首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 78 毫秒
1.
Soils in similar geomorphic settings in hyperarid deserts (< 50 mm yr−1) should have similar characteristics because a negative moisture balance controls their development. However, Reg soils in the hyperarid southern Negev and Namib deserts are distinctly different. Soils developed on stable alluvial surfaces with only direct input of rainfall and dust depend heavily on rainfall characteristics. Annual rainfall amount can be similar (15-30 mm), but storm duration can drastically alter Reg soil properties in deserts. The cooler fall/winter and dry hot summers of the southern Negev Desert with a predominance brief (≤ 1 day) rainstorms result in gypsic-saline soils without any calcic soil horizon. Although the Namib Desert receives only 50-60% of the southern Negev annual rainfall, its rainstorm duration is commonly 2-4 days. This improves leaching of the top soil under even lower annual rainfall amount and results in weeks-long grass cover. The long-term cumulative effect of these rare rain-grass relationships produces a calcic-gypsic-saline soil. The development of these different kinds of desert soils highlights the importance of daily to seasonal rainfall characteristics in influencing soil-moisture regime in deserts, and has important implications for the use of key desert soil properties as proxies in paleoclimatology.  相似文献   

2.
We measured Ca stable isotope ratios (δ44/40Ca) in an ancient (2 My), hyperarid soil where the primary source of mobile Ca is atmospheric deposition. Most of the Ca in the upper meter of this soil (3.5 kmol m−2) is present as sulfates (2.5 kmol m−2), and to a lesser extent carbonates (0.4 kmol m−2). In aqueous extracts of variably hydrated calcium sulfate minerals, δ44/40CaE values (vs. bulk Earth) increase with depth (1.4 m) from a minimum of −1.91‰ to a maximum of +0.59‰. The trend in carbonate-δ44/40Ca in the top six horizons resembles that of sulfate-δ44/40Ca, but with values 0.1-0.6‰ higher. The range of observed Ca isotope values in this soil is about half that of δ44/40Ca values observed on Earth. Linear correlation among δ44/40Ca, δ34S and δ18O values indicates either (a) a simultaneous change in atmospheric input values for all three elements over time, or (b) isotopic fractionation of all three elements during downward transport. We present evidence that the latter is the primary cause of the isotopic variation that we observe. Sulfate-δ34S values are positively correlated with sulfate-δ18O values (R2 = 0.78) and negatively correlated with sulfate δ44/40CaE values (R2 = 0.70). If constant fractionation and conservation of mass with downward transport are assumed, these relationships indicate a δ44/40Ca fractionation factor of −0.4‰ in CaSO4. The overall depth trend in Ca isotopes is reproduced by a model of isotopic fractionation during downward Ca transport that considers small and infrequent but regularly recurring rainfall events. Near surface low Ca isotope values are reproduced by a Rayleigh model derived from measured Ca concentrations and the Ca fractionation factor predicted by the relationship with S isotopes. This indicates that the primary mechanism of stable isotope fractionation in CaSO4 is incremental and effectively irreversible removal of an isotopically enriched dissolved phase by downward transport during small rainfall events.  相似文献   

3.
We evaluate the impact of exceptionally sparse plant cover (0-20%) and rainfall (2-114 mm/yr) on the stable carbon and oxygen composition of soil carbonate along elevation transects in what is among the driest places on the planet, the Atacama Desert in northern Chile. δ13C and δ18O values of carbonates from the Atacama are the highest of any desert in the world. δ13C (VPDB) values from soil carbonate range from −8.2‰ at the wettest sites to +7.9‰ at the driest. We measured plant composition and modeled respiration rates required to form these carbonate isotopic values using a modified version of the soil diffusion model of [Cerling (1984) Earth Planet. Sci. Lett.71, 229-240], in which we assumed an exponential form of the soil CO2 production function, and relatively shallow (20-30 cm) average production depths. Overall, we find that respiration rates are the main predictor of the δ13C value of soil carbonate in the Atacama, whereas the fraction C3 to C4 biomass at individual sites has a subordinate influence. The high average δ13C value (+4.1‰) of carbonate from the driest study sites indicates it formed—perhaps abiotically—in the presence of pure atmospheric CO2.δ18O (VPDB) values from soil carbonate range from −5.9‰ at the wettest sites to +7.3‰ at the driest and show much less regular variation with elevation change than δ13C values. δ18O values for soil carbonate predicted from local temperature and δ18O values of rainfall values suggest that extreme (>80% in some cases) soil dewatering by evaporation occurs at most sites prior to carbonate formation. The effects of evaporation compromise the use of δ18O values from ancient soil carbonate to reconstruct paleoelevation in such arid settings.  相似文献   

4.
Soils in the McMurdo Dry Valleys, Antarctica contain ice and considerable amounts of salt. Ice often occurs at shallow depth throughout the Dry Valleys and other areas of hyperarid permafrost, notably on Mars. This common occurrence of shallow ice is enigmatic; however, since according to published sublimation models it should disappear relatively quickly (at rates of order 0.1 mm a−1) due to vapor loss to the atmosphere. This loss may be offset by recharge from snowmelt infiltrating and freezing in the soil. Herein, we present a first quantitative estimate of this recharge based on measured vertical profiles of δD and δ18O that reveal considerable detail about the sources and sinks of ice. We model these profiles, taking into account the salt content and a soil temperature record along a 1.6 m depth profile of ∼10 ka old ice-cemented soils in Victoria Valley, Antarctica. The stable isotopes of ice are enriched in heavy isotopes at the top of the ice cement (20 cm depth); both δD and δ18O values plotted against depth exhibit a concave upward curve. At depth, the isotope composition is similar to that of Lake Victoria and modern meteoric water. The concave shape of the isotope profile is suggestive of downward advection-dispersion of snowmelt water enriched in heavy isotopes into the ice cement. Our advection-dispersion model, coupled with field data, enables us to quantify the advective flux and dispersion of melt water into the ice. The advective velocity and dispersion coefficient depend on the time since advection began and the ice-to-brine ratio; they are, respectively, of the order of 10−11-10−10 m s−1 and 10−12-10−11 m2 s−1. These values suggest that over the ∼10 ka time period, a total of 190 mm water infiltrated into the ice-cemented ground. The isotope composition and deuterium excess values of the uppermost ice cement can be modeled from snowmelt water enriched in salts using open system-Rayleigh fractionation. To develop the isotopic signature of the upper ice cement requires evaporation of ∼95% of the snowmelt water. Based on 190 mm brine infiltrating into the soil requires an initial total of ∼4 m of snowmelt water. This corresponds to ∼0.4 mm a−1 suggesting that, under the current climate condition, water from snowmelt is sufficient to compensate modeled sublimation rates, and therefore conserve ground ice in Victoria Valley.  相似文献   

5.
We report the application of an in situ method to obtain field dissolution rates of fine mineral particles in soils. Samples with different metal-containing mineral and slag particles (lead oxide, copper concentrate and copper slag) from the mining and smelting industry were buried in the topsoil of an acidic forest soil for up to 18 months. In addition we studied the dissolution of these particles in samples of the same soil, in a sand matrix and in acid solution under constant temperature and moisture conditions in the laboratory. Under field conditions the PbO particles dissolved quite rapidly (2.4 ± 0.7 × 10−10 mol Pb m−2 s−1), whereas the copper concentrate (<1 × 10−11 mol Cu m−2 s−1) and the copper slag particles (4.3 ± 0.8 × 10−11 mol Cu m−2 s−1) proved to be more resistant to weathering. In addition to qualitative information on dissolution features (SEM), the method yielded quantitative data on in situ dissolution rates. The dissolution rates followed the order: sand with acid percolation (pH 3.5; lab) < soil (lab) < soil (field) < acid solution (pH 3.5; lab). Dissolution rates in soil were found to be lower under laboratory than under field conditions. The faster field rates may in part be attributed to the higher biological activity in the field soil compared to the same soil in the laboratory.  相似文献   

6.
The use of stable Pb isotopes for tracing Pb contamination within the environment has strongly increased our understanding of the fate of airborne Pb contaminants within the boreal forest. This paper presents new stable Pb isotope (206Pb/207Pb ratio) measurements of solid soil samples, stream water (from a mire outlet and a stream draining a forest dominated catchment) and components of Picea abies (roots, needles and stemwood), and synthesizes some of the authors’ recent findings regarding the biogeochemistry of Pb within the boreal forest. The data clearly indicate that the biogeochemical cycling of Pb in the present-day boreal forest ecosystem is dominated by pollution Pb from atmospheric deposition. The 206Pb/207Pb ratios of the mor layer (O-horizon), forest plants and stream water (mainly between 1.14 and 1.20) are similar to atmospheric Pb pollution (1.14–1.19), while the local geogenic Pb of the mineral soil (C-horizon) has high ratios (>1.30). Roots and basal stemwood of the analyzed forest trees have higher 206Pb/207Pb ratios (1.15–1.30) than needles and apical stemwood (1.14–1.18), which indicate that the latter components are more dominated by pollution derived Pb. The low 206Pb/207Pb ratios of the mor layer suggest that the upward transport of Pb as a result of plant uptake is small (<0.04 mg m−2 a−1) in comparison to atmospheric inputs (∼0.5 mg m−2 a−1) and annual losses with percolating soil-water (∼2 mg m−2 a−1); consequently, the Pb levels in the mor layer are now decreasing while the pool of Pb in the mineral soil is increasing. Streams draining mires appear more strongly affected by pollution Pb than streams from forested catchments, as indicated by Pb concentrations about three times higher and lower 206Pb/207Pb ratios (1.16 ± 0.01 in comparison to 1.18 ± 0.02). To what extent stream water Pb levels will respond to the build-up of Pb in deeper mineral soil layers remains uncertain.  相似文献   

7.
Carbon dioxide emissions and heat flow have been determined from the Ohaaki hydrothermal field, Taupo Volcanic Zone (TVZ), New Zealand following 20 a of production (116 MWe). Soil CO2 degassing was quantified with 2663 CO2 flux measurements using the accumulation chamber method, and 2563 soil temperatures were measured and converted to equivalent heat flow (W m−2) using published soil temperature heat flow functions. Both CO2 flux and heat flow were analysed statistically and then modelled using 500 sequential Gaussian simulations. Forty subsoil CO2 gas samples were also analysed for stable C isotopes. Following 20 a of production, current CO2 emissions equated to 111 ± 6.7 T/d. Observed heat flow was 70 ± 6.4 MW, compared with a pre-production value of 122 MW. This 52 MW reduction in surface heat flow is due to production-induced drying up of all alkali–Cl outflows (61.5 MW) and steam-heated pools (8.6 MW) within the Ohaaki West thermal area (OHW). The drying up of all alkali–Cl outflows at Ohaaki means that the soil zone is now the major natural pathway of heat release from the high-temperature reservoir. On the other hand, a net gain in thermal ground heat flow of 18 MW (from 25 MW to 43.3 ± 5 MW) at OHW is associated with permeability increases resulting from surface unit fracturing by production-induced ground subsidence. The Ohaaki East (OHE) thermal area showed no change in distribution of shallow and deep soil temperature contours despite 20 a of production, with an observed heat flow of 26.7 ± 3 MW and a CO2 emission rate of 39 ± 3 T/d. The negligible change in the thermal status of the OHE thermal area is attributed to the low permeability of the reservoir beneath this area, which has limited production (mass extraction) and sheltered the area from the pressure decline within the main reservoir. Chemistry suggests that although alkali–Cl outflows once contributed significantly to the natural surface heat flow (∼50%) they contributed little (<1%) to pre-production CO2 emissions due to the loss of >99% of the original CO2 content due to depressurisation and boiling as the fluids ascended to the surface. Consequently, the soil has persisted as the major (99%) pathway of CO2 release to the atmosphere from the high temperature reservoir at Ohaaki. The CO2 flux and heat flow surveys indicate that despite 20 a of production the variability in location, spatial extent and magnitude of CO2 flux remains consistent with established geochemical and geophysical models of the Ohaaki Field. At both OHW and OHE carbon isotopic analyses of soil gas indicate a two-stage fractionation process for moderate-flux (>60 g m−2 d−1) sites; boiling during fluid ascent within the underlying reservoir and isotopic enrichment as CO2 diffuses through porous media of the soil zone. For high-flux sites (>300 g m−2 d−1), the δ13CO2 signature (−7.4 ± 0.3‰ OHW and −6.5 ± 0.6‰ OHE) is unaffected by near-surface (soil zone) fractionation processes and reflects the composition of the boiled magmatic CO2 source for each respective upflow. Flux thresholds of <30 g m−2 d−1 for purely diffusive gas transport, between 30 and 300 g m−2 d−1 for combined diffusive–advective transport, and ?300 g m−2 d−1 for purely advective gas transport at Ohaaki were assigned. δ13CO2 values and cumulative probability plots of CO2 flux data both identified a threshold of ∼15 g m−2 d−1 by which background (atmospheric and soil respired) CO2 may be differentiated from hydrothermal CO2.  相似文献   

8.
Methane microseepage is the result of natural gas migration from subsurface hydrocarbon accumulations to the Earth’s surface, and it is quite common in commercial petroleum fields. While the role of microseepage as a pathfinder in petroleum exploration has been known for about 80 a, its significance as an atmospheric CH4 source has only recently been studied, and flux data are currently available only in the USA and Europe. With the aim of increasing the global data-set and better understanding flux magnitudes and variabilities, microseepage is now being extensively studied in China. A static flux chamber method was recently applied to study microseepage emissions into the atmosphere in four different sectors of the Yakela condensed gas field in Tarim Basin, Xinjiang, China, and specifically in: (a) a faulted sector, across the Luntai fault systems; (b) an oil–water interface sector, at the northern margin of the field; (c) an oil–gas interface sector, in the middle of the field; (d) an external area, outside the northern gas field boundaries. The results show that positive CH4 fluxes are pervasive in all sectors and therefore, only part of the CH4 migrating from the deep oil–gas reservoirs is consumed in the soil by methanotrophic oxidation. The intensity of gas seepage seems to be controlled by subsurface geologic settings and lateral variabilities of natural gas pressure in the condensed gas field. The highest CH4 fluxes, up to ∼14 mg m−2 d−1 (mean of 7.55 mg m−2 d−1) with higher spatial variability (standard deviation, σ: 2.58 mg m−2 d−1), occur in the Luntai fault sector. Merhane flux was lower in the oil–water area (mean of 0.53 mg m−2 d−1) and the external area (mean of 1.55 mg m−2 d−1), and at the intermediate level in the gas–oil sector (mean of 2.89 mg m−2 d−1). These values are consistent with microseepage data reported for petroleum basins in the USA and Europe. The build-up of methane concentration in the flux chambers is always coupled with an enrichment of 13C, from δ13C1 of −46‰ to −42.5‰ (VPDB), which demonstrates that seeping methane is thermogenic, as that occurring in the deep Yakela reservoir. Daily variations of microseepage are very low, with minima in the afternoon, corresponding to higher soil temperature (and higher methanotrophic consumption), and maxima in the early morning (when soil temperatures are lowest). A preliminary and rough estimate of the total amount of CH4 exhaled from the Yakela field is in the order of 102 tonnes a−1.  相似文献   

9.
Hydrochemical patterns resulting from differing bedrock geochemistry were ascertained by concurrent streamwater sampling in three small catchments, each underlain by geochemically contrasting silicate rock types in the western Czech Republic, Central Europe in 2001–2010. The catchments are situated 5–7 km apart in the Slavkov Forest and are occupied by Norway spruce (Picea abies) plantations. They have similar altitude, area, topography, mean annual air temperature, and atmospheric deposition fluxes. The amount of base cations oxides (Ca + Mg + Na + K) is markedly different among the three studied rocks (leucogranite 8%, amphibolite 22%, serpentinite 36%). The leucogranite contains a very small amount of MgO, while the serpentinite contains extremely large amounts of MgO. The amphibolite contains an intermediate amount of MgO and elevated CaO. The Lysina, on leucogranite, exhibited very small concentrations of Mg (median 0.4 mg L−1) in streamwater; Pluh?v Bor, on serpentinite, contained extremely high concentrations of streamwater Mg (18 mg L−1). Streamwater in the Na Zeleném catchment, on amphibolite, contained an intermediate amount of Mg and an elevated Ca. Very low pH (4.2), negative alkalinity (−60 μeq L−1) and high inorganic monomeric Al concentrations (0.3 mg L−1) were found in the stream draining leucogranite. Serpentinite streamwater exhibited the highest pH (7.6), alkalinity (+940 μeq L−1) and Ni concentrations (100 μg L−1). Aquatic chemistry reflected the composition of the underlying rocks within the studied catchments. Contrasting streamwater compositions of the studied catchments were generated according to the MAGIC model simulations mainly by differences in chemical weathering rates of base cations (65 meq m−2 a−1 at Lysina, 198 meq m−2 a−1 at Na Zeleném, and 241 meq m−2 a−1 at Pluh?v Bor).  相似文献   

10.
Located in the uplands of the Valley and Ridge physiographic province of Pennsylvania, the Susquehanna/Shale Hills Critical Zone Observatory (SSHO) is a tectonically quiescent, first-order catchment developed on shales of the Silurian Rose Hill Formation. We used soil cores augered at the highest point of the watershed and along a subsurface water flowline on a planar hillslope to investigate mineral transformations and physical/chemical weathering fluxes. About 25 m of bedrock was also drilled to estimate parent composition. Depletion of carbonate at tens of meters of depth in bedrock may delineate a deep carbonate-weathering front. Overlying this, extending from ∼6 m below the bedrock-soil interface up into the soil, is the feldspar dissolution front. In the soils, depletion profiles for K, Mg, Si, Fe, and Al relative to the bedrock define the illite and chlorite reaction fronts. When combined with a cosmogenic nuclide-derived erosion rate on watershed sediments, these depletion profiles are consistent with dissolution rates that are several orders of magnitudes slower for chlorite (1-5 × 10−17 mol m−2 s−1) and illite (2-9 × 10−17 mol m−2 s−1) than observed in the laboratory. Mineral reactions result in formation of vermiculite, hydroxy-interlayered vermiculite, and minor kaolinite. During weathering, exchangeable divalent cations are replaced by Al as soil pH decreases.The losses of Mg and K in the soils occur largely as solute fluxes; in contrast, losses of Al and Fe are mostly as downslope transport of fine particles. Physical erosion of bulk soils also occurs: results from a steady-state model demonstrate that physical erosion accounts for about half of the total denudation at the ridgetop and midslope positions. Chemical weathering losses of Mg, Na, and K are higher in the upslope positions likely because of the higher degree of chemical undersaturation in porewaters. Chemical weathering slows down in the valley floor and Al and Si even show net accumulation. The simplest model for the hillslope that is consistent with all observations is a steady-state, clay weathering-limited system where soil production rates decrease with increasing soil thickness.  相似文献   

11.
Mercury air/surface exchange was measured over litter-covered soils with low Hg concentrations within various types of forests along the eastern seaboard of the USA. The fieldwork was conducted at six forested sites in state parks in South Carolina, North Carolina, New Jersey, Pennsylvania, New York and Maine from mid-May to early June 2005. The study showed that the Hg air/surface exchange was consistently very low and similar (overall daytime mean flux = 0.2 ± 0.9 ng m−2 h−1, n = 310, for all six sites monitored) with the various forest types. These flux values are comparable with those found in a year-long study in Tennessee (yearly daytime mean = 0.4 ± 0.5 ng m−2 h−1), but lower than many previous flux results reported for background soils. The Hg fluxes at all sites oscillated around zero, with many episodes of deposition (negative fluxes) occurring in both daytime and nighttime. While there were particular days showing significant correlations among the Hg air/surface exchange and certain environmental parameters, perhaps because of the low fluxes encountered, few significant correlations were found for any particular day of sampling between the Hg flux and environmental parameters such as solar radiation, soil temperature, air temperature (little variability seen), relative humidity, and ambient air Hg concentrations. Factors driving the Hg exchange as previously found for enriched soils may not hold for these background litter-covered forest soils. The results suggest that spatial variations of the Hg air/surface exchange were small among these different forest types for this particular time of year.  相似文献   

12.
Diffusion of 36Cl− in compacted bentonite was studied using through-diffusion, out-diffusion and profile analysis techniques. Both the bulk dry density of the bentonite and the composition of the external solution were varied. Increasing the bulk dry density of the bentonite resulted in a decrease of both the effective diffusion coefficient and the Cl-accessible porosity. Increasing the ionic strength of the external solutions resulted in an increase of both the effective diffusion coefficient and the Cl-accessible porosity. This can be explained by anion exclusion effects (Donnan exclusion). At high ionic strength values (I ? 1 M NaCl) the Cl-accessible porosity approaches the interparticle porosity. This interparticle porosity is the difference between the total and interlayer porosity of the bentonite. The interlayer porosity was found to depend on the degree of compaction. Up to a bulk dry density of 1300 kg m−3 the interlayer is built up of 3 water layers. Between 1300 and 1800 kg m−3 the interlayer water is reduced from 3 to 2 layers of water. Above 1800 kg m−3 evidence for a further decrease to 1 layer of water was found. These findings are in agreement with X-ray data found in the literature showing a decrease of the basal spacing of montmorillonite (the main clay mineral in bentonite) with increasing degree of compaction. The relationship between the effective diffusion coefficient of Cl− and the diffusion-accessible porosity can be described by an empirical relationship analogous to Archie’s law. To predict the effective diffusion coefficient of Cl− in compacted bentonite, the diffusion coefficient of Cl− in water, the bulk dry density and the ionic strength of the pore water have to be known.  相似文献   

13.
Concentrations of atmospheric Hg species, elemental Hg (Hg°), reactive gaseous Hg (RGM), and fine particulate Hg (Hg-PM2.5) were measured at a coastal site near Weeks Bay, Alabama from April to August, 2005 and January to May, 2006. Mean concentrations of the species were 1.6 ± 0.3 ng m−3, 4.0 ± 7.5 pg m−3 and 2.7 ± 3.4 pg m−3, respectively. A strong diel pattern was observed for RGM (midday maximum concentrations were up to 92.7 pg m−3), but not for Hg° or Hg-PM2.5. Elevated RGM concentrations (>25 pg m−3) in April and May of 2005 correlated with elevated average daytime O3 concentrations (>55 ppbv) and high light intensity (>500 W m−2). These conditions generally corresponded with mixed continental-Gulf and exclusively continental air mass trajectories. Generally lower, but still elevated, RGM peaks observed in August, 2005 and January–March, 2006 correlated significantly (p < 0.05) with peaks in SO2 concentration and corresponded to periods of high light intensity and lower average daytime O3 concentrations. During these times air masses were dominated by trajectories that originated over the continent. Elevated RGM concentrations likely resulted from photochemical oxidation of Hg° by atmospheric oxidants. This process may have been enhanced in and by the near-shore environment relative to inland sites. The marine boundary layer itself was not found to be a significant source of RGM.  相似文献   

14.
The preferential incorporation of High-Field-Strength Elements (HFSE) in rutile (TiO2), combined with its supposed stability in subduction zone settings, make it an ideal candidate to explain the low HFSE concentrations in subduction-derived magmas. The solubility behaviour of rutile is key to these arguments, but at present experimental and field-based evidence are contradictory.We have used abinitio molecular (meta)dynamics to investigate the coordination environment of Ti(IV) in pure water at 300 and 1000 K and densities ranging from 900-1260 kg m−3 (approximate pressures 0.9-3.6 GPa). In all high temperature simulations, the long-range structure of the solvent indicates a breakdown of the hydrogen bonding network as expected for supercritical water. The five-fold coordination of titanium to water is energetically most favourable in aqueous fluids at room temperature and pressure, separated from four and six-fold configurations by ∼175 and ∼200 kJ mol−1, respectively. The average first shell Ti-O distance is 2.00 Å, in excellent agreement with bond lengths obtained from experiments. At similar densities and 1000 K, titanium is on average six-fold coordinate with water, and shows some degree of water dissociation in the first hydration shell. This coordination environment is remarkably persistent with increasing density from 1021 to 1260 kg m−3 at constant temperature (1000 K). At lower densities, however, (900 kg m−3 at 1000 K), the coordination with first shell water molecules is less than five. The observed coordination changes could promote association of titanium with peralkaline or peraluminous domains in the aqueous fluid, and thereby explain field-and laboratory based evidence of enhanced HFSE concentrations.This study demonstrates that abinitio molecular dynamics has considerable potential to access details of element behaviour in aqueous fluids at geologically relevant conditions that are impossible to examine otherwise. Changes in the solvent structure due to density variations lead to differences in solvent behaviour allowing access to new domains for fluid-solid interaction. Moreover, changes in the solvent structure are strongly linked to the effectiveness of element solvation.  相似文献   

15.
Sr isotope data from soils, water, and atmospheric inputs in a small tropical granitoid watershed in the Luquillo Mountains of Puerto Rico constrain soil mineral development, weathering fluxes, and atmospheric deposition. This study provides new information on pedogenic processes and geochemical fluxes that is not apparent in watershed mass balances based on major elements alone. 87Sr/86Sr data reveal that Saharan mineral aerosol dust contributes significantly to atmospheric inputs. Watershed-scale Sr isotope mass balance calculations indicate that the dust deposition flux for the watershed is 2100 ± 700 mg cm−2 ka−1. Nd isotope analyses of soil and saprolite samples provide independent evidence for the presence of Saharan dust in the regolith. Watershed-scale Sr isotope mass balance calculations are used to calculate the overall short-term chemical denudation velocity for the watershed, which agrees well with previous denudation rate estimates based on major element chemistry and cosmogenic nuclides. The dissolved streamwater Sr flux is dominated by weathering of plagioclase and hornblende and partial weathering of biotite in the saprock zone. A steep gradient in regolith porewater 87Sr/86Sr ratio with depth, from 0.70635 to as high as 0.71395, reflects the transition from primary mineral-derived Sr to a combination of residual biotite-derived Sr and atmospherically-derived Sr near the surface, and allows multiple origins of kaolinite to be identified.  相似文献   

16.
An experimental study was carried out in order to evaluate the impact of nitrogen fertiliser-induced acidification in carbonated soils. Undisturbed soil columns containing different carbonate content were sampled in the field. Fertiliser spreading was simulated by NH4Cl addition on top of the soil column. Soil solution composition (mainly nitrate and base cations) was studied at the soil column’s base. Nitrification occurred to a different extent depending on soil type. Higher nitrification rates were observed in calcareous soils. In all the soil types, strong correlations between leached base cation and nitrate concentrations were observed. Regression coefficients between base cations, nitrate and chloride were used to determine the dominant processes occurring following NH4Cl spreading. In non-carbonated soils, nitrogen nitrification induced base cation leaching and soil acidification. In carbonated soils, no change of soil pH was observed. However, fertilisers induced a huge cation leaching. Carbonate mineral weathering led to the release of base cations, which replenished the soil exchangeable complex. Carbonated mineral weathering buffered acidification. Since direct weathering might have occurred without atmospheric CO2 consumption, the use of nitrogen fertiliser on carbonated soil induces a change in the cation and carbon budgets. When the results of these experiments are extrapolated on a global scale to the surface of fertilised areas lying on carbonate, carbonated reactions with N fertilisers would imply an additional flux of 5.7 × 1012 mol yr−1 of Ca + Mg. The modifications of weathering reactions in cultivated catchments and the ability of nitrogen fertilisers to significantly modify the CO2 budget should be included in carbon global cycle assessment.  相似文献   

17.
The influence of soil organisms on metal mobility and bioavailability in soils is not currently fully understood. We conducted experiments to determine whether calcium carbonate granules secreted by the earthworm Lumbricus terrestris could incorporate and immobilise lead in lead- and calcium-amended artificial soils. Soil lead concentrations were up to 2000 mg kg−1 and lead:calcium ratios by mass were 0.5-8. Average granule production rates of 0.39 ± 0.04 mgcalcite earthworm−1 day−1 did not vary with soil lead concentration. The lead:calcium ratio in granules increased significantly with that of the soil (r2 = 0.81, p = 0.015) with lead concentrations in granules reaching 1577 mg kg−1. X-ray diffraction detected calcite and aragonite in the granules with indications that lead was incorporated into the calcite at the surface of the granules. In addition to the presence of calcite and aragonite X-ray absorption spectroscopy indicated that lead was present in the granules mainly as complexes sorbed to the surface but with traces of lead-bearing calcite and cerussite. The impact that lead-incorporation into earthworm calcite granules has on lead mobility at lead-contaminated sites will depend on the fraction of total soil lead that would be otherwise mobile.  相似文献   

18.
Wetlands are significant sources and sinks for arsenic (As), yet the geochemical conditions and processes causing a release of dissolved arsenic and its association with the solid phase of wetland soils are poorly known. Here we present experiments in which arsenic speciation was determined in peatland mesocosms in high spatiotemporal resolution over 10 months. The experiment included a drought/rewetting treatment, a permanently wet, and a defoliated treatment. Soil water content was determined by the TDR technique, and arsenic, iron and sulfate turnover from mass balancing stocks and fluxes in the peat, and solid phase contents by sequential extractions. Arsenic content ranged from 5 to 25 mg kg−1 and dissolved concentrations from 10 to 300 μg L−1, mainly in form of As(III), and secondarily of As(V) and dimethylated arsenic (DMA). Total arsenic was mainly associated with amorphous iron hydroxides (R2 > 0.95, α < 0.01) and deeper into the peat with an unidentified residual fraction. Arsenic release was linked to ferrous iron release and primarily occurred in the intensely rooted uppermost soil. Volumetric air contents of 2-13 % during drought eliminated DMA from the porewater and suppressed its release after rewetting for >30 d. Dissolved As(III) was oxidized and immobilized as As(V) at rates of up to 0.015 mmol m−3 d−1. Rewetting mobilized As(III) at rates of up to 0.018 mmol m−3 d−1 within days. Concurrently, Fe(II) was released at depth integrated rates of up 20 mmol m−3 d−1. The redox half systems of arsenic, iron, and sulfur were in persistent disequilibrium, with H2S being a thermodynamically viable reductant for As(V) to As(III). The study suggests that rewetting can lead to a rapid release of arsenic in iron-rich peatlands and that methylation is of lesser importance than co-release with iron reduction, which was largely driven by root activity.  相似文献   

19.
Mercury fluxes from air/surface interfaces in paddy field and dry land   总被引：3，自引：0，他引：3  
In order to provide insight into the characteristics of Hg exchange in soil/water-air surface from cropland (including paddy field and dry land), Hg fluxes were measured in Chengjiang. Mercury fluxes were measured using the dynamic flux chamber method, coupled with a Lumex® multifunctional Hg analyzer RA-915+ (Lumex Ltd., Russia). The Hg fluxes from paddy field and dry land were alternatively measured every 30 min. Data were collected for 24-48 h once per month for 5 months. Mercury fluxes in both fields were synchronously measured under the same conditions to compare Hg emissions between paddy field and dry land over diurnal and seasonal periods and find out what factors affect Hg emission on each surface. These results indicated that air Hg concentrations at the monitoring site was double the value observed at the global background sites in Europe and North America. The Hg release fluxes were 46.5 ± 22.8 ng m−2 h−1 in the warm season, 15.5 ± 18.8 ng m−2 h−1 in the cold season for dry land, and 23.8 ± 15.6 ng m−2 h−1 in the warm season, 6.3 ± 11.9 ng m−2 h−1 in the cold season for paddy field. Solar radiation is important in the emission of Hg over both sites. Hg exchange at the soil/air and water/air interfaces showed temporal variations. The amount of Hg emission from dry land was higher than that from the paddy field, and the emission in daytime was higher than that at night. Moreover, Hg emissions from land covered by crops, was lower than that for bare land.  相似文献   

20.
In soils, silicon released by mineral weathering can be retrieved from soil solution through clay formation, Si adsorption onto secondary oxides and plant uptake, thereby impacting the Si-isotopic signature and Ge/Si ratio of dissolved Si (DSi) exported to rivers. Here we use these proxies to study the contribution of biogenic Si (BSi) in a soil-plant system involving basaltic ash soils differing in weathering degree under intensive banana cropping. δ30Si and Ge/Si ratios were determined in bulk soils (<2 mm), sand (50-2000 μm), silt (2-50 μm), amorphous Si (ASi, 2-50 μm) and clay (<2 μm) fractions: δ30Si by MC-ICP-MS Nu Plasma in medium resolution, operating in dry plasma with Mg doping (δ30Si vs. NBS28 ± 0.12‰ ± 2σSD), Ge/Si computed after determination of Ge and Si concentrations by HR-ICP-MS and ICP-AES, respectively. Components of the ASi fraction were quantified by microscopic counting (phytoliths, diatoms, ashes). Compared to fresh ash (δ30Si = −0.38‰; Ge/Si = 2.21 μmol mol−1), soil clay fractions (<2 μm) were enriched in light Si isotopes and Ge: with increasing weathering degree, δ30Si decreased from −1.19 to −2.37‰ and Ge/Si increased from 4.10 to 5.25 μmol mol−1. Sand and silt fractions displayed δ30Si values close to fresh ash (−0.33‰) or higher due to saharian dust quartz deposition, whose contribution was evaluated by isotopic mass balance calculation. Si-isotopic signatures of bulk soils (<2 mm) were strongly governed by the relative proportions of primary and secondary minerals: the bulk soil Si-isotopic budget could be closed indicating that all the phases involved were identified. Microscopic counting highlighted a surface accumulation of banana phytoliths and a stable phytolith pool from previous forested vegetation. δ30Si and Ge/Si values of clay fractions in poorly developed volcanic soils, isotopically heavier and Ge-depleted in surface horizons, support the occurrence of a DSi source from banana phytolith dissolution, available for Si sequestration in clay-sized secondary minerals (clay minerals formation and Si adsorption onto Fe-oxide). In the soil-plant system, δ30Si and Ge/Si are thus highly relevant to trace weathering and input of DSi from phytoliths in secondary minerals, although not quantifying the net input of BSi to DSi.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号