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1.
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   

2.
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   

3.
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   

4.
Latitudinal distribution of radon-222 flux from continents   总被引:1,自引:0,他引:1  
Global atmospheric transport models are frequently tested by using 222Rn as a tracer. Generally this tracer is assumed to be emitted at a uniform rate (1 atom cm−2 s−1) from all ice-free land surfaces. The analysis of published data suggests a strong decrease from 30°N northwards to 0.2 atom cm−2 s−1 at 70°N. This could be a result of increasing water tables and proportions of organic soils as indicated by larger proportions of wetlands in northern latitudes.  相似文献   

5.
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   

6.
An atmospheric transport model, NIRE-CTM-96, was evaluated by using measured radon-222 concentrations. The model has 2.5×2.5 degree horizontal resolution and 15 vertical levels. Assimilated global meteorological data for 1990–1996 from the European Centre for Medium Range Weather Forecasts were used to drive the model. We used an emanation rate of radon-222 of 1 atom cm−2 s−1 over mostly ice-free land. Simulated concentrations were compared with measured concentrations for 22 sites worldwide including 10 stations in China. Simulated annual mean concentrations for Freiburg, Germany, and Socorro, New Mexico, and for four stations in northern China were consistent with the measured concentrations. Simulated daily concentrations for Ogasawara-Hahajima, Japan, correlated well with the measured concentrations. Simulated upper tropospheric concentrations for Moffet Field, California, demonstrated the cross-Pacific transport from central Eurasia and India-Indochina area. Simulated concentrations for two stations in southern China were almost half of the measured concentrations. Mixing layer depth in the model was consistent with other estimates which indicates higher emanation rate there. Simulated concentrations for the South Indian Ocean and the Antarctic during summer were significantly lower than the measured concentrations; this difference was accounted for when emanation from the ocean at a rate of 0.01 atom cm−2 s−1 was included in the model. The model failed to simulate amplitudes of high-concentration events at Mauna Loa. These high-concentration events were possibly a result of filament-like horizontal structure or laminated vertical structure. The vertical as well as horizontal resolution of the model were supposed to be insufficient to reproduce these fine structures.  相似文献   

7.
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   

8.
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   

9.
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   

10.
During the Saharan Mineral Dust Experiment (SAMUM) conducted in summer 2006 in southeast Morocco, the complex refractive index of desert dust was determined from airborne measurements of particle size distributions and aerosol absorption coefficients at three different wavelengths in the blue (467 nm), green (530 nm) and red (660 nm) spectral regions. The vertical structure of the dust layers was analysed by an airborne high spectral resolution lidar (HSRL). The origin of the investigated dust layers was estimated from trajectory analyses, combined with Meteosat 2nd Generation (MSG) scenes and wind field data analyses. The real part n of the dust refractive index was found almost constant with values between 1.55 and 1.56, independent of the wavelength. The values of the imaginary part k varied between the blue and red spectral regions by a factor of three to ten depending on the dust source region. Absolute values of k ranged from 3.1 × 10−3 to 5.2 × 10−3 at 450 nm and from 0.3 × 10−3 to 2.5 × 10−3 at 700 nm. Groupings of k values could be attributed to different source regions.  相似文献   

11.
In situ measurements of optical and physical properties of mineral dust were performed at the outskirts of the Saharan Desert in the framework of the Saharan Mineral Dust Experiment part 1 (SAMUM-1). Goals of the field study were to achieve information on the extent and composition of the dust particle size distribution and the optical properties of dust at the ground. For the particle number size distribution, measured with a DMPS/APS, a size dependent dynamic shape factor was considered. The mean refractive index of the particles in this field study is  1.53–4.1 × 10−3 i   at 537 nm wavelength and  1.53–3.1 × 10−3 i   at 637 nm wavelength derived from measurements of scattering and absorption coefficients, as well as the particle size distribution. Whereas the real part of the refractive index is rather constant, the imaginary part varies depending on the mineral dust concentrations. For high dust concentration the single scattering albedo is primarily influenced by iron oxide and is  0.96 ± 0.02  and  0.98 ± 0.01  at 537 nm and 637 nm wavelength, respectively. During low dust concentration the single scattering albedo is more influenced by a soot-type absorber and is  0.89 ± 0.02  and  0.93 ± 0.01  for the same wavelengths.  相似文献   

12.
During the SAMUM-1 experiment, absorption coefficients and imaginary parts of refractive indices of mineral dust particles were investigated in southern Morocco. Main absorbing constituents of airborne samples were identified to be iron oxide and soot. Spectral absorption coefficients were measured using a spectral optical absorption photometer (SOAP) in the wavelength range from 300 to 800 nm with a resolution of 50 nm. A new method that accounts for a loading-dependent correction of fibre filter based absorption photometers, was developed. The imaginary part of the refractive index was determined using Mie calculations from 350 to 800 nm. The spectral absorption coefficient allowed a separation between dust and soot absorption. A correlation analysis showed that the dust absorption coefficient is correlated ( R 2 up to 0.55) with the particle number concentration for particle diameters larger than 0.5 μm, whereas the coefficient of determination R 2 for smaller particles is below 0.1. Refractive indices were derived for both the total aerosol and a dust aerosol that was corrected for soot absorption. Average imaginary parts of refractive indices of the entire aerosol are 7.4 × 10−3, 3.4 × 10−3 and 2.0 × 10−3 at wavelengths of 450, 550 and 650 nm. After a correction for the soot absorption, imaginary parts of refractive indices are 5.1 × 10−3, 1.6 × 10−3 and 4.5 × 10−4.  相似文献   

13.
Using 5 yr (December 2000–November 2005) of satellite data from the clouds and the earths radiant energy system (CERES) and moderate resolution imaging spectroradiometer (MODIS), we examine the instantaneous short-wave radiative efficiency ( Eτ ) of aerosols during the morning Terra satellite overpass time over the global oceans (60°N–60°S). We calculate Eτ using two commonly used methods. The first method uses the MODIS aerosol optical thickness (AOT) at 0.55 μm with radiative transfer calculations, whereas the second method utilizes the same AOT values along with a new generation of aerosol angular distribution models to convert the CERES-measured broad-band radiances to fluxes. Over the 5 yr, the global mean instantaneous Eτ between the methods is remarkably consistent and within 5 W m−2τ−1 with a mean value of –70 W m−2τ−1. The largest differences between the methods occur in high-latitude regions, primarily in the Southern Hemisphere, where AOT is low. In dust dominated regions, there is an excellent agreement between the methods with differences of <3 W m−2τ−1. These differences are largely due to assumptions in aerosol models and definition of clear sky backgrounds. Independent assessments of aerosol radiative effects from different satellite sensors and methods are extremely valuable and should be used to verify numerical modelling simulations.  相似文献   

14.
Terrestrial radon-222 flux density for the Asian continent, integrated over distances of 4500 km, is estimated in two 20° latitudinal bands centred on 48.8°N and 63.2°N. The evaluation is based on three years of wintertime radon measurements at Sado Island, Japan, together with meteorological and trajectory information. A selection of 18% of observations are suitable for evaluation of an analytical expression for the continental surface flux. Various meteorological assumptions are discussed; it is found that there is a substantial effect of increased complexity of the formulation on the flux estimates obtained. The distribution of spatially integrated radon flux over the Asian landmass is reported for the first time. Expressed as geometric means and 1σ-ranges, estimated fluxes are 14.1 mBq m−2 s−1 (1σ-range: 18 mBq m−2 s−1) and 8.4 mBq m−2 s−1 (1σ-range: 10 mBq m−2 s−1) for the lower and higher latitude bands. These results constitute an annual minimum in flux densities for these regions, and are higher than previously reported. The existence of a latitudinal gradient in the continental radon source function is confirmed; the present estimate for Asia (−0.39 mBq m−2 s−1 per degree of latitude) is in agreement with the northern hemisphere terrestrial radon flux gradient proposed previously.  相似文献   

15.
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   

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.
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   

18.
An aerosol dynamics model, AEROFOR2, is developed in the context of the BIOFOR project focussing on boreal forest aerosol. It is the second version of a Lagrangian type box model AEROFOR for investigating the formation and growth of particles under clear sky atmospheric conditions. Particles can consist of soluble and insoluble material and the particle population can be externally or internally mixed. AEROFOR2 includes gas phase chemistry and aerosol dynamics, and calculates the number and composition distributions of particles as functions of time. Observed growth rates of the nucleation mode particles after a typical nucleation event are 2–3 nm/h. The model simulations predict that 3·107 molecules cm−3 of insoluble organic vapour and less than 6·106 molecules cm−3 of soluble vapour condensing onto particles are enough to make them grow in good agreement with the observed growth rates. Then the source rate of the organic vapour must be an order of 105 molecules cm−3 s−1, and its saturation vapour density should be below 106 molecules cm−3. If the aerosol was initially an internal mixture of soluble (70%) and insoluble (30%) constituents it transformed to an externally mixed aerosol during the simulation. By applying the externally‐mixed aerosol based on measured soluble volume fractions, it was concluded that the modelled soluble fraction of the nucleation mode was too low in comparison with the measurements, and thus, a part of the condensable organic vapour must be water soluble.  相似文献   

19.
Potential impact of climate change on marine dimethyl sulfide emissions   总被引:1,自引:0,他引:1  
Dimethyl sulfide (DMS) is a biogenic compound produced in sea-surface water and outgased to the atmosphere. Once in the atmosphere, DMS is a significant source of cloud condensation nuclei in the unpolluted marine atmosphere. It has been postulated that climate may be partly modulated by variations in DMS production through a DMS-cloud condensation nuclei-albedo feedback. We present here a modelled estimation of the response of DMS sea-water concentrations and DMS fluxes to climate change, following previous work on marine DMS modeling ( Aumont et al., 2002 ) and on the global warming impact on marine biology ( Bopp et al., 2001 ). An atmosphere–ocean general circulation model (GCM) was coupled to a marine biogeochemical scheme and used without flux correction to simulate climate response to increased greenhouse gases (a 1% increase per year in atmospheric CO2 until it has doubled). The predicted global distribution of DMS at  1 × CO2  compares reasonably well with observations; however, in the high latitudes, very elevated concentrations of DMS due to spring and summer blooms of Phaeocystis can not be reproduced. At  2 × CO2  , the model estimates a small increase of global DMS flux to the atmosphere (+2%) but with large spatial heterogeneities (from −15% to +30% for the zonal mean). Mechanisms affecting DMS fluxes are changes in (1) marine biological productivity, (2) relative abundance of phytoplankton species and (3) wind intensity. The mean DMS flux perturbation we simulate represents a small negative feedback on global warming; however, the large regional changes may significantly impact regional temperature and precipitation patterns.  相似文献   

20.
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   

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