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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.
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   

3.
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   

4.
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   

5.
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   

6.
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   

7.
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   

8.
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   

9.
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   

10.
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   

11.
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   

12.
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13.
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   

14.
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   

15.
Estimates of Asian emissions of air pollutants and carbonaceous aerosols and their mid-term projections have been changing significantly in the last years. The remote sensing community has shown that increase in NO x in Central East Asia is much stronger than any of the emission inventories or projections indicated so far. A number of studies reviewing older estimates appeared. Here, we review the key contributions and compare them to the most recent results of the GAINS model application for Asia and to the SRES projections used in the IPPC work. The recent projections indicate that the growth of emissions of SO2 in Asia should slow down significantly towards 2010 or even stabilize at the current level. For NO x , however, further growth is projected although it will be most likely slower that in the last decade, owing to introduction of measures in transport. Emissions of carbonaceous aerosols (black carbon and organic carbon) are expected to decline after 2010, largely due to reduced use of biofuels in residential sector and efficiency improvements. The estimates of these emissions are burdened with significantly larger uncertainties than SO2 and NO x ; even for the year 2000 the differences in estimates between studies are up to a factor of 2.  相似文献   

16.
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   

17.
Enclosure measurements have been performed on a bare mineral soil at an experimental field site near Heidelberg, Germany. From observed molecular hydrogen (H2) mixing ratio changes in the enclosure, deposition velocities were calculated ranging from  8.4 × 10−3  to  8.2 × 10−2 cm s−1  and with an annual mean value of  3.1 × 10−2 cm s−1  . In the studied range of  2– 27 °C  , the uptake showed a significant temperature dependence. However, this turned out not to be the primary driving mechanism of the uptake flux. Soil moisture content, co-varying with temperature, was identified as the major parameter being responsible for the diffusive permeability of H2 in the soil and the final rate of H2 uptake. A simple Millington–Quirk diffusion model approach could largely explain this behaviour and yielded a diffusion path length of H2 in the studied soil of only 0.2–1.8 cm, suggesting that total H2 consumption occurs within the first few centimetres of the soil. The diffusion model, when applied to continuous measurements of soil moisture content, atmospheric pressure, temperature and the mixing ratio of H2 in the atmosphere, could largely reproduce the measured deposition flux densities, assuming a mean thickness of the diffusion path length of 0.7 cm.  相似文献   

18.
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   

19.
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   

20.
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   

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