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1.
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   

2.
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   

3.
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   

4.
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   

5.
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   

6.
We analysed interannual and decadal changes in the atmospheric CO2 concentration gradient (ΔCO2) between Europe and the Atlantic Ocean over the period 1995–2007. Fourteen measurement stations are used, with Mace-Head being used to define background conditions. The variability of ΔCO2 reflects fossil fuel emissions and natural sinks activity over Europe, as well as atmospheric transport variability. The mean ΔCO2 increased by 1–2 ppm at Eastern European stations (∼30% growth), between 1990–1995 and 2000–2005. This built up of CO2 over the continent is predominantly a winter signal. If the observed increase of ΔCO2 is explained by changes in ecosystem fluxes, a loss of about 0.46 Pg C per year would be required during 2000–2005. Even if severe droughts have impacted Western Europe in 2003 and 2005, a sustained CO2 loss of that magnitude is unlikely to be true. We sought alternative explanations for the observed CO2 build-up into transport changes and into regional redistribution of fossil fuel CO2 emissions. Boundary layer heights becoming shallower can only explain 32% of the variance of the signal. Regional changes of emissions may explain up to 27% of the build-up. More insights are given in the Aulagnier et al. companion paper.  相似文献   

7.
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   

8.
Many researchers have reported the widespread occurrence of excess 210 Po in the global atmosphere and suggested probable sources such as resuspension of top soils, stratospheric aerosols, sea spray of the surface micro‐layer, volcanic emission, and bio‐volatile 210Po species from the productive ocean. We have observed excess 210Po on aerosols in the coastal atmosphere of the Chesapeake and Delaware Bays. On‐board measurements in the Chesapeake Bay atmosphere show that the increase of this excess 210Po is dependent upon wind speed. Simultaneously measured activity ratios of 7Be/210Pb and 210Pb/222Rn argue against either higher altitude air or continental soils as the source of this excess. We hypothesize that the excess 210Po originates mainly from surface waters either by the sea‐spray of the surface microlayer, or more likely, by gas exchange. We conclude gas exchange as the mechanism since the polonium excess increases linearly with wind speed over a threshold of 3 m s−1(mean) similar to other gases (i.e., CO2, SF6 , and DMS). In addition, higher 210Po excess with lower 222Rn is observed in on‐shore marine air at Lewes, DE. This suggests sea‐air exchange of volatile Po along with other bio‐volatile species (i.e., DMS, DMSe, and MMHg) in the coastal productive ocean during high wind speeds.  相似文献   

9.
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   

10.
Samples of a core (52 m) of ablating Antarctic ice were analysed for 14CO and 14CO2 by accelerator mass spectrometry. The data were compared with a 14C in situ production model that includes muon capture in addition to oxygen spallation by neutrons. The analysis reveals significant in situ 14C at depths below 10 m, which we attribute to 14C production by cosmic ray muons. The age of the ice was determined as 9.3±0.4 14C ka BP.  相似文献   

11.
The Optical Transient Detector (OTD) lightning data for the 12‐month period of 1996 are used to estimate the seasonal and global distributions of lightning‐produced NO x . The relatively small viewing footprint and the low detection efficiency of the OTD sensor and other difficulties require extrapolations of the OTD data to the actual global flash distributions. Furthermore, available measurements for the ratios of intracloud (IC) to cloud‐to‐ground (CG) flashes have been used to partition lightning counts for IC versus CG flashes from the OTD observations. The resulting lightning distributions are then used to calculate the global and seasonal production of NO x , assuming a NO production rate of 6.2×1025 molecules for each CG flash and 8.7×1024 molecules for each IC flash. Consequently, we find that CG flashes produce more NO x than IC flashes despite fewer CG flashes by a factor of 3 or more. NO x production by lightning varies seasonally in accordance with the global lightning distribution, with the maximum production occurring in the Northern Hemisphere in the local summer. The latitudinal distribution of NO x production exhibits a strong seasonal variation outside the tropics with the production occurring mainly in the summer hemisphere, whereas in the tropics the production is high throughout the year. The annual contribution to NO x production by lightning is higher in the Northern Hemisphere than that in the Southern Hemisphere.  相似文献   

12.
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   

13.
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   

14.
The dominant sink of atmospheric molecular hydrogen (H2) is its enzymatic destruction in soils. Quantitative estimates of the global sink strength, as derived from bottom-up process studies, are, however, still associated to large uncertainties. Here we present an alternative way to estimate atmosphere-to-soil flux densities, respectively deposition velocities of H2, based on atmospheric H2 and 222Rn observations in the boundary layer. Two and a half years of continuous measurements from a polluted site in the Rhine-Neckar area have been evaluated and night-time flux densities were calculated for situations of strong nocturnal boundary layer inversions using the Radon-Tracer Method. The influences from local anthropogenic combustion sources could be detected and successfully separated by parallel measurements of carbon monoxide. Inferred daily uptake fluxes in the Heidelberg catchment area range from 0.5 to 3 × 10−8 g H2 m−2 s−1 with a mean value of (1.28 ± 0.31) × 10−8 g H2 m−2 s−1. Uptake rates are about 25% larger during summer than during winter, when soil moisture is high, and diffusive transport of H2 into the soil is inhibited. The mean deposition velocity is 3.0 ± 0.7 × 10−2 cm s−1, which is very well in line with direct measurements on similar soil types in Europe and elsewhere.  相似文献   

15.
CO and H2 uptake by soil was studied as a diffusion process. A diffusion model was used to determine how the surface fluxes (net deposition velocities) were controlled by in‐situ microbial uptake rates and soil gas diffusivity calculated from the 3‐phase system (solid, liquid, gas) in the soil. Analytical solutions of the diffusion model assuming vertical uniformity of soil properties showed that physical properties such as air‐filled porosity and soil gas diffusivity were more important in the uptake process than in the emission process. To incorporate the distribution of in‐situ microbial uptake, we used a 2‐layer model incorporating "a microbiologically inactive layer and an active layer" as suggested from experimental results. By numerical simulation using the 2‐layer model, we estimated the effect of several factors on deposition velocities. The variations in soil gas diffusivity due to physical properties, i.e., soil moisture and air‐filled porosity, as well as to the depth of the inactive layer and in‐situ microbial uptake, were found to be important in controlling deposition velocities. This result shows that the diffusion process in soil is critically important for CO and H2 uptake by soil, at least in soils with higher in‐situ uptake rates and/or with large variation in soil moisture. Similar uptake rates and the difference in deposition velocity between CO and H2 may be attributable to differences in CO and H2 molecular diffusivity. The inactive layer is resistant to diffusion and creates uptake limits in CO and H2 by soil. The coupling of high temperature and a thick inactive layer, common in arid soils, markedly lowers net CO deposition velocity. The temperature for maximum uptake of CO changes with depth of the inactive layer.  相似文献   

16.
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   

17.
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   

18.
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   

19.
The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO2 concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO2 to sulphate aerosol. The modelled SO2 concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH3 and HCl gas were also found to play an important rôle in cloud processing in the model.  相似文献   

20.
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   

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