doubled in the pine stand. Furthermore, vegetation type appeared to have an influence on which was the dominant sulfur gas released from the forest soils. The added nitrogen caused a dramatic increase in COS emissions from the hardwood stand (a factor of three increase), while CS2 emissions from this site were not affected. We observed the opposite response in the pine stand; that is, the nitrogen fertilization had no affect on COS emissions, but did stimulate CS2 emissions (a factor of more than nine increase).  相似文献   

13.
Ocean emissions of inorganic and organic iodine compounds drive the biogeochemical cycle of iodine and produce reactive ozone-destroying iodine radicals that influence the oxidizing capacity of the atmosphere. Di-iodomethane (CH2I2) and chloro-iodomethane (CH2ICl) are the two most important organic iodine precursors in the marine boundary layer. Ship-borne measurements made during the TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogens and Oxygenated VOC) field campaign in the east tropical Pacific Ocean in January/February 2012 revealed strong diurnal cycles of CH2I2 and CH2ICl in air and of CH2I2 in seawater. Both compounds are known to undergo rapid photolysis during the day, but models assume no night-time atmospheric losses. Surprisingly, the diurnal cycle of CH2I2 was lower in amplitude than that of CH2ICl, despite its faster photolysis rate. We speculate that night-time loss of CH2I2 occurs due to reaction with NO3 radicals. Indirect results from a laboratory study under ambient atmospheric boundary layer conditions indicate a k CH2I2+NO3 of ≤4 × 10?13 cm3 molecule?1 s?1; a previous kinetic study carried out at ≤100 Torr found k CH2I2+NO3 of 4 × 10?13 cm3 molecule?1 s?1. Using the 1-dimensional atmospheric THAMO model driven by sea-air fluxes calculated from the seawater and air measurements (averaging 1.8 +/? 0.8 nmol m?2 d?1 for CH2I2 and 3.7 +/? 0.8 nmol m?2 d?1 for CH2ICl), we show that the model overestimates night-time CH2I2 by >60 % but reaches good agreement with the measurements when the CH2I2 + NO3 reaction is included at 2–4 × 10?13 cm3 molecule?1 s?1. We conclude that the reaction has a significant effect on CH2I2 and helps reconcile observed and modeled concentrations. We recommend further direct measurements of this reaction under atmospheric conditions, including of product branching ratios.  相似文献   

14.
A novel cryogenic sampling method combining the matrix isolation technique with FTIR spectroscopy has been developed for atmospheric trace gas analysis. It is applicable to a wide range of molecules with detection limits typically in the 10–50 ppt range. The method is described along with some measurements of N2O, CFCl3, CF2Cl2, OCS, CS2, SO2 and PAN from samples collected at ground level and from an aircraft between 9 and 14 km.  相似文献   

15.
Rate coefficients have been measured for the gas phasereactions of hydroxyl (OH) radicals and ozone with twounsaturated esters, allyl acetate(CH3C(O)OCH2CH=CH2) and isopropenylacetate (CH3C(O)OC(CH3)=CH2). The OHexperiments were carried out using the pulsed laserphotolysis – laser induced fluorescence technique overthe temperature range 243–372 K and the kinetic dataused to derive the following Arrhenius expressions (inunits of cm3 molecule-1 s-1): allylacetate, k 1 = (2.33 ± 0.27) ×10-12 exp[(732 ± 34)/T]; and isopropenyl acetate,k 2 = (4.52 ± 0.62) × 10-12exp[(809 ± 39)/T]. At 298 K, the rate coefficients obtained (inunits of 10-12 cm3 molecule-1 s-1)are: k 1 = (27.1 ± 3.0) and k 2= (69.6± 9.4). The relative rate technique has been usedto determine rate coefficients for the reaction ofozone with the acetates. Using methyl vinyl ketone asthe reference compound and a value of4.8 × 10-18 cm3 molecule-1s-1 asthe rate coefficient for its reaction with O3,the following rate coefficients were derived at 298 ± 4 K (in units of10-18 cm3molecule-1 s-1): allyl acetate, (2.4 ± 0.7) andisopropenyl acetate (0.7 ± 0.2). Theresults are discussed in terms of structure-activityrelationships and used to derive atmospheric lifetimesfor the acetates.  相似文献   

16.
Data concerning carbon cycle variations on the earth's surface during the past 200,000 years are reviewed.The variations of the surface temperature (T) and concentration of carbon dioxide (CO2) in the atmosphere of Antarctica are compared to those of the isotopic ratios of oxygen 18O/16O (δ18O) and of carbon 13C/12C (°13C) of waters in the deep oceans for the two last glacial cycles. This comparison shows that the decrease of the atmospheric CO2 concentration is accompanied by a carbon transferase from the continental biosphere to the oceanic deep waters. At the glacial maximum this transfer is estimated to be about 500 GtC (1 GtC = 1015g of carbon) equivalent to 25% of the carbon storage of the biosphere. It occurs mainly in the high latitudes of the Southern Hemisphere by incorporation of CO2 into particulate matter during photosynthesis. It is shown that the mean oceanic productivity does not increase with a supplementary supply of ions such as phosphate (PO43−) or nitrate (NO3−) but that the intensity of the thermohaline circulation is certainly reduced. As the warming up of the oceans and the melting of the ice-sheet begin carbon transfer takes place to restore the continental biosphere.Another carbon transfer of a much more important intensity is also at work in the sea shore environment. Its intensity could be sufficient to renew the entire carbon of the continental biospheric, atmospheric and oceanic reservoirs in a length of time comparable to a glacial cycle. This fact shows the importance of studying the deposition of carbon in oceanic zones which are uncovered with drops in sea level. At the present time data on the coastal environment in relation to the global carbon cycle are very scarce and warrants more research in this area.  相似文献   

17.
Nearly all scenarios for future U.S. energy supply systems show heavy dependence on coal. The magnitude depends on assumptions as to reliance on nuclear fission, degree of electrification, and rate of GNP growth, and ranges from 700 million tons to 2300 million tons per year. However, potential climate change resulting from increasing atmospheric carbon dioxide concentrations may prevent coal from playing a major role. The carbon in the carbon dioxide produced from fossil fuels each year is about 1/10 the net primary production by terrestrial plants, but the fossil fuel production has been growing exponentially at 4.3% per year. Observed atmospheric CO2 concentrations have increased from 315 ppm in 1958 to 330 ppm in 1974 - in 1900, before much fossil fuel was burned, it was about 290–295 ppm. Slightly over one-half the CO2 released from fossil fuels is accounted for by the increase observed in the atmosphere; at present growth rates the quantities are doubling every 15–18 years. Atmospheric models suggest a global warming of about 2 K if the concentration were to rise to two times its pre-1900 value - enough to change the global climate in major (but largely unknown) ways. With the current rate of increase in fossil fuel use, the atmospheric concentration should reach these levels by about 2030. A shift to coal as a replacement for oil and gas gives more carbon dioxide per unit of energy; thus if energy growth continues with a concurrent shift toward coal, high concentrations can be reached somewhat earlier. Even projections with very heavy reliance on non-fossil energy (Neihaus) after 2000 show atmospheric carbon dioxide concentrations reaching 475 ppm.First presented to the symposium, Coal Science and our National Expectations, Annual Meeting of the American Association for the Advancement of Science, Boston, Massachusetts, February 20, 1976.  相似文献   

18.
Atmospheric response to deep-sea injections of fossil-fuel carbon dioxide   总被引：1，自引：0，他引：1  
The possibility of controlling atmospheric carbon dioxide accumulation and attendant climatic effects from fossil-fuel burning by diverting a fraction of the combustion product and injecting it into the deep-ocean, as proposed by Marchetti, is analyzed using an atmosphere/mixed layer/diffusive deep-ocean model for the carbon cycle. The model includes the nonlinear buffering of CO2 at the air/sea interface, and considers the long term trends associated with consuming an assumed fossil-fuel reserve equivalent to 7.09 × 1015 kg carbon as a logistic function of time as in the projections of Siegenthaler and Oeschger, except that atmospheric carbon dioxide levels are computed for five alternate strategies: (a) 100% injected into atmosphere, (b) 50% injected at oceanic depth of 1500 m and 50% into atmosphere, (c) 50% injected at sea floor (4000 m) and 50% into atmosphere, (d) 100% at 1500 m depth and (e) 100% at sea floor. Since no carbon leaves the system, all runs approached the same post-fossil fuel equilibrium after several thousand years, C a - 1150 ppm, almost four times the pre-fossil fuel value (- 300 ppm). But the transient response of these cases showed a marked variation ranging from a peak overshoot value of 2800 ppm in the year 2130 for 100% atmospheric injection to a slight decrease to the pre-fossil fuel 300 ppm lasting till 2300 with a subsequent slow approach to equilibrium for the 100% deep-ocean injection. The implications of these results for an oceanic injection strategy to mitigate the climatic impact of fossil-fuel CO2 is discussed, as are the ingredients of a second generation carbon cycle model for carrying out such forecasts on an engineering design basis.  相似文献   

19.
The kinetics of the reaction of nitrous acid (HONO) with nitric acid (HNO3), nitrate radicals (NO3) and dinitrogen pentoxide (N2O5) have been studied using Fourier transform infrared spectroscopy. Experiments were performed at 700 torr total pressure using synthetic air or argon as diluents. From the observed decay of HONO in the presence of HNO3 a rate constant of k<7×10-19 cm3 molecule-1 s-1 was derived for the reaction of HONO with HNO3. From the observed decay of HONO in the presence of mixtures of N2O5 and NO2 we have also derived upper limits for the rate constants of the reactions of HONO with NO3 and N2O5 of 2×10-15 and 7×10-19 cm3 molecule-1 s-1, respectively. These results are discussed with respect to previous studies and to the atmospheric chemistry of HONO.  相似文献   

20.
This paper deals with direct calculations of the radiation-equilibrium temperature profile in the Earth’s atmosphere from experimental spectroscopic data. The calculations are made for its present composition and for the modified ones, when concentration of a gas, namely, one of carbon dioxide CO2, methane CH4, nitrous oxide N2O or water vapor H2O is changed. Calculations were carried out with one-dimensional (horizontally homogeneous) radiation model proceeding from the values of absorption coefficients of atmospheric layers estimated from actual data. Calculations are carried out for small disturbances of the said gases’concentrations. Approximate estimates of large disturbance were made for the cases of total withdrawal of concrete gas from the atmosphere or, on the contrary, of large increase in its concentration.  相似文献   

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