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1.
In natural river systems, the chemical and isotopic composition of stream- and ground waters are mainly controlled by the geology and water-rock interactions. The leaching of major cations from soils has been recognized as a possible consequence of acidic deposition from atmosphere for over 30 years. Moreover, in agricultural areas, the application of physiological acid fertilizers and nitrogen fertilizers in the ammonia form may enhance the cation leaching through the soil profile into ground- and surface waters. This origin of leached cations has been studied on two small and adjacent agricultural catchments in Brittany, western France. The study catchments are drained by two first-order streams, and mainly covered with cambisoils, issued from the alteration and weathering of a granodiorite basement. Precipitations, soil water- and NH4 acetate-leachates, separated minerals, and stream waters have been investigated. Chemical element ratios, such as Ba/Sr, Na/Sr and Ca/Sr ratios, as well as Sr isotopic ratios are used to constrain the relative contribution from potential sources of stream water elements.Based on Sr isotopic ratio and element concentration, soil water- and NH4 acetate leaching indicates (1) a dominant manure/slurry contribution in the top soil, representing a cation concentrated pool, with low 87Sr/86Sr ratios; (2) in subsoils, mineral dissolution is enhanced by fertilizer application, becoming the unique source of cations in the saprolite. The relatively high weathering rates encountered implies significant sources of cations which are not accessory minerals, but rather plagioclase and biotite dissolution.Stream water has a very different isotopic and chemical composition compared to soil water leaching suggesting that stream water chemistry is dominated by elements issued from mineral and rock weathering. Agriculture, by applications of chemical and organic fertilizers, can influence the export of major base cations, such as Na+. Plagioclase dissolution, rather than anthropogenically controlled soil water, seems to be the dominant source of Na+ in streams. However, Ca2+ in streams is mostly derived from slurries and manures deposited on top soils, and transferred into the soil ion-exchange pool and stream waters. Less than 10% of Na+, 5-40% of Sr2+ and 20-100% of Ca2+ found in streams can be directly derived from the application of organic fertilizers.  相似文献   

2.
A simple, unifying approach to classifying quantitatively the susceptibility of catchment soils and surface waters to acidification is suggested. In areas subject to a strong maritime influence, such as the UK and substantial parts of NW Europe, wherever soil mineral weathering rates are low and soils are unfertilised, atmospherically derived base cations of maritime origins have a greater effect than those derived from biogeochemical weathering on the exchangeable soil base cations. This is directly reflected in the relative base cation concentrations of the associated drainage waters, which become increasingly Na-dominated. Using 10 sub-catchments of the River Dee in north-eastern Scotland, it is shown here that the extent of Na dominance, the ratio of Na+ to ΣNa++Ca2++Mg2+, at any point in a river provides a quantitative index of the upstream weathering rate and thus of the susceptibility of the river concerned to acidification under diverse flow conditions. Data from a further 58 sub-catchments from the same river system, and from 4 other catchments from around Scotland, were used to validate this theory.  相似文献   

3.
Plant-available reserves of major base cations, Ca2+ and Mg2+, decreased markedly in soils over the past century, thus posing a potential threat to forest ecosystem health. Trees are thought to obtain dissolved Ca2+ ions mainly from an easily accessible soil-water reservoir also termed the ‘exchangeable cation pool’. The status of Ca reserves in this soil pool is sensitive to anthropogenic perturbations such as soil acidification induced by acid rain and/or excessive timber harvesting. Here we show that in a base-poor forest of the northeastern USA (i.e. Wachusett Mountain, Massachusetts) the ‘exchangeable Ca pool’ of deeper mineral soils has a unique isotope signature that is significantly enriched in the radiogenic 40Ca, due to the dissolution of K-rich silicate minerals such as biotite. Using a simple isotope mass balance, and assuming that the input of Ca from biotite has a εCa signature of ∼16, the results of our calculation indicate that the weathering of biotite may supply a sizeable fraction, up to 25%, of Ca2+ ions into the ‘exchangeable cation pool’ of deeper mineral soils. Importantly, samples of local vegetation (i.e. woody tissues of red oak) show no detectable excess of the radiogenic 40Ca, and based on our model the upper limit of a possible biotite-derived Ca contribution in vegetation is estimated at ∼5%. We also found no evidence of the radiogenic 40Ca signal in the samples of forest floor and the uppermost organic-rich soils (0-15 cm depth), which in turn suggest that over the long-term development of the forest and its organic matter accumulation, the vegetation growth must have also relied primarily on the non-radiogenic Ca sources. Based on our experimental data, such sources may include (i) wet atmospheric deposition, (ii) the organically-complexed Ca in topsoil horizons, and (iii) chemical weathering and/or fungal-mediated dissolution of apatite and Ca-rich plagioclase. Hence, our stable and radiogenic Ca isotope data indicate that the studied base-poor forest is able to bypass the ‘exchangeable cation pool’ of deeper (i.e. below 15 cm) mineral soils, and still manages to meet its nutritional requirements with respect to Ca. Another important implication of this study is that the organically-complexed Ca in the topsoil horizon (0-15 cm depth) has to be tightly bound to the ion exchange sites, otherwise the large radiogenic 40Ca signatures present in the ‘exchangeable cation pool’ of deep mineral soils would be swamped by the downward gravitational flux of non-radiogenic Ca from the decaying organic matter and litterfall. Hence, the limited mobility of the organically-complexed Ca in soils and its tight biological cycling could explain the lack of a significant impact of vegetation on the Ca isotope systematics observed in large rivers.  相似文献   

4.
The potential mineralization and immobilization of soil nitrogen (N), phosphorus (P) and sulfur (S) are relatively high in natural ecosystems. This study was conducted to investigate the changes in essential plant macronutrients; N, P, and S status in response to different soil depth in rangeland ecosystems in vitro. The net nutrient mineralization was measured during 90 days at different depths (0–15, 15–30, 30–45 and 45–60 cm), using kinetic models to estimate the release rate. The net ammonification and mineralization of P and S were described using parabolic diffusion equation, while the power function equation was used to describe the net nitrification. The results indicated that the amount of released ammonium (NH4 +) decreased with time and depth and the rates of net ammonification were negative in all samples. Conversely, nitrification increased with time and depth and the rates were all positive. The net mineralization for both P and S reduced with time. The concentration of mineralized SO4 2? increased with depth like nitrate (NO3 ?). Accumulation of SO4 2? and NO3 ? in subsurface soils and NH4 + and P at surface horizons can increase the potential of their loss by leaching or volatilization.  相似文献   

5.
Ectomycorrhiza-forming fungi (EMF) alter the nutrient-acquisition capabilities of vascular plants, and may play an important role in mineral weathering and the partitioning of products of weathering in soils under nutrient-limited conditions. In this study, we isolated the weathering function of Suillus tomentosus in liquid-cultures with biotite micas incubated at room temperature. We hypothesized that the fungus would accelerate weathering by hyphal attachment to biotite surfaces and transmission of nutrient cations via direct exchange into the fungal biomass. We combined a mass-balance approach with scanning electron microscopy (SEM) and atomic force microscopy (AFM) to estimate weathering rates and study dissolution features on biotite surfaces. Weathering of biotite flakes was about 2-3 orders of magnitude faster in shaken liquid-cultures with fungus compared to shaken controls without fungus, but with added inorganic acids. Adding fungus in nonshaken cultures caused a higher dissolution rate than in inorganic pH controls without fungus, but it was not significantly faster than organic pH controls without fungus. The K+, Mg2+ and Fe2+ from biotite were preferentially partitioned into fungal biomass in the shaken cultures, while in the nonshaken cultures, K+ and Mg2+ was lost from biomass and Fe2+ bioaccumulated much less. Fungal hyphae attached to biotite surfaces, but no significant surface changes were detected by SEM. When cultures were shaken, the AFM images of basal planes appeared to be rougher and had abundant dissolution channels, but such channel development was minor in nonshaken conditions. Even under shaken conditions the channels only accounted for only 1/100 of the total dissolution rate of 2.7 × 10−10 mol of biotite m−2 s−1. The results suggest that fungal weathering predominantly occurred not by attachment and direct transfer of nutrients via hyphae, but because of the acidification of the bulk liquid by organic acids, fungal respiration (CO2), and complexation of cations which accelerated dissolution of biotite. Results further suggest that both carbohydrate source (abundant here) and a host with which nutrients are exchanged (missing here) may be required for EMF to exert an important weathering effect in soils. Unsaturated conditions and physical dispersal of nutrient-rich minerals in soils may also confer a benefit for hyphal growth and attachment, and promote the attachment-mediated weathering which has been observed elsewhere on soil mineral surfaces.  相似文献   

6.
High concentrations of ammonium nitrogen released from tannery sludge during storage in open air may cause nitrogen pollution to soil and groundwater. To study the transformation mechanism of NH4+-N by nitrifying functional bacteria in tannery sludge contaminated soils, a series of contaminated soil culture experiments were conducted in this study. The contents of ammonium nitrogen (as NH4+-N), nitrite nitrogen (as NO2?-N) and nitrate nitrogen (as NO3?-N) were analyzed during the culture period under different conditions of pollution load, soil particle and redox environment. Sigmodial equation was used to interpret the change of NO3?-N with time in contaminated soils. The abundance variations of nitrifying functional genes (amoA and nxrA) were also detected using the real-time quantitative fluorescence PCR method. The results show that the nitrification of NH4+-N was aggravated in the contaminated silt soil and fine sand under the condition of lower pollution load, finer particle size and more oxidizing environment. The sigmodial equation well fitted the dynamic accumulation curve of the NO3?-N content in the tannery sludge contaminated soils. The Cr(III) content increased with increasing pollution load, which inhibited the reproduction and activity of nitrifying bacteria in the soils, especially in coarse-grained soil. The accumulation of NO2?-N contents became more obvious with the increase of pollution load in the fine sand, and only 41.5% of the NH4+-N was transformed to NO3?-N. The redox environment was the main factor affecting nitrification process in the soil. Compared to the aerobic soil environment, the transformation of NH4+-N was significantly inhibited under anaerobic incubation condition, and the NO3?-N contents decreased by 37.2%, 61.9% and 91.9% under low, medium and high pollution loads, respectively. Nitrification was stronger in the silt soil since its copy number of amoA and nxrA genes was two times larger than that of fine sand. Moreover, the copy numbers of amoA and nxrA genes in the silt soil under the aerobic environment were 2.7 times and 2.2 times larger than those in the anaerobic environment. The abundance changes of the amoA and nxrA functional genes have a positive correlation with the nitrification intensity in the tannery sludge-contaminated soil.  相似文献   

7.
Silicate weathering of soil-mantled slopes in an active Alpine landscape   总被引：1，自引：0，他引：1  
Despite being located on high, steep, actively uplifting, and formerly glaciated slopes of the Swiss Central Alps, soils in the upper Rhone Valley are depleted by up to 50% in cations relative to their parent bedrock. This depletion was determined by a mass loss balance based on Zr as a refractory element. Both Holocene weathering rates and physical erosion rates of these slopes are unexpectedly low, as measured by cosmogenic 10Be-derived denudation rates. Chemical depletion fractions, CDF, range from 0.12 to 0.48, while the average soil chemical weathering rate is 33 ± 15 t km−2 yr−1. Both the cosmogenic nuclide-derived denudation rates and model calculations suggest that these soils have reached a weathering steady-state since deglaciation 15 ky ago. The weathering signal varies with elevation and hillslope morphology. In addition, the chemical weathering rates decrease with elevation indicating that temperature may be a dominant controlling factor on weathering in these high Alpine basins. Model calculations suggest that chemical weathering rates are limited by reaction kinetics and not the supply rate of fresh material. We compare hillslope and catchment-wide weathering fluxes with modern stream cation flux, and show that high relief, bare-rock slopes exhibit much lower chemical weathering rates despite higher physical erosion rates. The low weathering fluxes from rocky, rapidly eroding slopes allow for the broader implication that mountain building, while elevating overall denudation rates, may not cause increased chemical weathering rates on hillslopes. In order for this sediment to be weathered, intermediate storage, for instance in floodplains, is required.  相似文献   

8.
Dual isotopic analysis of nitrate (15N/14N and 18O/16O) is increasingly used to investigate the environmental impacts of human-induced elevated atmospheric nitrate deposition. In forested ecosystems, the nitrate found in surface water and groundwater can originate from two sources: (1) atmospheric deposition, and (2) nitrate produced from nitrification in forest soils (microbial nitrate). Application of the dual nitrate isotope technique for determining the relative importance of nitrate sources in forested catchments requires knowledge of the isotopic composition of microbial nitrate. We excluded precipitation inputs to three zero-tension lysimeters installed below the F-horizon (Oe) at the Turkey Lakes Watershed (TLW) in order to measure the isotopic composition of microbial nitrate produced in situ. To our knowledge, this is the first in situ study of the isotopic composition of microbial nitrate in forest soils. Over a 2-week period, nitrate produced by nitrification was periodically flushed to the lysimeters by watering the area with a nitrogen-free solution. Nitrate produced in the forest floor had δ18O values ranging from +3.1‰ to +10.1‰ with a mean of +5.2‰. These values were only slightly higher than from the expected value of +1.0‰ calculated for chemolithoautotrophic nitrification, which depends on the δ18O of available O2 and H2O. In addition to nitrate, we also collected soil gas to determine if soil respiration and O2 diffusion affected soil gas δ18O-O2, which is typically assumed to be identical to atmospheric O2 (+23.5‰) when calculating microbial nitrate δ18O values. No significant difference in δ18O-O2 from atmospheric O2 was found in forest soils to a depth of 55 cm, and therefore 18O-enrichment of soil gas O2 could not explain the modest enrichment of nitrate 18O. Evaporative 18O-enrichment of soil water available to nitrifiers in the forest floor is a plausible mechanism for slightly elevated nitrate δ18O values. However, the observed nitrate δ18O values could also be explained by a minor contribution of nitrate from heterotrophic nitrifiers. The δ15N of nitrate produced ranged from −10.4 to −7.3‰ and, as expected, was depleted in 15N relative to soil organic nitrogen. Microbial nitrate produced in the forest floor was also significantly depleted in 15N relative to microbial nitrate exported in groundwater and headwater streams at the TLW. We hypothesize that 15N-depleted forest floor nitrate is not detected in groundwaters largely because of: (1) the immobilization of forest floor nitrate in the mineral soil and (2) the mixing of the remaining forest floor nitrate with nitrate generated in the mineral soil, which is expected to have higher δ15N values. This study demonstrates that current methods of calculating a priori the δ18O of microbial nitrate provide a reasonable value for nitrate produced by nitrification at the TLW.  相似文献   

9.
The goal of this study was to highlight the occurrence of an additional proton-promoted weathering pathway of carbonate rocks in agricultural areas where N-fertilizers are extensively spread, and to estimate its consequences on riverine alkalinity and uptake of CO2 by weathering. We surveyed 25 small streams in the calcareous molassic Gascogne area located in the Garonne river basin (south-western France) that drain cultivated or forested catchments for their major element compositions during different hydrologic periods. Among these catchments, the Hay and the Montoussé, two experimental catchments, were monitored on a weekly basis. Studies in the literature from other small carbonate catchments in Europe were dissected in the same way. In areas of intensive agriculture, the molar ratio (Ca + Mg)/HCO3 in surface waters is significantly higher (0.7 on average) than in areas of low anthropogenic pressure (0.5). This corresponds to a decrease in riverine alkalinity, which can reach 80% during storm events. This relative loss of alkalinity correlates well with the content in surface waters. In cultivated areas, the contribution of atmospheric/soil CO2 to the total riverine alkalinity (CO2 ATM-SOIL/HCO3) is less than 50% (expected value for carbonate basins), and it decreases when the nitrate concentration increases. This loss of alkalinity can be attributed to the substitution of carbonic acid (natural weathering pathway) by protons produced by nitrification of N-fertilizers (anthropogenic weathering pathway) occurring in soils during carbonate dissolution. As a consequence of these processes, the alkalinity over the last 30 years shows a decreasing trend in the Save river (one of the main Garonne river tributaries, draining an agricultural catchment), while the nitrate and calcium plus magnesium contents are increasing.We estimated that the contribution of atmospheric/soil CO2 to riverine alkalinity decreased by about 7-17% on average for all the studied catchments. Using these values, the deficit of CO2 uptake can be estimated as up to 0.22-0.53 and 12-29 Tg1 yr−1 CO2 on a country scale (France) and a global scale, respectively. These losses represent up to 5.7-13.4% and only 1.6-3.8% of the total CO2 flux naturally consumed by carbonate dissolution, for France and on a global scale, respectively. Nevertheless, this loss of alkalinity relative to the Ca + Mg content relates to carbonate weathering by protons from N-fertilizers nitrification, which is a net source of CO2 for the atmosphere. This anthropogenic CO2 source is not negligible since it could reach 6-15% of CO2 uptake by natural silicate weathering and could consequently partly counterbalance this natural CO2 sink.  相似文献   

10.
《Applied Geochemistry》1993,8(3):273-283
A new model for base cation release due to chemical weathering of soil minerals has been developed based on transition state theory, and included in the integrated soil chemistry model PROFILE. The data required for model application can be operationally determined on soil samples, making the model generally applicable and independent of any type of calibration. The model considers the contribution to the weathering rate from 12 groups of the most common primary and secondary minerals of soils, reacting in separate reactions with H+-ion, H2O, CO2 and organic acids expressed as dissolved organic carbon (DOC). The weathering rate sub-model couples the effects of dissolved Al and base cations on the reaction mechanisms. The model takes into account changes in soil temperature, different chemical conditions, the effect of vegetation interactions with the soil and N transformations. The kinetic coefficients and reaction orders are based on a complete re-evaluation of weathering data available in the literature, and additional kinetic data determined by the authors.Data from 23 different independent determinations of the field weathering rate from 15 sites in Scandinavia, Central Europe and North America were compiled and used to verify the model. The model is capable of estimating the release rate of base cations due to chemical weathering from information on soil mineralogy, texture and geochemical properties of the order of ±20% of the rate determined by independent methods. The results indicate that small amounts of dark minerals like epidote and hornblende, and the plagioclase content, largely determine the field weathering rate.  相似文献   

11.
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12.
The spatial and temporal changes in hydrology and pore water elemental and 87Sr/86Sr compositions are used to determine contemporary weathering rates in a 65- to 226-kyr-old soil chronosequence formed from granitic sediments deposited on marine terraces along coastal California. Soil moisture, tension and saturation exhibit large seasonal variations in shallow soils in response to a Mediterranean climate. These climate effects are dampened in underlying argillic horizons that progressively developed in older soils, and reached steady-state conditions in unsaturated horizons extending to depths in excess of 15 m. Hydraulic fluxes (qh), based on Cl mass balances, vary from 0.06 to 0.22 m yr−1, resulting in fluid residence times in the terraces of 10-24 yrs.As expected for a coastal environment, the order of cation abundances in soil pore waters is comparable to sea water, i.e., Na > Mg > Ca > K > Sr, while the anion sequence Cl > NO3 > HCO3 > SO4 reflects modifying effects of nutrient cycling in the grassland vegetation. Net Cl-corrected solute Na, K and Si increase with depth, denoting inputs from feldspar weathering. Solute 87Sr/86Sr ratios exhibit progressive mixing of sea water-dominated precipitation with inputs from less radiogenic plagioclase. While net Sr and Ca concentrations are anomalously high in shallow soils due to biological cycling, they decline with depth to low and/or negative net concentrations. Ca/Mg, Sr/Mg and 87Sr/86Sr solute and exchange ratios are similar in all the terraces, denoting active exchange equilibration with selectivities close to unity for both detrital smectite and secondary kaolinite. Large differences in the magnitudes of the pore waters and exchange reservoirs result in short-term buffering of the solute Ca, Sr, and Mg. Such buffering over geologic time scales can not be sustained due to declining inputs from residual plagioclase and smectite, implying periodic resetting of the exchange reservoir such as by past vegetational changes and/or climate.Pore waters approach thermodynamic saturation with respect to albite at depth in the younger terraces, indicating that weathering rates ultimately become transport-limited and dependent on hydrologic flux. Contemporary rates Rsolute are estimated from linear Na and Si pore weathering gradients bsolute such that
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13.
Temporal variations in the concentration and N isotopic ratios of inorganic N (NH4– and NO3–N) as affected by the soil temperature regime together with the input of bird excreta were analyzed in a sedentary soil under a dense colony (1.6 nests/m2) of breeding Black-tailed Gulls (Laruscrassirostris: a ground-nesting seabird). Surface soil samples were taken monthly from mid-March to late July 2005 from Kabushima Island, Hachinohe, northeastern Japan. The spatial concentration of inorganic N in the soils varied considerably on all sampling dates. There may be a statistically significant trend, showing increased NH4–N content from settlement up to early June when the input of fecal N attains its maximum, and then decreases towards the end of breeding activity (early August). Abundant NO3–N was observed in all soils, particularly in the later stage of breeding (up to 3800 mg-N/kg dry soil), refuting earlier claims that nitrification is unimportant in the soils. δ15N values of NH4 in the soils showed unusually high values up to +51‰, reflecting N isotope fractionation due to volatilization of NH3 during the mineralization. Mean δ15N values of the monthly collected totals of NH4 and NO3 were not significantly different at the 5% level based on ANOVA and significant differences were observed only among the three means of NO3–N collected in mid-March (settlement of colony: δ15N = −0.2 ± 3.5‰) and late July (later stages of breeding: δ15N = +22.1 ± 7.0‰, +23.3 ± 7.8‰) at the 1% and 5% levels by t-test, respectively. Such an observation of significantly increased δ15N values for NO3–N in soils from the fledgling stage indicates the integration of denitrification coupled with nitrification under a limited supply of fecal N.  相似文献   

14.
The Yarlung Tsangpo-Brahmaputra river drains a large portion of the Himalaya and southern Tibetan plateau, including the eastern Himalayan syntaxis, one of the most tectonically active regions on the globe. We measured the solute chemistry of 161 streams and major tributaries of the Tsangpo-Brahmaputra to examine the effect of tectonic, climatic, and geologic factors on chemical weathering rates. Specifically, we quantify chemical weathering fluxes and CO2 consumption by silicate weathering in southern Tibet and the eastern syntaxis of the Himalaya, examine the major chemical weathering reactions in the tributaries of the Tsangpo-Brahmaputra, and determine the total weathering flux from carbonate and silicate weathering processes in this region. We show that high precipitation, rapid tectonic uplift, steep channel slopes, and high stream power generate high rates of chemical weathering in the eastern syntaxis. The total dissolved solids (TDS) flux from the this area is greater than 520 tons km−2 yr−1 and the silicate cation flux more than 34 tons km−2 yr−1. In total, chemical weathering in this area consumes 15.2 × 105 mol CO2 km−2 yr−1, which is twice the Brahmaputra average. These data show that 15-20% of the total CO2 consumption by silicate weathering in the Brahmaputra catchment is derived from only 4% of the total land area of the basin. Hot springs and evaporite weathering provide significant contributions to dissolved Na+ and Cl− fluxes throughout southern Tibet, comprising more than 50% of all Na+ in some stream systems. Carbonate weathering generates 80-90% of all dissolved Ca2+ and Mg2+ cations in much of the Yarlung Tsangpo catchment.  相似文献   

15.
The sequestration of silicon in soil clay-sized iron oxides may affect the terrestrial cycle of Si. Iron oxides indeed specifically adsorb aqueous monosilicic acid (H4SiO40), thereby influencing Si concentration in soil solution. Here we study the impact of H4SiO40 adsorption on the fractionation of Si isotopes in basaltic ash soils differing in weathering degree (from two weathering sequences, Cameroon), hence in clay and Fe-oxide contents, and evaluate the potential isotopic impact on dissolved Si in surrounding Cameroon rivers. Adsorption was measured in batch experiment series designed as function of time (0-72 h) and initial concentration (ic) of Si in solution (0.61-1.18 mM) at 20 °C, constant pH (5.5) and ionic strength (1 mM). After various soil-solution contact times, the δ30Si vs. NBS28 compositions were determined in selected solutions by MC-ICP-MS (Nu Plasma) in medium resolution, operating in dry plasma with Mg doping with an average precision of ±0.15‰ (±2σSEM). The quantitative adsorption of H4SiO40 by soil Fe-oxides left a solution depleted in light Si isotopes, which confirms previous study on synthetic Fe-oxides. Measured against its initial composition (δ30Si = +0.02 ± 0.07‰ (±2σSD)), the solutions were systematically enriched in 30Si reaching maximum δ30Si values ranging between +0.16‰ and +0.95‰ after 72 h contact time. The enrichment of the solution in heavy isotopes increased with increasing values of three parameters: soil weathering degree, iron oxide content, and proportion of short-range ordered Fe-oxide. The Si-isotopic signature of the solution was partly influenced by Si release, possibly through mineral dissolution and Si desorption from oxide surfaces, depending on soil type, highlighting the complex pattern of natural soils. Surrounding Cameroon rivers displayed a mean Si-isotopic signature of +1.19‰. Our data imply that in natural environments, H4SiO40 adsorption by soil clay-sized Fe-oxides at least partly impacts the Si-isotopic signature of the soil solution exported to water streams.  相似文献   

16.
The chemical weathering of primary Fe-bearing minerals, such as biotite and chlorite, is a key step of soil formation and an important nutrient source for the establishment of plant and microbial life. The understanding of the relevant processes and the associated Fe isotope fractionation is therefore of major importance for the further development of stable Fe isotopes as a tracer of the biogeochemical Fe cycle in terrestrial environments. We investigated the Fe mineral transformations and associated Fe isotope fractionation in a soil chronosequence of the Swiss Alps covering 150 years of soil formation on granite. For this purpose, we combined for the first time stable Fe isotope analyses with synchrotron-based Fe-EXAFS spectroscopy, which allowed us to interpret changes in Fe isotopic composition of bulk soils, size fractions, and chemically separated Fe pools over time in terms of weathering processes. Bulk soils and rocks exhibited constant isotopic compositions along the chronosequence, whereas soil Fe pools in grain size fractions spanned a range of 0.4‰ in δ56Fe. The clay fractions (<2 μm), in which newly formed Fe(III)-(hydr)oxides contributed up to 50% of the total Fe, were significantly enriched in light Fe isotopes, whereas the isotopic composition of silt and sand fractions, containing most of the soil Fe, remained in the range described by biotite/chlorite samples and bulk soils. Iron pools separated by a sequential extraction procedure covered a range of 0.8‰ in δ56Fe. For all soils the lightest isotopic composition was observed in a 1 M NH2OH-HCl-25% acetic acid extract, targeting poorly-crystalline Fe(III)-(hydr)oxides, compared with easily leachable Fe in primary phyllosilicates (0.5 M HCl extract) and Fe in residual silicates. The combination of the Fe isotope measurements with the speciation data obtained by Fe-EXAFS spectroscopy permitted to quantitatively relate the different isotope pools forming in the soils to the mineral weathering reactions which have taken place at the field site. A kinetic isotope effect during the Fe detachment from the phyllosilicates was identified as the dominant fractionation mechanism in young weathering environments, controlling not only the light isotope signature of secondary Fe(III)-(hydr)oxides but also significantly contributing to the isotope signature of plants. The present study further revealed that this kinetic fractionation effect can persist over considerable reaction advance during chemical weathering in field systems and is not only an initial transient phenomenon.  相似文献   

17.
Rare earth element (REE) distributions and Pb isotope compositions were explored in soils varying in age from ca. 0.4 to ?300 ka, developed on moraines in the Wind River Mountains, Wyoming. Soil extracts (0.6 M HCl) were used to examine the soil labile pool while the major element distribution in soil profiles was used to determine the extent of weathering at different soil depths. The results show that the chondrite-normalized REE patterns of the deepest bulk soil within each profile reflects the composition of the moraine till, except for the oldest soil. Up to ca. 12 ka, the soil extract fraction is enriched in light REE, indicating early release of light REE to the soil labile pool while that of the two oldest soils are relatively enriched in heavy REE. In the soil extracts the La/Sm ratio normalized to the deepest soil (LaD/SmD) decreases systematically with soil age. Similarly, the Eu-anomaly in the deepest soil from each profile (EuD/EuD*) decreases slightly with soil age in the three young soils; however, EuD/EuD* increases with soil age in the older soils. The systematic trends of these two ratios indicate the depletion of light REE in young soils and the enrichment of Eu and heavy REE in the older soils. Based on the Pb isotope ratios, the relative contribution of Pb to the soil labile pool via mineral weathering of U- or Th-rich phases was assessed for the different stages of weathering. The whole-soil profile 208Pb/204Pb ratio was found to decrease with soil age and with LaD/SmD, whereas it increased with the EuD/EuD* ratio. In each horizon, Pb isotope ratios (206Pb/204Pb, 207Pb/204Pb, and 208Pb/204Pb) ratio generally decrease with soil age. In order to overcome possible effects from parent material heterogeneity, the amount of radiogenic Pb as compared to the whole-soil composition was calculated and this was found to decrease systematically with soil age.  相似文献   

18.
Benthic nitrogen (N) cycling was investigated at six stations along a transect traversing the Peruvian oxygen minimum zone (OMZ) at 11°S. An extensive dataset including porewater concentration profiles and in situ benthic fluxes of nitrate (NO3−), nitrite (NO2−) and ammonium (NH4+) was used to constrain a 1-D reaction-transport model designed to simulate and interpret the measured data at each station. Simulated rates of nitrification, denitrification, anammox and dissimilatory nitrate reduction to ammonium (DNRA) by filamentous large sulfur bacteria (e.g. Beggiatoa and Thioploca) were highly variable throughout the OMZ yet clear trends were discernible. On the shelf and upper slope (80-260 m water depth) where extensive areas of bacterial mats were present, DNRA dominated total N turnover (?2.9 mmol N m−2 d−1) and accounted for ?65% of NO3− + NO2− uptake by the sediments from the bottom water. Nonetheless, these sediments did not represent a major sink for dissolved inorganic nitrogen (DIN = NO3− + NO2− + NH4+) since DNRA reduces NO3− and, potentially NO2−, to NH4+. Consequently, the shelf and upper slope sediments were recycling sites for DIN due to relatively low rates of denitrification and high rates of ammonium release from DNRA and ammonification of organic matter. This finding contrasts with the current opinion that sediments underlying OMZs are a strong sink for DIN. Only at greater water depths (300-1000 m) did the sediments become a net sink for DIN. Here, denitrification was the major process (?2 mmol N m−2 d−1) and removed 55-73% of NO3− and NO2− taken up by the sediments, with DNRA and anammox accounting for the remaining fraction. Anammox was of minor importance on the shelf and upper slope yet contributed up to 62% to total N2 production at the 1000 m station. The results indicate that the partitioning of oxidized N (NO3−, NO2−) into DNRA or denitrification is a key factor determining the role of marine sediments as DIN sinks or recycling sites. Consequently, high measured benthic uptake rates of oxidized N within OMZs do not necessarily indicate a loss of fixed N from the marine environment.  相似文献   

19.
The regulatory effect of salinity on nitrogen dynamics in estuarine sediments was investigated in the Randers Fjord estuary, Denmark, using sediment slurries and intact sediment cores and applying 15N-isotope techniques. Sediment was sampled at three representative stations varying in salinity, and all experiments were run at 0‰, 10‰, 20‰, and 30‰. The sediment NH4 + adsorption capacity decreased markedly at all stations when salinity was increased from 0‰ to 10‰; further increase showed little effect. In situ nitrification and denitrification also decreased with increasing salinities, with the most pronounced reduction of approximately 50% being observed when the salinity was raised from 0‰ to 10‰. The salinity-induced reduction in NH4 + adsorption capacity and stimulation of NH4 + efflux has previously been argued to cause a reduction in nitrification activity since the nitrifying bacteria become limited by NH4 + availability at higher salinities. However, using a potential nitrification assay where NH4 + was added in excess, it was demonstrated that potential nitrification activity also decreased with increasing salinity, indicating that the inhibitory salinity effect may also be a physiological effect on the microorganisms. This hypothesis was supported by the finding that denitrification based on NO3 − from the overlying water (Dw), which is independent of the nitrification process, and hence NH4 + availability, also decreased with increasing salinity. We conclude that changes in salinity have a significant effect on nitrogen dynamics in estuarine sediments, which must be considered when nitrogen transformations are measured and evaluated.  相似文献   

20.
Two sediment cores retrieved at the northern slope of Sakhalin Island, Sea of Okhotsk, were analyzed for biogenic opal, organic carbon, carbonate, sulfur, major element concentrations, mineral contents, and dissolved substances including nutrients, sulfate, methane, major cations, humic substances, and total alkalinity. Down-core trends in mineral abundance suggest that plagioclase feldspars and other reactive silicate phases (olivine, pyroxene, volcanic ash) are transformed into smectite in the methanogenic sediment sections. The element ratios Na/Al, Mg/Al, and Ca/Al in the solid phase decrease with sediment depth indicating a loss of mobile cations with depth and producing a significant down-core increase in the chemical index of alteration. Pore waters separated from the sediment cores are highly enriched in dissolved magnesium, total alkalinity, humic substances, and boron. The high contents of dissolved organic carbon in the deeper methanogenic sediment sections (50-150 mg dm−3) may promote the dissolution of silicate phases through complexation of Al3+ and other structure-building cations. A non-steady state transport-reaction model was developed and applied to evaluate the down-core trends observed in the solid and dissolved phases. Dissolved Mg and total alkalinity were used to track the in-situ rates of marine silicate weathering since thermodynamic equilibrium calculations showed that these tracers are not affected by ion exchange processes with sediment surfaces. The modeling showed that silicate weathering is limited to the deeper methanogenic sediment section whereas reverse weathering was the dominant process in the overlying surface sediments. Depth-integrated rates of marine silicate weathering in methanogenic sediments derived from the model (81.4-99.2 mmol CO2 m−2 year−1) are lower than the marine weathering rates calculated from the solid phase data (198-245 mmol CO2 m−2 year−1) suggesting a decrease in marine weathering over time. The production of CO2 through reverse weathering in surface sediments (4.22-15.0 mmol CO2 m−2 year−1) is about one order of magnitude smaller than the weathering-induced CO2 consumption in the underlying sediments. The evaluation of pore water data from other continental margin sites shows that silicate weathering is a common process in methanogenic sediments. The global rate of CO2 consumption through marine silicate weathering estimated here as 5-20 Tmol CO2 year−1 is as high as the global rate of continental silicate weathering.  相似文献   

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