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1.
Measurements of  Δ14C  in atmospheric CO2 are an effective method of separating CO2 additions from fossil fuel and biospheric sources or sinks of CO2. We illustrate this technique with vertical profiles of CO2 and  Δ14C  analysed in whole air flask samples collected above Colorado, USA in May and July 2004. Comparison of lower tropospheric composition to cleaner air at higher altitudes (>5 km) revealed considerable additions from respiration in the morning in both urban and rural locations. Afternoon concentrations were mainly governed by fossil fuel emissions and boundary layer depth, also showing net biospheric CO2 uptake in some cases. We estimate local industrial CO2:CO emission ratios using in situ measurements of CO concentration. Ratios are found to vary by 100% and average 57 mole CO2:1 mole CO, higher than expected from emissions inventories. Uncertainty in CO2 from different sources was ±1.1 to ±4.1 ppm for addition or uptake of −4.6 to 55.8 ppm, limited by  Δ14C  measurement precision and uncertainty in background  Δ14C  and CO2 levels.  相似文献   

2.
Two airborne campaigns were carried out to measure the tropospheric concentrations and variability of CO2, CO and O3 over Siberia. In order to quantify the influence of remote and regional natural and anthropogenic sources, we analysed a total of 52 vertical profiles of these species collected in April and September 2006, every ∼200 km and up to 7 km altitude. CO2 and CO concentrations were high in April 2006 (respectively 385–390 ppm CO2 and 160–200 ppb CO) compared to background values. CO concentrations up to 220 ppb were recorded above 3.5 km over eastern Siberia, with enhancements in 500–1000 m thick layers. The presence of CO enriched air masses resulted from a quick frontal uplift of a polluted air mass exposed to northern China anthropogenic emissions and to fire emissions in northern Mongolia. A dominant Asian origin for CO above 4 km (71.0%) contrasted with a dominant European origin below this altitude (70.9%) was deduced both from a transport model analysis, and from the contrasted ΔCO/ΔCO2 ratio vertical distribution. In September 2006, a significant O3 depletion (∼–30 ppb) was repeatedly observed in the boundary layer, as diagnosed from virtual potential temperature profiles and CO2 gradients, compared to the free troposphere aloft, suggestive of a strong O3 deposition over Siberian forests.  相似文献   

3.
Diurnal variation in the atmospheric CO2 concentration and the carbon isotopic composition (Δ14C and δ13C) was measured in a forest in an urban area on 9 February 1999. The carbon isotope approach used in the present study differentiated between the quantitative contributions from anthropogenic and biogenic CO2 sources in the urban atmosphere. The anthropogenic (fossil fuel) and biogenic (soil respiration) contributions was estimated, and they ranged from 1 to 16% and from 2 to 8% of the total atmospheric CO2. The diurnal variation of the anthropogenic CO2 was the major cause of the total atmospheric CO2 variation, while the biogenic CO2 remained relatively constant throughout the day. Estimating the contribution of soil respired CO2 provided the mean residence time of soil respired CO2 within the forest atmosphere.  相似文献   

4.
Climate effects on atmospheric carbon dioxide over the last century   总被引:1,自引:0,他引:1  
The buildup of atmospheric CO2 since 1958 is surprisingly well explained by the simple premise that 57% of the industrial emissions (fossil fuel burning and cement manufacture) has remained airborne. This premise accounts well for the rise both before and after 1980 despite a decrease in the growth rate of fossil fuel CO2 emissions, which occurred at that time, and by itself should have caused the airborne fraction to decrease. In contrast, the buildup prior to 1958 was not simply proportional to cumulative fossil fuel emissions, and notably included a period during the 1940s when CO2 growth stalled despite continued fossil fuel emissions. Here we show that the constancy of the airborne fraction since 1958 can be in part explained by decadal variations in global land air temperature, which caused a warming-induced release of CO2 from the land biosphere to the atmosphere. We also show that the 1940s plateau may be related to these decadal temperature variations. Furthermore, we show that there is a close connection between the phenomenology producing CO2 variability on multidecadal and El Niño timescales.  相似文献   

5.
In this issue, Ramonet et al. revealed a positive trend in European, atmospheric CO2 concentrations relative to a marine, North Atlantic reference baseline, for the years 2001–2006. The observed build up mainly occurred during the cold season where it reaches a 0.8 ppm yr−1 at low-altitude stations to a 0.3 ppm yr−1 at mid-altitude stations. We explore the cause of this build-up using the mesoscale model CHIMERE. We first model the observed trends, using interannually varying fluxes and transport, then suppress the interannual variability in fluxes or aspects of transport to elucidate the cause. The run with no interannual variability in fluxes still matches observed trends suggesting that transport is the major cause. Separate runs varying either boundary layer height or winds show that changes in boundary layer height explain the trends at low-altitude stations within the continents while changes in wind regimes drive changes elsewhere.  相似文献   

6.
Long‐range transport of anthropogenic and biogenic CO2 to a remote site in the Arctic is studied. A limited area, off‐line, Eulerian atmospheric transport model is used, and the results are compared to the observed CO2 concentration at the "Ny‐Alesund International Arctic Research and Monitoring Facility". Inventories of anthropogenic CO2 emissions and estimates of biogenic CO2 emissions are used to investigate the respective impact of these emissions on Arctic CO2 variations during 4 winter months. A direct comparison of the modelled and observed concentrations reveals remarkably good timing in the modelled variations as compared to the observed variations for most of the time. The correlation of observed versus modelled CO2 concentration is significant at the 95% confidence level. The biogenic and the anthropogenic CO2 emissions are shown to have approximately equal influence on Arctic CO2 variations during winter. Europe is found to be the dominant source of anthropogenic CO2 at the monitoring station, while Siberia and Northern America have little influence on Arctic CO2, during the months studied. These results contradict Engardt and Holmén whose results indicate that the lower‐Ob region in western Siberia has a large impact on Arctic CO2.  相似文献   

7.
The impact of land use on the global carbon cycle and climate is assessed. The Bern carbon cycle-climate model was used with land use maps from HYDE3.0 for 1700 to 2000 A.D. and from post-SRES scenarios for this century. Cropland and pasture expansion each cause about half of the simulated net carbon emissions of 188 Gt C over the industrial period and 1.1 Gt C yr−1 in the 1990s, implying a residual terrestrial sink of 113 Gt C and of 1.8 Gt C yr−1, respectively. Direct CO2 emissions due to land conversion as simulated in book-keeping models dominate carbon fluxes due to land use in the past. They are, however, mitigated by 25% through the feedback of increased atmospheric CO2 stimulating uptake. CO2 stimulated sinks are largely lost when natural lands are converted. Past land use change has eliminated potential future carbon sinks equivalent to emissions of 80–150 Gt C over this century. They represent a commitment of past land use change, which accounts for 70% of the future land use flux in the scenarios considered. Pre-industrial land use emissions are estimated to 45 Gt C at most, implying a maximum change in Holocene atmospheric CO2 of 3 ppm. This is not compatible with the hypothesis that early anthropogenic CO2 emissions prevented a new glacial period.  相似文献   

8.
The amounts of microbial and root‐respired CO2 in a maize/winter wheat agricultural system in south western Germany were investigated by measurements of the CO2 mixing ratio and the 13C/12C ratio in soil air. CO2 fluxes at the soil surface for the period of investigation (1993–1995) were also determined. Root respired CO2 shows a strong correlation with the plant mass above ground surface of the respective vegetation (R2≥0.88); the maximum CO2 release from roots was in August for the maize (2.0±0.5 mmol m−2 h−1) and in June for winter wheat (1.5±0.5 mmol m−2 h−1). Maximum CO2 production by roots correlate well with the maximum amount of plant root matter. Integrating the CO2 production over the whole growing season and normalizing to the dry root matter yields, the CO2 production per gram dry organic root matter (DORM) of maize was found to be 0.14±0.03 gC (g DORM)−1. At the sites investigated, root‐produced CO2 contributed (16±4)% for maize, and (24±4)% for winter wheat, respectively, to the total annual CO2 production in the soil (450±50 gC m−2 for maize, 210±30 gC m−2 for winter wheat).  相似文献   

9.
Global warming simulations are performed with a coupled climate model of reduced complexity to investigate global warming–marine carbon cycle feedbacks. The model is forced by emissions of CO2 and other greenhouse agents from scenarios recently developed by the Intergovernmental Panel on Climate Change and by CO2 stabilization profiles. The uptake of atmospheric CO2 by the ocean is reduced between 7 to 10% by year 2100 compared to simulations without global warming. The reduction is of similar size in the Southern Ocean and in low‐latitude regions (32.5°S‐32.5°N) until 2100, whereas low‐latitude regions dominate on longer time scales. In the North Atlantic the CO2 uptake is enhanced, unless the Atlantic thermohaline circulation completely collapses. At high latitudes, biologically mediated changes enhance ocean CO2 uptake, whereas in low‐latitude regions the situation is reversed. Different implementations of the marine biosphere yield a range of 5 to 16% for the total reduction in oceanic CO2 uptake until year 2100. Modeled oceanic O2 inventories are significantly reduced in global warming simulations. This suggests that the terrestrial carbon sink deduced from atmospheric O2/N2 observations is potentially overestimated if the oceanic loss of O2 to the atmosphere is not considered.  相似文献   

10.
This paper uses a refined soil gradient method to estimate soil CO2 efflux. Six different models are used to determine the relative gas diffusion coefficient (ξ). A weighted harmonic averaging is used to estimate the soil CO2 diffusion coefficient, yielding a better estimate of soil CO2 efflux. The resulting soil CO2 efflux results are then compared to the soil CO2 efflux measured with a soil chamber. Depending on the choice of ξ model used, the estimated soil CO2 efflux using the gradient method reasonably approximates the efflux obtained using the soil chamber method. In addition, the estimated soil CO2 efflux obtained by this improved method is well described by an exponential function of soil temperature at a depth of 0.05 m with the temperature sensitivity ( Q 10) of 1.81 and a linear function of soil moisture at a depth of 0.12 m, in general agreement with previous findings. These results suggest that the gradient method is a practical cost-effective means to measure soil CO2 emissions. Results from the present study suggest that the gradient method can be used successfully to measure soil CO2 efflux provided that proper attention is paid to the judicious use of the proper diffusion coefficient.  相似文献   

11.
Abstract The spatial and temporal variations of atmospheric CO2 at 8–13 km from April 1993 to April 1999 were observed by measuring CO2 mixing ratios in samples collected biweekly from a commercial airliner between Australia and Japan. The CO2 growth rate showed a considerable interannual variation, with a maximum of about 3 ppm yr−1 during late 1997. This variation is related to the El Niño/Southern Oscillation (ENSO) events. A year-to-year change related to the ENSO events was also found in the latitudinal distribution pattern of the CO2 annual mean between 30°N and 30°S. The averaged CO2 seasonal cycle in the Northern Hemisphere gradually decayed toward the equator, and a relatively complicated variation with a double seasonal maximum appeared in the Southern Hemisphere. A significant yearly change of the seasonal cycle pattern was observed in the Southern Hemisphere. The impact of a tropical biomass-burning injection on the upper tropospheric CO2 was estimated on the basis of the CO data from the same airliner observation.  相似文献   

12.
The net flux of carbon dioxide (CO2) from the land surface into the atmospheric boundary layer has a diurnal cycle. Drawdown of CO2 occurs during daytime photosynthesis, and return of CO2 to the atmosphere occurs during night. Even when the net diurnal-average surface flux vanishes, the diurnal-average profile of atmospheric CO2 mixing ratio is usually not vertically uniform. This is because of the diurnal rectifier effect, by which atmospheric vertical transport and the surface flux conspire to produce a surplus of CO2 near the ground and a deficit aloft.
This paper constructs an idealized, 1-D, eddy-diffusivity model of the rectifier effect and provides an analytic series solution. When non-dimensionalized, the intensity of the rectifier effect is related solely to a single 'rectifier parameter'. Given this model's governing equation and boundary conditions, we prove that the existence of the rectifier effect is related to the correlation of CO2 gradient and transport, and also to the day–night symmetry of transport.
The rectifier-induced near-surface CO2 surplus ought to be included in inverse calculations that use near-surface CO2 mixing ratio to infer land–surface sources and sinks of carbon. Such inverse modeling is facilitated by our model's simplicity. To illustrate, we use a 1-D inverse calculation to infer the amplitude of diurnal CO2 surface flux.  相似文献   

13.
Ambient CO2 concentration, air temperature and relative humidity were measured intermittently for a 3-year period from the floor to the canopy top of a tropical rainforest in Pasoh, Peninsular Malaysia. Mean diurnal CO2 storage flux ( S c; μmol m−2 s−1) and sensible and latent heat storage fluxes ( Q a and Q w; W m−2) ranged from −12.7 to 3.2 μmol m−2 s−1, −15 to 27 W m−2 and −10 to 20 W m−2, respectively. Small differences in diurnal changes were observed in S c and Q a between the driest and wettest periods. Compared with the ranges of mean diurnal CO2 eddy flux (−14.7 to 4.9 μmol m−2 s−1), sensible eddy flux (−12 to 169 W m−2) and latent eddy flux (0 to 250 W m−2), the contribution of CO2 storage flux was especially large. Comparison with summertime data from a temperate Japanese cypress forest suggested a higher contribution of S c in the tropical rainforest, probably mainly due to the difference in nighttime friction velocity at the sites. On the other hand, differences in Q a and Q w were smaller than the difference in S c, probably because of the smaller nighttime sinks/sources of heat and water vapour.  相似文献   

14.
We studied the commencement and finishing of the growing season using different air temperature indices, the surface albedo, the chlorophyll fluorescence (Fv/Fm) and the carbon dioxide (CO2) tropospheric concentration, together with eddy covariance measurements of CO2 flux. We used CO2 flux data from four boreal coniferous forest sites covering a wide latitudinal range, and CO2 concentration measurements from Sammaltunturi in Pallas. The CO2 gas exchange was taken as the primary determinant for the growing season to which other methods were compared.
Indices based on the cumulative temperature sum and the variation in daily mean temperature were successfully used for approximating the start and cessation of the growing season. The beginning of snow melt was a successful predictor of the onset of the growing season. The chlorophyll fluorescence parameter Fv/Fm and the CO2 concentration were good indicators of both the commencement and cessation of the growing season. By a derivative estimation method for the CO2 concentration, we were also able to capture the larger-scale spring recovery. The trends of the CO2 concentration and temperature indices at Pallas/Sammaltunturi were studied over an 11-yr time period, and a significant tendency towards an earlier spring was observed. This tendency was not observed at the other sites.  相似文献   

15.
Oceanic excess radiocarbon data is widely used as a constraint for air–sea gas exchange. However, recent estimates of the global mean piston velocity  〈 k 〉  from Naegler et al., Krakauer et al., Sweeney et al. and Müller et al. differ substantially despite the fact that they all are based on excess radiocarbon data from the GLODAP data base. Here I show that these estimates of  〈 k 〉  can be reconciled if first, the changing oceanic radiocarbon inventory due to net uptake of CO2 is taken into account; second, if realistic reconstructions of sea surface  Δ14C  are used and third, if  〈 k 〉  is consistently reported with or without normalization to a Schmidt number of 660. These corrections applied, unnormalized estimates of  〈 k 〉  from these studies range between 15.1 and 18.2 cm h−1. However, none of these estimates can be regarded as the only correct value for  〈 k 〉  . I thus propose to use the 'average' of the corrected values of  〈 k 〉  presented here (16.5 ± 3.2 cm h−1) as the best available estimate of the global mean unnormalized piston velocity  〈 k 〉  , resulting in a gross ocean-to-atmosphere CO2 flux of 76 ± 15 PgC yr−1 for the mid-1990s.  相似文献   

16.
Diurnal and annual variations of CO2, O3, SO2, black carbon and condensation nuclei and their source areas were studied by utilizing air parcel trajectories and tropospheric concentration measurements at a boreal GAW site in Pallas, Finland. The average growth trend of CO2 was about 2.5 ppm yr−1 according to a 4-yr measurement period starting in October 1996. The annual cycle of CO2 showed concentration difference of about 19 ppm between the summer minimum and winter maximum. The diurnal cycle was most pronounced during July and August. The variation between daily minimum and maximum was about 5 ppm. There was a diurnal cycle in aerosol concentrations during spring and summer. Diurnal variation in ozone concentrations was weak. According to trajectory analysis the site was equally affected by continental and marine air masses. During summer the contribution of continental air increased, although the southernmost influences decreased. During daytime in summer the source areas of CO2 were mainly located in the northern parts of the Central Europe, while during winter the sources were more evenly distributed. Ozone showed similar source areas during summer, while during winter, unlike CO2, high concentrations were observed in air arriving from the sea. Sulfur dioxide sources were more northern (Kola peninsula and further east) and CO2 sources west-weighted in comparison to sources of black carbon. Source areas of black carbon were similar to source areas of aerosols during winter. Aerosol source area distributions showed signs of marine sources during spring and summer.  相似文献   

17.
The hydrogen-to-carbon monoxide (H2/CO) emission ratio of anthropogenic combustion sources was determined from more than two years of quasi-continuous atmospheric observations in Heidelberg (49°24' N, 8°42' E), located in the polluted Rhein-Neckar region. Evaluating concurrent mixing ratio changes of H2 and CO during morning rush hours yielded mean molar H2/CO ratios of 0.40 ± 0.06, while respective results inferred from synoptic pollution events gave a mean value of 0.31 ± 0.05 mole H2/mole CO. After correction for the influence of the H2 soil sink on the measured ratios, mean values of 0.46 ± 0.07 resp. 0.48 ± 0.07 mole H2/mole CO were obtained, which are in excellent agreement with direct source studies of traffic emissions in the Heidelberg/Mannheim region (0.448 ± 0.003 mole H2/mole CO). Including results from other European studies, our best estimate of the mean H2/CO emission ratio from anthropogenic combustion sources (mainly traffic) ranges from 0.45 to 0.48 mole H2/mole CO, which is about 20% smaller than the value of 0.59 mole H2/mole CO which is frequently used as the basis to calculate global H2 emissions from anthropogenic combustion sources.  相似文献   

18.
19.
The seasonal cycle of atmospheric CO2 at surface observation stations in the northern hemisphere is driven primarily by net ecosystem production (NEP) fluxes from terrestrial ecosystems. In addition to NEP from terrestrial ecosystems, surface fluxes from fossil fuel combustion and ocean exchange also contribute to the seasonal cycle of atmospheric CO2. Here the authors use the Goddard Earth Observing System-Chemistry (GEOS-Chem) model (version 8-02-01), with modifications, to assess the impact of these fluxes on the seasonal cycle of atmospheric CO2 in 2005. Modifications include monthly fossil and ocean emission inventories. CO2 simulations with monthly varying and annual emission inventories were carried out separately. The sources and sinks of monthly averaged net surface flux are different from those of annual emission inventories for every month. Results indicate that changes in monthly averaged net surface flux have a greater impact on the average concentration of atmospheric CO2 in the northern hemisphere than on the average concentration for latitudes 30-90°S in July. The concentration values differ little between both emission inventories over the latitudinal range from the equator to 30°S in January and July. The accumulated impacts of the monthly averaged fossil and ocean emissions contribute to an increase of the total global monthly average of CO2 from May to December.An apparent discrepancy for global average CO2 concentration between model results and observation was because the observation stations were not sufficiently representative. More accurate values for monthly varying net surface flux will be necessary in future to run the CO2 simulation.  相似文献   

20.
We performed model studies on how anthropogenic emission changes in Southeast Asia (region between 60–150°E and 10°S–50°N) in the period 1980–2020 could contribute to changes in hydroxyl and methane lifetime on a global scale. From 1980 to 2000, we calculate small global OH and methane lifetime changes due to compensating effects by emission changes in Southeast Asia and emission changes in the rest of the world. There is no guarantee that this offset will persist in the future. Southeast Asia is going through rapid economic development and emission increases there may be a major driver for changes. The development of Asian emissions after year 2000 is under much debate and for this period we apply several emission scenarios. For most emission scenarios the simulated Southeast Asian induced changes in global hydroxyl and methane lifetime after year 2000 are moderate. However, an upper estimate assuming very high increases in NO x emissions results in substantial increases of hydroxyl and corresponding reductions in global methane lifetime. Interestingly, for the high NO x emission case our results fit very well with recent satellite observations on trends of NO2 over central eastern China.  相似文献   

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