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1.
Forest conditions in Europe have been monitored over 20 years jointly by the International Cooperative Programme on Assessment and Monitoring of Air Pollution Effects on Forests (ICP Forests) and the European Union (EU). Maps for mean bulk SO4, NO3 and NH4 deposition at around 400 intensive monitoring plots in the years 1999–2001, as well as time trends for the period 1996–2001, are presented. Mean bulk SO4 deposition at 169 plots mostly located in central Europe decreased from 7.4 to 5.8 kgS ha−1 a−1. Mean NH4 bulk deposition decreased from 6.2 to 5.3 kgN ha−1 a−1. Nitrate bulk deposition fluctuated around 5 kgN ha−1 a−1. On average, throughfall deposition was considerably higher than bulk deposition. Time trends for mean tree crown defoliation as an overall indicator for forest condition show a peak in the mid 1990s for most of the monitored main tree species and a recent increase for the years 2003 and 2004. Multivariate linear regression analyses show some significant relations between deposition and defoliation. These relations depend on the tree species and site characteristics. Effects of deposition are moderated by the influence of biotic stress factors such as insects and fungi and by abiotic stress factors, such as weather.  相似文献   

2.
Tissue N contents and δ15N signatures in 175 epilithic mosses were investigated from urban to rural sites in Guiyang (SW China) to determine atmospheric N deposition. Moss N contents (0.85–2.97%) showed a significant decrease from the urban area (mean = 2.24 ± 0.32%, 0–5 km) to the rural area (mean = 1.27 ± 0.13%, 20–25 km), indicating that the level of N deposition decreased away from the urban environment, while slightly higher N contents re-occurred at sites beyond 30 km, suggesting higher N deposition in more remote rural areas. Moss δ15N ranged from −12.50‰ to −1.39‰ and showed a clear bimodal distribution (−12‰ to −6‰ and −5‰ to −2‰), suggesting that there are two main sources for N deposition in the Guiyang area. More negative δ15N (mean = −8.87 ± 1.65‰) of urban mosses mainly indicated NH3 released from excretory wastes and sewage, while the less negative δ15N (from −3.83 ± 0.82‰ to −2.48 ± 0.95‰) of rural mosses were mainly influenced by agricultural NH3. With more negative values in the urban area than in the rural area, the pattern of moss δ15N variation in Guiyang was found to be opposite to cities where N deposition is dominated by NOx–N. Therefore, NHx–N is the dominant N form deposited in the Guiyang area, which is supported by higher NHx–N than NOx–N in local atmospheric deposition. From the data showing that moss is responding to NHx–N/NOx–N in deposition it can be further demonstrated that the variation of moss δ15N from the Guiyang urban to rural area was more likely controlled by the ratio of urban-NHx/agriculture-NHx than the ratio of NHx–N/NOx–N. The results of this study have extended knowledge of atmospheric N sources in city areas, showing that urban sewage discharge could be important in cities co-generic to Guiyang.  相似文献   

3.
Despite reduced anthropogenic deposition during the last decades, deposition sulphate may still play an important role in the biogeochemical cycles of S and many catchments may act as net sources of S that may remain for several decades. The aim of this study is to elucidate the temporal and spatial dynamics of both SO42− and δ34SSO4 in stream water from catchments with varying percentage of wetland and forest coverage and to determine their relative importance for catchment losses of S. Stream water samples were collected from 15 subcatchments ranging in size from 3 to 6780 ha, in a boreal stream network, northern Sweden. In forested catchments (<2% wetland cover) S-SO42− concentrations in stream water averaged 1.7 mg L−1 whereas in wetland dominated catchments (>30% wetland cover) the concentrations averaged 0.3 mg L−1. A significant negative relationship was observed between S-SO42− and percentage wetland coverage (r2 = 0.77, p < 0.001) and the annual export of stream water SO42− and wetland coverage (r2 = 0.76, p < 0.001). The percentage forest coverage was on the other hand positively related to stream water SO42− concentrations and the annual export of stream water SO42− (r2 = 0.77 and r2 = 0.79, respectively). The annual average δ34SSO4 value in wetland dominated streams was +7.6‰ and in streams of forested catchments +6.7‰. At spring flood the δ34SSO4 values decreased in all streams by 1‰ to 5‰. The δ34SSO4 values in all streams were higher than the δ34SSO4 value of +4.7‰ in precipitation (snow). The export of S ranged from 0.5 kg S ha−1 yr−1 (wetland headwater stream) to 3.8 kg S ha−1 yr−1 (forested headwater stream). With an average S deposition in open field of 1.3 kg S ha−1 yr−1 (2002-2006) the mass balance results in a net export of S from all catchments, except in catchments with >30% wetland. The high temporal and spatial resolution of this study demonstrates that the reducing environments of wetlands play a key role for the biogeochemistry of S in boreal landscapes and are net sinks of S. Forested areas, on the other hand were net sources of S.  相似文献   

4.
In a comprehensive study, we compared depositional conditions, organic matter (OM) composition, and organic carbon turnover in sediments from two different depositional systems along the Chilean continental margin: at ∼23° S off Antofagasta and at ∼36° S off Concepción. Both sites lie within the Chilean coastal upwelling system and have an extended oxygen minimum zone in the water column. However, the northern site (23° S) borders the Atacama Desert, while the southern site (36° S) has a humid hinterland. Eight surface sediment cores (up to 30 cm long) from water depths of 126-1350 m were investigated for excess 210Pb (210Pbxs) activity, total organic and total inorganic carbon concentrations (TOC and TIC, respectively), C/N-ratios, organic carbon isotopic compositions (δ13C), chlorin concentrations, Chlorin Indices (CI), and sulfate reduction rates (SRR). Sediment accumulation rates obtained from 210Pb-analysis were similar in both regions (0.04-0.15 cm yr−1 at 23° S, 0.10-0.19 cm yr−1 at 36° S), although total 210Pbxs fluxes indicated that the vertical particle flux was higher at 36° S than at 23° S. We propose that sediment focusing in isolated deposition centers led to high sediment accumulation rates at 23° S. Furthermore, there were no indications for sediment mixing at 23° S, while bioturbation was intense at 36° S. δ13C-values (−24.5‰ to −20.1‰ vs. VPDB) and C/N-ratios (molar, 8.6-12.8) were characteristic of a predominantly marine origin of the sedimentary OM in both investigated areas. The extent of OM alteration in the water column was partly reflected in the surface sediments as chlorin concentrations decreased and C/N-ratios and CI increased with increasing water depth of the sampling site. SRR were lower at 23° S (areal SRR 0.12-0.60 mmol m−2 d−1) than at 36° S (areal SRR 0.82-1.18 mmol m−2 d−1), which was partly due to the greater water depth of most of the sediments investigated in the northern region and consistent with a lower quality of the sedimentary OM at 23° S. Reaction rate constants for TOC degradation that were obtained from measured SRR (kSRR; 0.0004-0.0022 yr−1) showed a good correspondence to kTOC that were derived from the depth profiles of TOC (0.0003-0.0014 yr−1). Both, kSRR and kTOC, reflect differences in OM composition. At 36° S they were related to the degradation state of bulk OM (represented by C/N-ratios), whereas near 23° S they were related to the freshness of a small fraction of labile OM (represented by CI). Our study shows that although rates of organic carbon accumulation were similar in both investigated sites, the extent and kinetics of organic carbon degradation were closely linked to differing depositional conditions.  相似文献   

5.
The distribution and speciation of mercury (Hg) in the water column, the inputs (wet deposition and tributaries) and the outputs (atmospheric evasion and outlet) of an artificial partially anoxic tropical lake (Petit-Saut reservoir, French Guiana) were investigated on a seasonal basis in order to appraise the cycling and transformations of this metal. The total mercury (HgT) concentrations in the oxygenated epilimnetic waters averaged 5 ± 3 pmol L−1 in the unfiltered samples (HgTUNF) and 4 ± 2 pmol L−1 in the dissolved (HgTD) phase (<0.45 μm). On average, the monomethylmercury (MMHg) constituted 8%, 40% and 18% of the HgT in the dissolved phase, the particulate suspended matter and in the unfiltered samples, respectively. Covariant elevated concentrations of particulate MMHg and chlorophyll a in the epilimnion suggest that phytoplankton is an active component for the MMHg transfer in the lake. In the anoxic hypolimnion the HgTUNF averages 13 ± 6 pmol L−1 and the HgTD 8 ± 4 pmol L−1. The averages of MMHgP and MMHgD in hypolimnetic waters were two and three times the corresponding values of the epilimnion, 170 ± 90 pmol g−1 and 0.9 ± 0.5 pmol L−1, respectively. In the long dry and wet seasons, at the flooded forest and upstream dam sampling stations, the vertical profiles of MMHgD concentrations accounted for two distinct maxima: one just below the oxycline and the other near the benthic interface. Direct wet atmospheric deposition accounted for 14 moles yr−1 HgTUNF, with 0.7 moles yr−1 as MMHgUNF, while circa 76 moles yr−1 of HgTUNF, with 4.7 moles yr−1 as MMHgUNF, coming from tributaries. Circa 78 moles (∼17% as MMHg) are annually exported through the dam, while 23 moles yr−1 of Hg0 evolve in the atmosphere. A mass balance calculation suggests that the endogenic production of MMHgUNF attained 8.1 moles yr−1, corresponding to a methylation rate of 0.06% d−1. As a result, the Petit-Saut reservoir is a large man-made reactor that has extensively altered mercury speciation in favor of methylated species.  相似文献   

6.
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   

7.
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8.
Water samples from the Fraser, Skeena and Nass River basins of the Canadian Cordillera were analyzed for dissolved major element concentrations (HCO3−, SO42−, Cl−, Ca2+, Mg2+, K+, Na+), δ13C of dissolved inorganic carbon (δ13CDIC), and δ34S of dissolved sulfate (δ34SSO4) to quantify chemical weathering rates and exchanges of CO2 between the atmosphere, hydrosphere, and lithosphere. Weathering rates of silicates and carbonates were determined from major element mass balance. Combining the major element mass balance with δ34SSO4 (−8.9 to 14.1‰CDT) indicates sulfide oxidation (sulfuric acid production) and subsequent weathering of carbonate and to a lesser degree silicate minerals are important processes in the study area. We determine that on average, 81% of the riverine sulfate can be attributed to sulfide oxidation in the Cordilleran rivers, and that 25% of the total weathering cation flux can be attributed to carbonate and silicate dissolution by sulfuric acid. This result is validated by δ13CDIC values (−9.8 to −3.7‰ VPDB) which represents a mixture of DIC produced by the following weathering pathways: (i) carbonate dissolution by carbonic acid (−8.25‰) > (ii) silicate dissolution by carbonic acid (−17‰) ≈ (iii) carbonate dissolution by sulfuric acid derived from the oxidation of sulfides (coupled sulfide-carbonate weathering) (+0.5‰).δ34SSO4 is negatively correlated with δ13CDIC in the Cordilleran rivers, which further supports the hypothesis that sulfuric acid produced by sulfide oxidation is primarily neutralized by carbonates, and that sulfide-carbonate weathering impacts the δ13CDIC of rivers. The negative correlation between δ34SSO4 and δ13CDIC is not observed in the Ottawa and St. Lawrence River basins. This suggests other factors such as landscape age (governed by tectonic uplift) and bedrock geology are important controls on regional sulfide oxidation rates, and therefore also on the magnitude of sulfide-carbonate weathering—i.e., it is more significant in tectonically active areas.Calculated DIC fluxes due to Ca and Mg silicate weathering by carbonic acid (38.3 × 103 mol C · km−2 · yr−1) are similar in magnitude to DIC fluxes due to sulfide-carbonate weathering (18.5 × 103 mol C · km−2 · yr−1). While Ca and Mg silicate weathering facilitates a transfer of atmospheric CO2 to carbonate rocks, sulfide-carbonate weathering can liberate CO2 from carbonate rocks to the atmosphere when sulfide oxidation exceeds sulfide deposition. This implies that in the Canadian Cordillera, sulfide-carbonate weathering can offset up to 48% of the current CO2 drawdown by silicate weathering in the region.  相似文献   

9.
Eight DSDP/ODP cores were analyzed for major ion concentrations and δ37Cl values of water-soluble chloride (δ37ClWSC) and structurally bound chloride (δ37ClSBC) in serpentinized ultramafic rocks. This diverse set of cores spans a wide range in age, temperature of serpentinization, tectonic setting, and geographic location of drilled serpentinized oceanic crust. Three of the cores were sampled at closely spaced intervals to investigate downhole variation in Cl concentration and chlorine isotope composition.The average total Cl content of all 86 samples is 0.26 ± 0.16 wt.% (0.19 ± 0.10 wt.% as water-soluble Cl (XWSC) and 0.09 ± 0.09 wt.% as structurally bound Cl (XSBC)). Structurally bound Cl concentration nearly doubles with depth in all cores; there is no consistent trend in water-soluble Cl content among the cores. Chlorine isotope fractionation between the structurally bound Cl− site and the water-soluble Cl− site varies from − 1.08‰ to + 1.16‰, averaging to + 0.21‰. Samples with negative fractionations may be related to reequilibration of the water-soluble chloride with seawater post-serpentinite formation. Six of the cores have positive bulk δ37Cl values (+ 0.05‰ to + 0.36‰); the other two cores (173-1068A (Leg-Hole) and 84-570) have negative bulk δ37Cl values (− 1.26‰ and − 0.54‰). The cores with negative δ37Cl values also have variable Cl− / SO42 ratios, in contrast to all other cores. The isotopically positive cores (153-920D and 147-895E) show no isotopic variation with depth; the isotopically negative core (173-1068A) decreases by ∼1‰ with depth for both the water-soluble and structurally bound Cl fractions.Non-zero bulk δ37Cl values indicate Cl in serpentinites was incorporated during original hydration and is not an artifact of seawater infiltration during drilling. Cores with positive δ37Cl values are most likely explained by open system fractionation during hydrothermal alteration, with preferential incorporation of 37Cl from seawater into the serpentinite and loss of residual light Cl back to the ocean. Fluid / rock ratios were probably low as evidenced by the presence of water-soluble salts. The two isotopically negative cores are characterized by a thick overlying sedimentary package that was in place prior to serpentinization. We believe the low δ37Cl values of these cores are a result of hydration of ultramafic rock by infiltrating aqueous pore fluids from the overlying sediments. The resulting serpentinites inherit the characteristic negative δ37Cl values of the pore waters. Chlorine stable isotopes can be used to identify the source of the serpentinizing fluid and ultimately discern chemical and tectonic processes involved in serpentinization.  相似文献   

10.
The S and O isotopic composition of dissolved SO4, used as a tracer for SO4 sources, was applied to the water of the Llobregat River system (NE Spain). The survey was carried out at 30 sites where surface water was sampled on a monthly basis over a period of 2a. The concentration of dissolved SO4 varied from 20 to 1575 mg L−1. Sulphur isotopic compositions clustered in two populations: one – 93% of the samples – had positive values with a mode of +9‰; the other had negative values and a mode of −5‰. Data for δ18OSO4 showed a mean value of +11‰, with no bi-modal distribution, though lower values of δ18O corresponded to samples with negative δ34S. These values can not be explained solely by the contribution of bedrock SO4 sources: that is, sulphide oxidation and the weathering of outcrops of sulphates, though numerous chemical sediments exist in the basin. Even in a river with a high concentration of natural sources of dissolved SO4, such as the Llobregat River, the δ34S values suggest that dissolved SO4 is controlled by a complex mix of both natural and anthropogenic sources. The main anthropogenic sources in this basin are fertilizers, sewage, potash mine effluent and power plant emissions. Detailed river water sampling, together with the chemical and isotopic characterisation of the main anthropogenic inputs, allowed determination of the influence of redox processes, as well as identification of the contribution of natural and anthropogenic SO4 sources and detection of spatial variations and seasonal changes among these sources. For instance, in the Llobregat River the input of fertilisers is well marked seasonally. Minimum values of δ34S are reported during fertilization periods – from January to March – indicating a higher contribution of this source. The dual isotope approach, δ34S and δ18O, is useful to better constrain the sources of SO4. Moreover, in small-scale studies, where the inputs are well known and limited, the mixing models can be enhanced and the contribution of the different sources can be quantified to some extent.  相似文献   

11.
In the Tivoli Plain (Rome, Central Italy) the interaction between shallow and deep groundwater flow systems enhanced by groundwater extraction has been investigated using isotopic and chemical tracers. A conceptual model of the groundwater flowpaths has been developed and verified by geochemical modeling. A combined hydrogeochemical and isotopic investigation using ion relationships such as DIC/Cl−, Ca/(Ca + Mg)/SO4/(SO4 + HCO3), and environmental isotopes (δ18O, δ2H, 87Sr/86Sr, δ34S and δ13C) was carried out in order to determine the sources of recharge of the aquifer, the origin of solutes and the mixing processes in groundwater of Tivoli Plain. Multivariate statistical methods such as principal component analysis and Cluster analyses have confirmed the existence of different geochemical facies and the role of mixing in the chemical composition of the groundwater.  相似文献   

12.
Evaporite outcrops are rare in the Basque Cantabrian basin due to a rainy climate, but saline springs with total dissolved solids ranging from 0.8 to 260 g/L are common and have long been used to supply spas and salterns. New and existing hydrochemistry of saline springs are used to provide additional insight on the origin and underground extent of their poorly known source evaporites. Saline water hydrochemistry is related to dissolution of halite and gypsum from two evaporitic successions (Triassic “Keuper” and Lower Cretaceous “Wealden”), as supported by rock samples from outcrops and oil exploration drill cuttings. The δ34S value of gypsum in the Keuper evaporites and sulfate in the springs is δ34SSO4 = 14.06 ± 1.07‰ and δ18OSO4 = 13.41 ± 1.44‰, and the relationship between Cl/Br ratio of halite and water shows that waters have dissolved halite with Br content between 124 and 288 ppm. The δ34S value of gypsum in the Wealden evaporites and sulfate in the springs is δ34SSO4 = 19.66 ± 1.76‰, δ18OSO4 = 14.93 ± 2.35‰, and the relationship between Cl/Br ratio of halite and water shows that waters have dissolved halite with Br content between 15 and 160 ppm. Wealden evaporites formed in a continental setting after the dissolution of Keuper salt. Gypsum δ34SSO4 and δ18OSO4 modification from Keuper to Wealden evaporites was due mainly to bacterial SO4 reduction in an anoxic, organic matter-rich environment. Saline springs with Wealden δ34SSO4 values are present in a 70 × 20 km wide area. Saline water temperatures, their δ2HH2O and δ18OH2O values, and the geological structure defines a hydrogeological model, where meteoric water recharges at heights up to 620 m above spring levels and circulates down to 720 m below them, thereby constraining the height range of evaporite dissolution. Groundwater flow towards saline springs is driven by gravity and buoyancy forces constrained by a thrust and fault network.  相似文献   

13.
The speciation of aqueous dissolved sulfur was determined in hydrothermal waters in Iceland. The waters sampled included hot springs, acid-sulfate pools and mud pots, sub-boiling well discharges and two-phase wells. The water temperatures ranged from 4 to 210 °C, the pHT was between 2.20 and 9.30 at the discharge temperature and the SO4 and Cl concentrations were 0.020-52.7 and <0.01-10.0 mmol kg−1, respectively. The analyses were carried out on-site within ∼10 min of sampling using ion chromatography (IC) for sulfate (SO42−), thiosulfate (S2O32−) and polythionates (SxO62−) and titration and/or colorimetry for total dissolved sulfide (S2−). Sulfite (SO32−) could also be determined in a few cases using IC. Alternatively, for few samples in remote locations the sulfur oxyanions were stabilized on a resin on site following elution and analysis by IC in the laboratory. Dissolved sulfate and with few exceptions also S2− were detected in all samples with concentrations of 0.02-52.7 mmol kg−1 and <1-4100 μmol kg−1, respectively. Thiosulfate was detected in 49 samples of the 73 analyzed with concentrations in the range of <1-394 μmol kg−1 (S-equivalents). Sulfite was detected in few samples with concentrations in the range of <1-3 μmol kg−1. Thiosulfate and SO32− were not detected in <100 °C well waters and S2O32− was observed only at low concentrations (<1-8 μmol kg−1) in ∼200 °C well waters. In alkaline and neutral pH hot springs, S2O32− was present in significant concentrations sometimes corresponding to up to 23% of total dissolved sulfur (STOT). In steam-heated acid-sulfate waters, S2O32− was not a significant sulfur species. The results demonstrate that S2O32− and SO32− do not occur in the deeper parts of <150 °C hydrothermal systems and only in trace concentrations in ∼200-300 °C systems. Upon ascent to the surface and mixing with oxygenated ground and surface waters and/or dissolution of atmospheric O2, S2− is degassed and oxidized to SO32− and S2O32− and eventually to SO42− at pH >8. In near-neutral hydrothermal waters the oxidation of S2− and the interaction of S2− and S0 resulting in the formation of Sx2− are considered important. At lower pH values the reactions seemed to proceed relatively rapidly to SO42− and the sulfur chemistry of acid-sulfate pools was dominated by SO42−, which corresponded to >99% of STOT. The results suggest that the aqueous speciation of sulfur in natural hydrothermal waters is dynamic and both kinetically and source-controlled and cannot be estimated from thermodynamic speciation calculations.  相似文献   

14.
δ13C values of dissolved inorganic C (DIC), dissolved organic C (DOC), and particulate organic C (POC) together with δ18O and δ2H values of water, δ34S values of dissolved SO4, and major ion concentrations were measured in the Murray River and its tributaries between November 2005 and April 2007 to constrain the origins and behaviour of riverine C. δ13CDIC values in the Murray River vary between −9.5 and −4.7‰ with a range of <3‰ within any sampling round. δ13CDIC values of the tributaries are −11.0‰ to −5.1‰. DIC concentrations of the Murray River increase from ∼25 mg/L in the middle and upper reaches of the river to 45–55 mg/L in the lower reaches. However, the mass ratio of DIC as a proportion of the total dissolved solids (TDS) decreases from ∼0.6–0.7 in the headwaters to ∼0.2–0.3 in the lower reaches of the river, with similar downstream changes in DIC/Cl ratios. This precludes simple evaporative concentration of DIC and is interpreted as the river evading CO2; this interpretation is consistent with pCO2 values that are in the range 550–11,200 ppm volume (ppmv), which are far higher than those in equilibrium with the atmosphere (∼360 ppmv). The δ13CDIC values are similar to those that would be produced by the weathering of marine limestone (δ13C ∼ 0‰). However, the lack of marine limestones cropping out in the Murray–Darling Basin and the relatively uniform δ13CDIC values of the Murray River (even in upland reaches where the dominant rock types are metamorphosed silicates and granites) make this unlikely. Rather the high pCO2 values and δ13CDIC values are best explained by a combination of mineralisation of low δ13C organic C and evasion to the atmosphere. The rate of these two processes may attain near steady state and control both DIC concentrations and δ13C values.  相似文献   

15.
We measured δD values of long chain n-alkanes isolated from 30 surface soil samples along two elevation transects on the Tibetan Plateau differing in precipitation regime and water source. The East Asian Monsoon precipitation dominates the wetter regime on the eastern slope (from 1230 to 4300 m) of Gongga Shan on the eastern Tibetan Plateau. Precipitation from the Polar Westerlies dominates the drier region on the slope from 1900 to 5000 m in the West Kunlun Shan on the northwestern Tibetan Plateau. The decrease in δD value with elevation in the wetter region greatly exceeded that in drier region by, −1.9 ± 0.1‰/100 m and −1.4 ± 1.0‰/100 m respectively. The apparent fractionation between leaf wax and precipitation εwax-p values in the wetter region (ca. −164‰) were more negative than those in drier region (ca. −125‰ above 3200 m).We also measured δD values in leaves of six common living trees (values from −287‰ to −193‰) from Gongga Shan, ranging from about 2900-4200 m. The abundance-weighted average values of the n-alkanes (δDwax) show a strong reverse correlation with sample source elevation (R2 0.78 for soils from Gongga Shan; R2 0.85 for soils from West Kunlun Shan above 3200 m), suggesting that n-alkane δDwax faithfully records the precipitation δD and that the isotopic altitude effect of precipitation controls δDwax altitudinal gradients in the mountains. The data show a fairly strong monotonic dependency of n-alkane δD values on elevation for the eastern Plateau, but a complex relationship between n-alkane δD values and elevation for the northwestern Plateau. The δDwax values at sites below 3200 m from the Kunlun Shan area exhibit an unexpected positive correlation with elevation. The study confirms the potential for using sediment δDwax values to reconstruct paleo-elevation in wetter regions, but suggests caution in applying the approach to dry regions. Our results also show it is essential to consider the intricacy of the pattern of atmospheric circulation and water sources and their influence on the lapse rate of δD values with elevation.  相似文献   

16.
Climate change in the SW USA is likely to involve drier conditions and higher surface temperatures. In order to better understand the evolution of water chemistry and the sources of aqueous SO4 in these semi-arid settings, chemical and S isotope compositions were determined of springs, groundwater, and bedrock associated with a Permian fractured carbonate aquifer located in the southern Sacramento Mountains, New Mexico, USA. The results suggest that the evolution of water chemistry in the semi-arid carbonate aquifer is mainly controlled by dedolomitization of bedrock, which was magnified by increasing temperature and increasing dissolution of gypsum/anhydrite along the groundwater flow path. The δ34S of dissolved SO4 in spring and groundwater samples varied from +9.0‰ to +12.8‰, reflecting the mixing of SO4 from the dissolution of Permian gypsum/anhydrite (+12.3‰ to +13.4‰) and oxidation of sulfide minerals (−24.5‰ to −4.2‰). According to S isotope mass balance constraints, the contribution of sulfide-derived SO4 was considerable in the High Mountain recharge areas, accounting for up to ∼10% of the total SO4 load. However, sulfide weathering decreased in importance in the lower reaches of the watershed. A smaller SO4 input of ∼2–4% was contributed by atmospheric wet deposition. This study implies that the δ34S variation of SO4 in semi-arid environments can be complex, but that S isotopes can be used to distinguish among the different sources of weathering. Here it was found that H2SO4 dissolution due to sulfide oxidation contributes up to 5% of the total carbonate weathering budget, while most of the SO4 is released from bedrock sources during dedolomitization.  相似文献   

17.
Atmospheric carbon dioxide is widely studied using records of CO2 mixing ratio, δ13C and δ18O. However, the number and variability of sources and sinks prevents these alone from uniquely defining the budget. Carbon dioxide having a mass of 47 u (principally 13C18O16O) provides an additional constraint. In particular, the mass 47 anomaly (Δ47) can distinguish between CO2 produced by high temperature combustion processes vs. low temperature respiratory processes. Δ47 is defined as the abundance of mass 47 isotopologues in excess of that expected for a random distribution of isotopes, where random distribution means that the abundance of an isotopologue is the product of abundances of the isotopes it is composed of and is calculated based on the measured 13C and 18O values. In this study, we estimate the δ13C (vs. VPDB), δ18O (vs. VSMOW), δ47, and Δ47 values of CO2 from car exhaust and from human breath, by constructing ‘Keeling plots’ using samples that are mixtures of ambient air and CO2 from these sources. δ47 is defined as , where is the R47 value for a hypothetical CO2 whose δ13CVPDB = 0, δ18OVSMOW = 0, and Δ47 = 0. Ambient air in Pasadena, CA, where this study was conducted, varied in [CO2] from 383 to 404 μmol mol−1, in δ13C and δ18O from −9.2 to −10.2‰ and from 40.6 to 41.9‰, respectively, in δ47 from 32.5 to 33.9‰, and in Δ47 from 0.73 to 0.96‰. Air sampled at varying distances from a car exhaust pipe was enriched in a combustion source having a composition, as determined by a ‘Keeling plot’ intercept, of −24.4 ± 0.2‰ for δ13C (similar to the δ13C of local gasoline), δ18O of 29.9 ± 0.4‰, δ47 of 6.6 ± 0.6‰, and Δ47 of 0.41 ± 0.03‰. Both δ18O and Δ47 values of the car exhaust end-member are consistent with that expected for thermodynamic equilibrium at∼200 °C between CO2 and water generated by combustion of gasoline-air mixtures. Samples of CO2 from human breath were found to have δ13C and δ18O values broadly similar to those of car exhaust-air mixtures, −22.3 ± 0.2 and 34.3 ± 0.3‰, respectively, and δ47 of 13.4 ± 0.4‰. Δ47 in human breath was 0.76  ± 0.03‰, similar to that of ambient Pasadena air and higher than that of the car exhaust signature.  相似文献   

18.
Numerous studies of weathering fluxes have been carried out on major world rivers during the last decade, to estimate CO2 consumption rates, landscape evolution and global erosion rates. For obvious logistical reasons, most of these studies were based on large scale investigations carried out on short timescales. By comparison, much less effort has been devoted to long term monitoring, as a means to verify the temporal variability of the average characteristics, their trends, and the representativeness of short-term investigations. Here we report the results of a three-year survey (November 2000 to December 2003) of the major and trace element composition of dissolved and suspended matter in the lower Rhone River (France), the largest river of the Mediterranean area. Subsurface water samples were collected in Arles, about 48 km upstream of the estuary, twice a month routinely, and at higher frequency during flood events.During each flood event, the suspended particulate matter (SPM) show the usual trend of clockwise hysteresis with higher SPM concentrations on the rising limb of the flood than at the same discharge on the falling limb. We show that the annual average SPM flux of the Rhone River to the Mediterranean Sea (7.3 ± 0.6 × 106 tons yr−1) was largely controlled by the flood events (83% of the solid discharge occurred in less than 12% of the time), and that the precision on the total output flux depends strongly on the precise monitoring of SPM variations during the floods.The chemical composition of water and SPM are characterized by the predominance of Ca2+ due to the abundance of carbonate rocks in the Rhone watershed. Chemical budgets have been calculated to derive the contributions of atmospheric deposition, carbonate, silicate and evaporite weathering, and anthropogenic inputs. The chemical weathering rate of carbonates is estimated to be 89 ± 5 t km−2 yr−1 compared to 14.4 ± 3 t km−2 yr−1 from silicates. By contrast, the physical erosion rate of silicates is about 51 t km−2 yr−1 against 19 t km−2 yr−1 for carbonates.The steady-state model of Gaillardet et al. (1995) has been applied to the chemical composition of dissolved and solid products. The results show that the Rhone River currently exports much less material than produced at steady-state by weathering in its watershed. The sediment flux inferred from the steady-state calculation (21-56 × 106 t yr−1) is on the same order as that estimated in literature for the 19th and the beginning of the 20th centuries. This imbalance may suggest that the Rhone is under a transient erosion regime following climate change (i.e. significant decrease of the flooding frequency since the beginning of the 19th century). On the other hand, the imbalance may also be due to the trapping of alluvion by the numerous dams on the river and its tributaries.Our data corroborate with previous studies that suggest a strong coupling between chemical and physical erosion fluxes, during the hydrological seasonal cycle of the Rhone River. The correlation between physical and chemical transport rates is, however, clearly different from that reported for global annual averages in large world rivers.  相似文献   

19.
Lithological, chemical, and stable isotope data are used to characterize lacustrine tufas dating back to pre-late Miocene and later unknown times, capping different surfaces of a Tertiary carbonate (Sinn el-Kedab) plateau in Dungul region in the currently hyperarid south-western Egypt. These deposits are composed mostly of calcium carbonate, some magnesium carbonate and clastic particles plus minor amounts of organic matter. They have a wide range of (Mg/Ca)molar ratios, from 0.03 to 0.3. The bulk-tufa carbonate has characteristic isotope compositions: (δ13Cmean = −2.49 ± 0.99‰; δ18Omean = −9.43 ± 1.40‰). The δ13C values are consistent with a small input from C4 vegetation or thinner soils in the recharge area of the tufa-depositing systems. The δ18O values are typical of fresh water carbonates. Covariation between δ13C and δ18O values probably is a reflection of climatic conditions such as aridity. The tufas studied are isotopically similar to the underlying diagenetic marine chalks, marls and limestones (δ13Cmean = −2.06 ± 0.84‰; δ18Omean = −10.06 ± 1.39‰). The similarity has been attributed to common meteoric water signatures. This raises large uncertainties in using tufas (Mg/Ca)molar, δ13C and δ18O records as proxies of paleoclimatic change and suggests that intrinsic compositional differences in material sources within the plateau may mask climatic changes in the records.  相似文献   

20.
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   

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