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1.
Geochemistry of soil, soil water, and soil gas was characterized in representative soil profiles of three Michigan watersheds. Because of differences in source regions, parent materials in the Upper Peninsula of Michigan (the Tahquamenon watershed) contain only silicates, while those in the Lower Peninsula (the Cheboygan and the Huron watersheds) have significant mixtures of silicate and carbonate minerals. These differences in soil mineralogy and climate conditions permit us to examine controls on carbonate and silicate mineral weathering rates and to better define the importance of silicate versus carbonate dissolution in the early stage of soil-water cation acquisition.Soil waters of the Tahquamenon watershed are the most dilute; solutes reflect amphibole and plagioclase dissolution along with significant contributions from atmospheric precipitation sources. Soil waters in the Cheboygan and the Huron watersheds begin their evolution as relatively dilute solutions dominated by silicate weathering in shallow carbonate-free soil horizons. Here, silicate dissolution is rapid and reaction rates dominantly are controlled by mineral abundances. In the deeper soil horizons, silicate dissolution slows down and soil-water chemistry is dominated by calcite and dolomite weathering, where solutions reach equilibrium with carbonate minerals within the soil profile. Thus, carbonate weathering intensities are dominantly controlled by annual precipitation, temperature and soil pCO2. Results of a conceptual model support these field observations, implying that dolomite and calcite are dissolving at a similar rate, and further dissolution of more soluble dolomite after calcite equilibrium produces higher dissolved inorganic carbon concentrations and a Mg2+/Ca2+ ratio of 0.4.Mass balance calculations show that overall, silicate minerals and atmospheric inputs generally contribute <10% of Ca2+ and Mg2+ in natural waters. Dolomite dissolution appears to be a major process, rivaling calcite dissolution as a control on divalent cation and inorganic carbon contents of soil waters. Furthermore, the fraction of Mg2+ derived from silicate mineral weathering is much smaller than most of the values previously estimated from riverine chemistry.  相似文献   

2.
Water samples from precipitation, glacier melt, snow melt, glacial lake, streams and karst springs were collected across SE of Kashmir Valley, to understand the hydrogeochemical processes governing the evolution of the water in a natural and non-industrial area of western Himalayas. The time series data on solute chemistry suggest that the hydrochemical processes controlling the chemistry of spring waters is more complex than the surface water. This is attributed to more time available for infiltrating water to interact with the diverse host lithology. Total dissolved solids (TDS), in general, increases with decrease in altitude. However, high TDS of some streams at higher altitudes and low TDS of some springs at lower altitudes indicated contribution of high TDS waters from glacial lakes and low TDS waters from streams, respectively. The results show that some karst springs are recharged by surface water; Achabalnag by the Bringi stream and Andernag and Martandnag by the Liddar stream. Calcite dissolution, dedolomitization and silicate weathering were found to be the main processes controlling the chemistry of the spring waters and calcite dissolution as the dominant process in controlling the chemistry of the surface waters. The spring waters were undersaturated with respect to calcite and dolomite in most of the seasons except in November, which is attributed to the replenishment of the CO2 by recharging waters during most of the seasons.  相似文献   

3.
Dolomitization is a dissolution–re‐precipitation process which proceeds via micrometre‐scale interface reaction horizons. However, the effect of this fundamental local medium of replacement process on precipitated dolomite crystals is rarely investigated. For this purpose, dolomite samples of Ordovician Boat Harbour Formation carbonates (Newfoundland, Canada) from Main Brook and Daniel's Harbour (about 150 km apart) were studied. The investigation used high‐resolution approaches to carry out imaging and elemental analyses of individual dolomite crystals, including scanning electron microscopy, scanning electron microscopy‐based cathodoluminescence, secondary ion mass spectrometry and electron microprobe analysis. The purpose was to better understand geochemical variations across the crystal traverses and their association with dolomite replacement processes and conditions. The scanning electron microscopy‐based cathodoluminescence‐zoning character reveals three major crystal facies. Distinctly (planar boundaries) zoned core and indistinctly zoned core are zoned dolomite crystal facies in burial dolomite from Main Brook. Relatively unzoned crystal facies was identified in that of Daniel's Harbour. Compositionally zoned dolomite crystals are characterized by decreasing Sr, Na, Y and ∑REE but increasing Mn and Fe from core to rim sections. ‘Core to rim’ zoning was not found for major (Mg and Ca) elements. The zoning exhibited by the replacive dolomite crystals is interpreted to be, principally, a result of limited exchange between solutes of the bulk pore fluid and those of dissolving precursor marine carbonate. In tandem with petrographic features, the systematic compositional zoning character demonstrates that the effectiveness of the dolomitization process grades from indistinctly zoned core to relatively unzoned crystal facies via interface reaction horizons. Homogenization of major elements of core and rim sections, seen in distinctly zoned core crystal facies and to a much greater extent in relatively unzoned crystal facies, via a secondary reaction interface, is the first recognized stage of the ‘maturation process’ followed by homogenization of the trace elements seen largely in relatively unzoned crystal facies.  相似文献   

4.
In the light of progressive depletion of groundwater reservoir and water quality deterioration of the Independence aquifer, an investigation on chemical data of dissolved major and minor constituents in 246 recent groundwater samples was performed. The main objective was the detection of processes responsible for the geochemical evolution and mineralization throughout the area. Multivariate techniques revealed different sources of solutes (a) dissolution of calcium and magnesium carbonate minerals, (b) weathering of acid volcanic minerals, (c) alteration of manganese containing alkaline silicates, (d) leaching of halite deposits of meteoric origin, (e) contamination from agricultural and urban wastewaters, and (f) evaporative effects due to intensive irrigation. Although nitrate contamination is associated with pollution from intensive cultivated areas, natural contamination plays an important role in the study area. The investigation reveals that weathering of acid volcanic rocks (rhyolite) and oxidation of arsenic bearing sulfide minerals are the responsible processes for high fluorine (up to 16 mg/l) and arsenic (up to 0.12 mg/l) contents, respectively, exceeding the Mexican maximum admissible concentration for drinking water. Except for kaolinite, all recharge processes are dissolution oriented (CO2, calcite, dolomite, K-feldspar, plagioclase). Silicate precipitation (amorphous silica and chalcedony) is of growing importance in discharge zones. Cation exchange is not an important issue in the whole study area.  相似文献   

5.
In the Variscan Western Tatra granites hybridization phenomena such as mixing and mingling can be observed at the contact of mafic precursors of dioritic composition and more felsic granitic host rocks. The textural evidence of hybridization include: plagioclase?CK-feldspar?Csphene ocelli, hornblende- and biotite-rimmed quartz ocelli, plagioclase with Ca-rich spike zonation, inversely zoned K-feldspar crystals, mafic clots, poikilitic plagioclase and quartz crystals, mixed apatite morphologies, zoned K-feldspar phenocrysts. The apparent pressure range of the magma hybridization event was calculated at 6.1?kbar to 4.6?kbar, while the temperature, calculated by independent methods, is in the range of 810°C?770°C. U-Pb age data of the hybrid rocks were obtained by in-situ LA-MC-ICP-MS analysis of zircon. The oscillatory zoned zircon crystals yield a concordia age of 368?±?8?Ma (MSWD?=?1.1), interpreted as the age of magma hybridization and timing of formation of the magmatic precursors. It is the oldest Variscan magmatic event in that part of the Tatra Mountains.  相似文献   

6.
Amphiboles represent a crucial phase of the ultra-high-pressure (UHP) metamorphic rocks as their solid solution behavior reflects both bulk compositional and P–T changes. Three different types of amphibole have been reported from the UHP metamafic rocks of the Tso Morari Crystalline Complex, NW Himalayas: Na-rich (glaucophane); Na–Ca-rich (barroisite, taramite, winchite) and Ca-rich (tremolite, magnesio-hornblende, pargasite). The Na-amphibole is presented as a core of the zoned amphibole with Na–Ca-rich rim; Na–Ca-amphibole is presented as inclusion in garnets as well as in matrix, and Ca-amphibole is generally found in the matrix. The Na–Ca-amphibole is observed at two different stages of metamorphism. The first is pre-UHP, and the second is post-garnet–omphacite assemblage though with a significant difference in composition. The pressure–temperature estimations of the formation of these two sets of Na–Ca-amphiboles corroborate their textural associations. Ca-rich amphiboles are generally present in the matrix either as symplectite with plagioclase or as a pseudomorph after garnet along with other secondary minerals like chlorite and biotite. Two different types of zoning have been observed in the amphibole grains: (1) core is Na-rich followed by Na–Ca rim and (2) core of Na–Ca-amphibole is followed by Ca-rich rim. The pre-UHP (or the prograde P–T path) and post-UHP stages (or the retrograde P–T path) of Tso Morari eclogites are defined by characteristic amphibole compositions, viz. Na/Na–Ca-amphibole, Na–Ca-amphibole and Ca-amphibole and thus indicate their utility in inferring crustal evolution of this UHP terrain.  相似文献   

7.
We investigated chemical weathering in a high elevation granitic environment in three selected watersheds located in the Pyrenees (France). The sites were located on glacial deposits derived from similar Hercynian (∼300 Ma) granites characterized by the occurrence of zoned plagioclases and trace calcic phases (epidote, prehnite, sphene, apatite). The surface waters at those sites show high Ca/Na molar ratios (>1) which could not be explained by the dissolution of the major plagioclase (oligoclase) present in the rocks. The coupled approach of investigating stream water chemistry and the mineralogy and chemistry of rocks and soils allowed us to explore the role of the weathering of trace calcic minerals in calcium export at the watershed scale. The weathering of the trace calcic minerals which represent ∼ 1% of the total rock volume are responsible for more than 90% of the calcium export at the sites. Annual cationic fluxes (∼ 23.104 eq/km2/yr) calculated for the Estibère watershed are among the highest reported for high elevation systems draining granitic rocks and ∼ 80% of this annual cationic flux can be attributed to the weathering of trace calcic phases. Calculations based on isotopic values (87Sr/86Sr) go in the same direction. Except apatite, the trace calcic phases appear to be mainly silicates, thus the type of chemical weathering observed in the Estibère watershed may have an influence on atmospheric CO2 consumption by granite weathering. However, comparison with other watersheds draining granitic environments worldwide, and with the two other sites in the Pyrenees, indicate that the role of trace calcic phases is important in most young environments exposed to chemical weathering (e.g., high elevation catchments on glacial deposits). Other factors such as the date of glacial retreat, the physical denudation rate, the hydrological functioning of the watershed and the nature and structure of the soil cover are also important.  相似文献   

8.
A detailed geochemical study on river waters of the Australian Victorian Alps was carried out to determine: (i) the relative significance of silicate, carbonate, evaporite and sulfide weathering in controlling the major ion composition and; (ii) the factors regulating seasonal and spatial variations of CO2 consumption via silicate weathering in the catchments. Major ion chemistry implies that solutes are largely derived from evaporation of precipitation and chemical weathering of carbonate and silicate lithologies. The input of solutes from rock weathering was determined by calculating the contribution of halite dissolution and atmospheric inputs using local rain and snow samples. Despite the lack of carbonate outcrops in the study area and waters being undersaturated with respect to calcite, the dissolution of vein calcite accounts for up to 67% of the total dissolved cations, generating up to 90% of dissolved Ca and 97% of Mg. Dissolved sulfate has δ34S values of 16 to 20‰CDT, indicating that it is derived predominantly from atmospheric deposition and minor gypsum weathering and not from bacterial reduction of FeS2. This militates against sulphuric acid weathering in Victorian rivers. Ratios of Si vs. the atmospheric corrected Na and K concentrations range from ~ 1.1 to ~ 4.3, suggesting incongruent weathering from plagioclase to smectite, kaolinite and gibbsite.Estimated long-term average CO2 fluxes from silicate weathering range from ~ 0.012 × 106 to 0.039 × 106 mol/km2/yr with the highest values in rivers draining the basement outcrops rather than sedimentary rocks. This is about one order of magnitude below the global average which is due to low relief, and the arid climate in that region. Time series measurements show that exposure to lithology, high physical erosion and long water–rock contact times dominate CO2 consumption fluxes via silicate weathering, while variations in water temperature are not overriding parameters controlling chemical weathering. Because the atmospheric corrected concentrations of Na, K and Mg act non-conservative in Victorian rivers the parameterizations of weathering processes, and net CO2 consumption rates in particular, based on major ion abundances, should be treated with skepticism.  相似文献   

9.
《Geochimica et cosmochimica acta》1999,63(13-14):1939-1953
Accessory calcite, present at concentrations between 300 and 3000 mg kg−1, occurs in fresh granitoid rocks sampled from the Merced watershed in Yosemite National Park, CA, USA; Loch Vale in Rocky Mountain National Park CO USA; the Panola watershed, GA USA; and the Rio Icacos, Puerto Rico. Calcite occurs as fillings in microfractures, as disseminated grains within the silicate matrix, and as replacement of calcic cores in plagioclase. Flow-through column experiments, using de-ionized water saturated with 0.05 atm. CO2, produced effluents from the fresh granitoid rocks that were dominated by Ca and bicarbonate and thermodynamically saturated with calcite. During reactions up to 1.7 yr, calcite dissolution progressively decreased and was superceded by steady state dissolution of silicates, principally biotite. Mass balance calculations indicate that most calcite had been removed during this time and accounted for 57–98% of the total Ca released from these rocks. Experimental effluents from surfically weathered granitoids from the same watersheds were consistently dominated by silicate dissolution. The lack of excess Ca and alkalinity indicated that calcite had been previously removed by natural weathering.The extent of Ca enrichment in watershed discharge fluxes corresponds to the amounts of calcite exposed in granitoid rocks. High Ca/Na ratios relative to plagioclase stoichiometries indicate excess Ca in the Yosemite, Loch Vale, and other alpine watersheds in the Sierra Nevada and Rocky Mountains of the western United States. This Ca enrichment correlates with strong preferential weathering of calcite relative to plagioclase in exfoliated granitoids in glaciated terrains. In contrast, Ca/Na flux ratios are comparable to or less than the Ca/Na ratios for plagioclase in the subtropical Panola and tropical Rio Icacos watersheds, in which deeply weathered regoliths exhibit concurrent losses of calcite and much larger masses of plagioclase during transport-limited weathering. These results indicate that the weathering of accessory calcite may strongly influence Ca and alkalinity fluxes from silicate rocks during and following periods of glaciation and tectonism but is much less important for older stable geomorphic surfaces.  相似文献   

10.
The early Pliocene Shirahama Limestone is a grainstone-packstone principally composed of fragments of algae, bryozoa, and echinoderm and subordinate volcanic rocks. The limestone was variously dolomitized and the regional distribution of dolomite is patchy. Dolomite occurs as isolated crystals filling pores, moulds, and solution vugs, and mosaic aggregates replacing bioclasts. Calcite occurs as rim and pore-filling sparry cements, and as calcareous skeletons. Isotopically, the dolomites are classified into a heavy oxygen group (?2 to ? 3.5%0 PDB) and a light oxygen group (?5.5 to ? 7.5%0 PDB). Calcite associated with heavy oxygen dolomite has δ18O of ? 6.5 to ?8.5%0 PDB, whereas those associated with light oxygen dolomite have a wide range from ?7.5 to ?14%0 PDB. Calcite in dolomite-free limestone has an oxygen isotopic composition of ?2 to ?8.5%0 PDB. Textures, chemistry, and isotopic evidence indicate that heavy oxygen calcite formed in freshwater, and heavy oxygen dolomite in a meteoric-marine mixture of 10–30% seawater. Light oxygen calcite and dolomite precipitated from modified hydrothermal fluids at approximately 30–65°C. Petrographic features, and both isotopic and chemical evidence suggest that the Shirahama Limestone was exposed to freshwater soon after deposition. Subsequently blocky calcite precipitated (Stage I). The limestone was locally submerged in the meteoric-marine mixture due to gradual subsidence or eustatic movement. This led to the precipitation of heavy oxygen, zoned dolomite and dolospar (Stage II). Hydrothermal alterations occurred in the area a few Myr ago, and related hydrothermal fluids and mixed meteoric-hydrothermal waters caused dedolomitization of some zoned dolomite, partial dissolution of vuggy dolomite, precipitation of limpid dolomite and recrystallization of some earlier dolomites (Stage III). Zeolites were also precipitated from these fluids. Finally, the Shirahama Limestone was exposed again to freshwater and sparry calcite precipitated to plug some of the remaining pores (Stage IV).  相似文献   

11.
Taiwan is a typical active orogenic belt situated at the collision boundary between the Eurasian Continental Plate and the Philippine Sea Plate. Dissolved major and trace constituents, as well as Sr and Sr isotopes in river waters collected from the Danshuei River basin in northern Taiwan have been studied to evaluate chemical weathering processes. The results of principal component analysis show that the ion sources in these river waters can be categorized into 3 major components: chemical weathering, seasalt contribution and local anthropogenic input. The chemical weathering is the most dominant factor that contributes about 85% of total variances. Significantly increased Na/Cl and Ca/Cl, as well 87Sr/86Sr, were observed in most upper stream samples. The Na/Cl and Ca/Cl ratios in the Dahan Stream, however, are much higher than the Shindien Stream. Even though average rainfall is stronger in the Shindien drainage basin, chemical evidence from river waters supports less intense weathering in the region. Selective dissolution of secondary calcites explains the observed high Ca/Cl, Sr/Cl and Ca/Na in the Dahan Stream. These results highlight the potential importance of tectonic factors, such as uplift and physical erosion in studying chemical weathering in an active orogenic belt.  相似文献   

12.
Finely cellular plagioclase intergrowths have been studied in xenocrystic andesine (An32) and andesine mantled K-feldspars within mafic magmatic enclaves in a quartz-feldspar porphyry from the Proterozoic subvolcanic Hammarudda complex, Åland rapakivi batholith, SW Finland. The cellular intergrowths usually occur as 0.2–2.0 mm mantles around xenocrysts but also as entirely cellular grains, and are built up of a network of two distinct phases: one relatively Na-rich (An31) and one relatively Ca-rich (An50). The grains are also covered by a thin (0.08–0.12 mm), continuous, normally zoned rim outside the cellular mantle. Small inclusions (0.01–0.05 mm) of Fe–Mg minerals are concentrated in the Ca-rich part of the network. Compositionally, the Na-rich phase of the network is close to the inner non-cellular andesine of the xenocrysts. However, it has a lower Or- and a slightly lower An-content. The Ca-rich phase has the same composition as the inner part of the normally zoned rim, which outwards grades into lower An-contents that overlap the An-content of the matrix plagioclases. The cellular network was developed after the andesine xenocrysts (or andesine mantled K-feldspars) were engulfed in mafic magmatic enclaves during a mixing event. The xenocrysts became heated to a temperature just below the liquidus of the mafic magma. Dissolution of the xenocrysts developed a spongy cellular texture which was penetrated by enclave magma. Ca-rich plagioclase crystallized in the cells in equilibrium with the enclave magma, trapping Fe–Mg-rich melt. As the enclaves cooled the outermost thin rim and matrix plagioclases crystallized from the mafic melt. These processes operated in fairly large enclaves, as the one studied here, which has a diameter of 70cm. Smaller enclaves, on the other hand, were cooled more rapidly to temperatures close to the solidus of the enclave magma, and consequently had no time to dissolve the xenoxrysts.  相似文献   

13.
The relationship between subglacial chemical weathering processes and the Sr isotope composition of runoff from Robertson Glacier, Alberta, Canada, is investigated. This glacier rests on predominantly carbonate bedrock of Upper Devonian age, but silicate minerals are also present. The provenance of solute in meltwaters is found to vary systematically with solute concentration and, by inference, subglacial water residence time. In dilute waters, the principal process of solute acquisition is calcite dissolution fueled by protons derived from the dissolution of CO2 and subsequent dissociation of carbonic acid. At higher solute concentrations, dolomite dissolution coupled to sulfide oxidation is more important. Sr concentration is found to increase with total solute concentration in two separate meltwater streams draining from the glacier, but 87Sr/86Sr only increases in the eastern melt stream. Carbonate and K-feldspar sources are shown to dominate the Sr content of the western stream, irrespective of concentration. They also dominate the Sr content of the eastern stream at low and intermediate concentrations, but at higher concentrations, muscovite (with high 87Sr/86Sr) is also an important Sr source. This reflects the outcrop of muscovite-bearing lithologies in the catchment of the eastern stream and an increase in the rate of weathering of K-silicates relative to that of carbonates as more concentrated solutions approach saturation with respect to carbonates. Nonstoichiometric release of 87Sr/86Sr and preferential release of Sr over K from freshly ground K-silicate surfaces may also occur. This may help to explain the radiogenic nature of runoff from distributed subglacial drainage systems, which are characterized by long water:rock contact times and water flow through environments in which crushing and grinding of bedrock are active processes.Although the exchangeable Sr in tills has higher 87Sr/86Sr than local carbonate bedrock, only the more concentrated meltwaters from the eastern stream display similarly high values. The most dilute waters, which probably transport the bulk of the dissolved Sr flux from the glacier, have 87Sr/86Sr characteristic of local carbonate bedrock. Thus, the results suggest that although enhanced weathering of silicate minerals containing radiogenic Sr (such as muscovite) does occur in glaciated carbonate terrains, it is unlikely to contribute to any enhanced flux of radiogenic Sr from glaciated continental surfaces to the oceans.  相似文献   

14.
The systematic sampling of the chemical composition of the groundwater from five karst springs (including an overflow spring) and one outflowing borehole have permitted to determine distinctive chemical changes in the waters that reflect the geochemical processes occurring in a carbonate aquifer system from southern Spain. The analysis of the dissolution parameters revealed that geochemical evolution of the karst waters basically depends on the availability of the minerals forming aquifer rocks and the residence time within the aquifers. In the three proposed scenarios in the aquifers, which include the preferential flow routines, the more important geochemical processes taking place during the groundwater flow from the recharge to the discharge zones are: CO2 dissolution and exsolution (outgassing), calcite net dissolution, calcite and dolomite sequential dissolution, gypsum/anhydrite and halite dissolution, de-dolomitization and calcite precipitation. A detailed analysis of the hydrochemical data set, saturation indices of the minerals and partial pressure of CO2 in the waters joined to the application of geochemical modelling methods allowed the elaboration of a hydrogeochemical model of the studied aquifers. The developed approach contributes to a better understanding of the karstification processes and the hydrogeological functioning of carbonate aquifers, the latter being a crucial aspect for the suitable management of the water resources.  相似文献   

15.
Flows of different hierarchy, which travel through limestone, schist, sandstone and ultra-basic rocks, with ages from the Paleocene to the Jurassic, at Sierra del Rosario, Pinar del Río, Cuba, were characterized. The waters were sampled from 1984 until 2004 and the data were statistically processed by means of chemical equilibrium and physico-chemical models, under a flow system view of interpretation. Results demonstrate that the physico-chemical properties of the water are controlled by water–rock interaction resulting from residence time since rainwater infiltrate and the path it follows to the discharge zone and the type of aquifer material the different groundwater flows are in contact with. Geochemical indices allow the definition of the different types of flow (local, intermediate, regional) to be characterized, permitting a further definition of the different flow systems and rock type involved, as well as its use for water supply and medical use. The main geochemical processes which control the chemical composition acquisitions mode are: congruent dissolution of calcite, dolomite, and halite; incongruent dissolution of plagioclase and microcline minerals; pyrite oxidation, sulphate reduction, and silica dissolution at the surface or silica precipitation at deep saturation and circulation zones.  相似文献   

16.
Determining the relative proportions of silicate vs. carbonate weathering in the Himalaya is important for understanding atmospheric CO2 consumption rates and the temporal evolution of seawater Sr. However, recent studies have shown that major element mass-balance equations attribute less CO2 consumption to silicate weathering than methods utilizing Ca/Sr and 87Sr/86Sr mixing equations. To investigate this problem, we compiled literature data providing elemental and 87Sr/86Sr analyses for stream waters and bedrock from tributary watersheds throughout the Himalaya Mountains. In addition, carbonate system parameters (PCO2, mineral saturation states) were evaluated for a selected suite of stream waters. The apparent discrepancy between the dominant weathering source of dissolved major elements vs. Sr can be reconciled in terms of carbonate mineral equilibria. Himalayan streams are predominantly Ca2+-Mg2+-HCO3− waters derived from calcite and dolomite dissolution, and mass-balance calculations demonstrate that carbonate weathering contributes ∼87% and ∼76% of the dissolved Ca2+ and Sr2+, respectively. However, calculated Ca/Sr ratios for the carbonate weathering flux are much lower than values observed in carbonate bedrock, suggesting that these divalent cations do not behave conservatively during stream mixing over large temperature and PCO2 gradients in the Himalaya.The state of calcite and dolomite saturation was evaluated across these gradients, and the data show that upon descending through the Himalaya, ∼50% of the streams evaluated become highly supersaturated with respect to calcite as waters warm and degas CO2. Stream water Ca/Mg and Ca/Sr ratios decrease as the degree of supersaturation with respect to calcite increases, and Mg2+, Ca2+, and HCO3− mass balances support interpretations of preferential Ca2+ removal by calcite precipitation. On the basis of patterns of saturation state and PCO2 changes, calcite precipitation was estimated to remove up to ∼70% of the Ca2+ originally derived from carbonate weathering. Accounting for the nonconservative behavior of Ca2+ during riverine transport brings the Ca/Sr and 87Sr/86Sr composition of the carbonate weathering flux into agreement with the composition of carbonate bedrock, thereby permitting consistency between elemental and Sr isotope approaches to partitioning stream water solute sources. These results resolve the dissolved Sr2+ budget and suggest that the conventional application of two-component Ca/Sr and 87Sr/86Sr mixing equations has overestimated silicate-derived Sr2+ and HCO3− fluxes from the Himalaya. In addition, these findings demonstrate that integrating stream water carbonate mineral equilibria, divalent cation compositional trends, and Sr isotope inventories provides a powerful approach for examining weathering fluxes.  相似文献   

17.
《Applied Geochemistry》2002,17(5):583-603
This study identifies and quantifies the water–rock interactions responsible for the composition of 25 spring waters, and derives the weathering rates of rock-forming minerals in a complex of petrologic units containing ultramafics, amphibolites, augengneisses and micaschists. Bulk chemical analyses were used to calculate the mineralogical composition of these rocks; the composition of the rock-forming minerals were determined by microprobe analyses. The soils developed on augengneisses and micaschists contain predominantly halloysite; on the other units mixtures of halloysite and smectites. The mineralogical and chemical data on rocks and soils are essential for writing the proper weathering reactions and for solving mole balances between the amounts of weathered primary minerals and secondary products formed (soils and solutes in groundwater). Ground waters emanating in springs were collected in 3 consecutive seasons, namely late Summer, Winter and Spring, and analyzed for major components. Using an algorithm based on mole and charge balance equations, the average concentrations of the solutes were linked with a combination of possible weathering reactions. To sort out the best match of weathering reactions and the concomitantly generated water composition, the results were checked against the limiting condition of similarity between the predicted and actual clay mineral abundance in the soils. Having selected the best-fit weathering reactions, the mineral weathering rates could also be calculated by combining the median discharge rates and recharge areas of the springs and normalizing the rates by the mineral abundance. For the one case—plagioclase—for which comparison with published results was possible, the results compare favorably with rates calculated by other groups. For the most abundant primary minerals the following order of decreasing weathering rates was found (in moles/(ha·a·%mineral)): forsterite (485) > clinozoisite (114) > chlorite (49) > plagioclase (45) > amphibole (28). In as far as this order differs from commonly used orders of weatherability, this has to be due to differences in the hydrologic regime within this area and between this and other case studies. As additional objective, the authors wanted to explain the effects of contributions by sources other than water-rock interactions. The latter processes are coupled with acquisition of carbonate alkalinity and dissolved silica. Contributions by sources other than water–rock interactions are manifest by the Cl−, SO2−4 and NO−3 concentrations. It was possible to approximate the contribution of atmospheric deposition. More importantly, knowledge of the application and composition of fertilizers enabled assessment of the effects of farming on the composition of ground waters emanating in the springs. It was also possible to estimate how selective uptake of nutrients and cations by vegetation as well as ion-exchange processes in the soil modified the spring water composition. Using this rather holistic approach, it is possible to satisfactorily explain how spring waters, in this petrologically and agriculturally diverse area, acquired their composition.  相似文献   

18.
Based on the geological background, R-mode factor statistics, and the analysis of the stability diagram for the corresponding system, five weathering reactions controlling the surface-water chemical composition in the watershed of the Changhuajiang River are deduced. In the mass balance model, the precipitation accounts for some solute input, since the rainwater is dilute without pollution. Most of the Ca2+ and HCO 3 – ions are from the dissolution of calcite, K+, Na+, H4SiO4 and some of the Mg2+ and HCO 3 – come from albite and biotite weathering to kaolinite. The dissolution of dolomite and gypsum controls the mass balances of Mg2+ and SO 4 2– . The dissolution of calcite is the dominant chemical weathering reaction in the watershed because of its reactivity and high concentration. In the watershed in 1986, the chemical weathering rate was 0.073 (kg/m2 a), and the mechanical denudation rate is 0.093 (kg/m2 a). The chemical weathering mass output proportion of carbonate rocks to silicate rocks was about three to one.  相似文献   

19.
碳酸盐岩的H2CO3溶蚀产生岩溶碳汇,占整个岩石风化碳汇的 94%。西南岩溶区硫酸型酸雨严重,硫酸型酸雨广泛参与碳酸盐岩的溶蚀。H2SO4参与的碳酸盐岩风化是一个大气CO2净释放过程,具有减汇作用巨大。另一方面,岩溶区石灰土壤和地下水具有较高的pH值及盐基饱和度,对H+有巨大的缓冲作用,大气酸沉降在碳酸盐岩地区可能并不会造成地下水的HCO3-和pH降低;相反,较高浓度的SO42-所产生的盐效应和SO2-4与各种阳离子形成的离子对会增大方解石、白云石溶解度,可增强H2CO3对碳酸盐的溶蚀,这可能会使岩溶作用产生更大的碳汇效应。因此,硫酸型酸雨参与碳酸盐岩风化的减汇效应不仅可能被高估,硫酸型酸雨还可能增强碳酸盐岩的H2CO3溶蚀,具有增加岩溶碳汇效应的作用。应结合石灰土壤对大气酸沉降的缓冲容量和阈值及大气酸沉降的H+与土壤中盐基离子的交换量,并综合考虑盐效应、离子对作用、同离子效应,客观评价硫酸型酸雨流经石灰土壤层后对碳酸盐岩溶蚀吸收大气/土壤CO2的影响   相似文献   

20.
《Applied Geochemistry》1999,14(2):237-254
Two major types of groundwater can be readily distinguished in the Variscian crystalline basement of the Black Forest in S–W Germany. Saline thermal water utilized in spas has its origin in 3–4 km deep reservoirs and developed its composition by 3 component mixing of surface freshwater, saltwater (of ultimately marine origin) and a water–rock reaction component. In contrast to the thermal water, CO2-rich mineral water, tapped and bottled from many wells in the Black Forest, has low salinities but a TDS distribution similar to that of thermal water. It developed its chemical composition entirely by reaction of CO2-rich water with the gneissic or granitic aquifer rock matrix. Particularly important is the contribution of various plagioclase dissolution and weathering reactions that may, at some locations, involve precipitation and dissolution of secondary calcite. Sodium/Ca ratios of water and of rock forming plagioclase in the basement rocks suggests that plagioclase weathering is strongly incongruent. Calcium is released to the water, whereas Na remains fixed to the albite feldspar component.The major element composition of 192 water samples used in this study also indicates a clear vertical stratification of the type of water chemistry; Ca–HCO3 near the surface, Na–Ca–HCO3–SO4 at intermediate depth and Na–Ca–Cl at great depth.The mean permeability of Black Forest granite is about K=10−6 m/s; it is significantly lower in gneisses (gneiss: mean K=5×10−8 m/s) leading to focused flow through granite. Highly permeable fracture and fault zones, particularly in granite, are utilized by high-TDS saline deep groundwater as ascent channels and flow paths. Although spatially closely associated, the topography driven upwelling system of saline deep water and the near-surface flow system of CO2-rich mineral waters are hydraulically and chemically unconnected.  相似文献   

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