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1.
Continental weathering plays a dominant role in regulating the global carbon cycle, soil chemistry and nutrient supply to oceans. The CO2-mediated silicate weathering acts as a major CO2 sink, whereas sulphuric acid-mediated carbonate dissolution releases CO2 to the atmosphere–ocean system. In this study, dissolved major ions and silica concentrations of two tropical (Damodar and Subarnarekha) river systems from India have been measured to constrain the type and rate of chemical weathering for these basins. The total dissolved solids (TDS) of these rivers, a measure of total solute supply from all possible sources, are about 2–3 times higher than that of the global average for rivers. Mass balance calculations involving inverse modelling estimate that 63 ± 11% of total cations are derived from rock weathering, of which 27 ± 7% of cations are supplied through silicate weathering. The sulphide-S concentrations are estimated by comparing the water chemistry of these two rivers with that of a nearby river (Brahmani) with similar lithology but no signatures of sulphide oxidation. The outflows of Damodar and Subarnarekha rivers receive 17% and 55% of SO4 through sulphide oxidation, respectively. The sulphide oxidation fluxes from the ore mining areas, such as upper Damodar (0.52 × 109 mol/yr) and lower Subarnarekha (0.66 × 109 mol/yr) basins, are disproportionally (~9 times) higher compared to their fractional areal coverage to the global drainage area. The corresponding CO2 release rate (2.84 × 104 mol/km2/yr) for the Damodar basin is lower by five times than its CO2 uptake rate (1.38 × 105 mol/km2/yr). The outcomes of this study underscore the dominance of sulphide oxidation in controlling the dissolved chemical (cationic and sulphur) fluxes.  相似文献   

2.
Meltwaters collected from boreholes drilled to the base of the Haut Glacier d'Arolla, Switzerland have chemical compositions that can be classified into three main groups. The first group is dilute, whereas the second group is similar to, though generally less concentrated in major ions, than contemporaneous bulk glacial runoff. The third group is more concentrated than any observed bulk runoff, including periods of flow recession. Waters of the first group are believed to represent supraglacial meltwater and ice melted during drilling. Limited solutes may be derived from interactions with debris in the borehole. The spatial pattern of borehole water levels and borehole water column stratification, combined with the chemical composition of the different groups, suggest that the second group represent samples of subglacial waters that exchange with channel water on a diurnal basis, and that the third group represent samples of water draining through a ‘distributed’ subglacial hydraulic system. High NO−3 concentrations in the third group suggest that snowmelt may provide a significant proportion of the waters and that the residence time of the waters at the bed in this particular section of the distributed system is of the order of a few months. The high NO−3 concentrations also suggest that some snowmelt is routed along different subglacial flowpaths to those used by icemelt. The average SO2−4: (HCO−3 + SO2−4) ratio of the third group of meltwaters is 0.3, suggesting that sulphide oxidation and carbonate dissolution (which gives rise to a ratio of 0.5) cannot provide all the HCO−3 to solution. Hence, carbonate hydrolysis may be occurring before sulphide oxidation, or there may be subglacial sources of CO2, perhaps arising from microbial oxidation of organic C in bedrock, air bubbles in glacier ice or pockets of air trapped in subglacial cavities. The channel marginal zone is identified as an area that may influence the composition of bulk meltwater during periods of recession flow and low diurnal discharge regimes. © 1997 by John Wiley & Sons, Ltd.  相似文献   

3.
Recent models of chemical weathering in alpine glacial meltwaters suggest that sulphide oxidation is a major source of solute in the distributed component of the subglacial hydrological system. This reaction requires O2, and may lower dissolved oxygen levels to below saturation with respect to the atmosphere. This should result in an inverse association between SO72- and dissolved oxygen saturation. However, measurements of O2 saturation in bulk meltwaters draining the Haut Glacier d'Arolla, Switzerland, show that there is a positive association between SO42- and O2 saturation. The O2 content of glacial meltwaters depends on the initial content of snow and icemelt, which may be controlled by the rate of melting, and the kinetic balance between O2 losses (e.g. sulphide oxidation, microbial respiration) and gains (e.g. diffusion of O2 into solution).  相似文献   

4.
Dissolved major ions, Sr concentrations and 87Sr/86Sr ratios of 10 coastal lakes from the Larsemann Hills, East Antarctica have been studied to constrain their solute sources, transport and glacial weathering patterns in their catchments. In absence of perennial river/streams, lakes serve as only reliable archive to study land surface processes in these low-temperature regions. The lake water chemistry is mostly Na-Cl type and it does not show any significant depth variations. Sr isotope compositions of these lakes vary from 0.7110 to 0.7211 with an average value of 0.7145, which is higher than modern seawater value. In addition to oceanic sources, major ions and Sr isotopic data show appreciable amount of solute supply from chemical weathering of silicate rocks in lake catchments and dissolution of Ca-Mg rich salts produced during the freezing of seawaters. The role of sulphide oxidation and carbonate weathering are found to be minimal on lake hydro-chemistry in this part of Antarctica. Inverse model calculations using this chemical dataset provide first-order estimates of dissolved cations and Sr; they are mostly derived from oceanic (seawater + snow) sources (cations approximately 76%) and (Sr approximately 92%) with minimal supplies from weathering of silicates (cations approximately 15%); (Sr approximately 2%) and Ca-rich minerals (cations approximately 9%); (Sr approximately 7%). The silicate weathering rate and its corresponding atmospheric CO2 consumption rate estimates for Scandrett lake catchment (3.6 ± 0.3 tons/km2/year and 0.5 × 105 moles/km2/year), are lower than that of reported values for the average global river basins (5.4 tons/km2/year and 0.9 × 105 tons/km2/year) respectively. The present study provides a comprehensive report of chemical weathering intensity and its role in atmospheric CO2 consumption in low-temperature pristine environment of Antarctica. These estimates underscore the importance of Antarctica weathering on atmospheric CO2 budget, particularly during the past warmer periods when the large area was exposed and available for intense chemical weathering.  相似文献   

5.
There are still relatively few hydrochemical studies of glacial runoff and meltwater routing from the high latitudes, where non-temperate glacier ice is frequently encountered. Representative samples of glacier meltwater were obtained from Scott Turnerbreen, a ‘cold-based’ glacier at 78° N in the Norwegian high Arctic archipelago of Svalbard, during the 1993 melt season and analysed for major ion chemistry. Laboratory dissolution experiments were also conducted, using suspended sediment from the runoff. Significant concentrations of crustal weathering derived SO2−4 are present in the runoff, which is characterized by high ratios of SO2−4: (SO2−4+HCO−3) and high p(CO2). Meltwater is not routed subglacially, but flows to the glacier terminus through subaerial, ice marginal channels, and partly flows through a proglacial icing, containing highly concentrated interstitial waters, immediately afront the terminus. The hydrochemistry of the runoff is controlled by: (1) seasonal variations in the input of solutes from snow- and icemelt; (2) proglacial solute acquisition from the icing; and (3) subaerial chemical weathering within saturated, ice-cored lateral moraine adjoining drainage channels at the glacier margins, sediment and concentrated pore water from which is entrained by flowing meltwater. Diurnal variations in solute concentration arise from the net effects of variable sediment pore water entrainment and dilution in the ice marginal streams. Explanation of the hydrochemistry of Scott Turnerbreen requires only one major subaerial flow path, the ice marginal channel system, in which seasonally varying inputs of concentrated snowmelt and dilute icemelt are modified by seepage or entrainment of concentrated pore waters from sediment in lateral moraine, and by concentrated interstitial waters from the proglacial icing, supplied by leaching, slow drainage at grain intersections or simple melting of the icing itself. The ice marginal channels are analogous neither to dilute supra/englacial nor to concentrated subglacial flow components. © 1998 John Wiley & Sons, Ltd.  相似文献   

6.
Climate factors play critical roles in controlling chemical weathering, while chemically weathered surface material can regulate climate change. To estimate global chemical weathering fluxes and CO2 balance, it is important to identify the characteristics and driving factors of chemical weathering and CO2 consumption on the Tibetan Plateau, especially in glaciated catchments. The analysis of the hydro-geochemical data indicated that silicate weathering in this area was inhibited by low temperatures, while carbonate weathering was promoted by the abundant clastic rocks with fresh surfaces produced by glacial action. Carbonate weathering dominated the riverine solute generation (with a contribution of 58%, 51%, and 43% at the QiangYong Glacier (QYG), the WengGuo Hydrological Station (WGHS), and the lake estuary (LE), respectively). The oxidation of pyrite contributed to 35%, 42%, and 30% of the riverine solutes, while silicate weathering contributed to 5%, 6%, and 26% of the riverine solutes at the QYG, WGHS, and LE, respectively. The alluvial deposit of easily weathering fine silicate minerals, the higher air temperature, plant density, and soil thickness at the downstream LE in comparison to upstream and midstream may lead to longer contact time between pore water and mineral materials, thus enhancing the silicate weathering. Because of the involvement of sulfuric acid produced by the oxidation of pyrite, carbonate weathering in the upstream and midstream did not consume atmospheric CO2, resulting in the high rate of carbonate weathering (73.9 and 75.6 t km−2 yr−1, respectively, in maximum) and potential net release of CO2 (with an upper constraint of 35.6 and 35.2 t km−2 yr−1, respectively) at the QYG and WGHS. The above results indicate the potential of the glaciated area of the Tibetan Plateau with pyrite deposits being a substantial natural carbon source, which deserves further investigation.  相似文献   

7.
Concerns related to climate change have resulted in an increasing interest in the importance of hydrological events such as droughts in affecting biogeochemical responses of watersheds. The effects of an unusually dry summer in 2002 had a marked impact on the biogeochemistry of three watersheds in the north‐eastern USA. Chemical, isotopic and hydrological responses with particular emphasis on S dynamics were evaluated for Archer Creek (New York), Sleepers River (Vermont) and Cone Pond (New Hampshire) watersheds. From 1 August to 14 September 2002, all three watersheds had very low precipitation (48 to 69 mm) resulting in either very low or no discharge (mean 0·015, 0·15 and 0·000 mm day?1 for Archer Creek, Sleepers River and Cone Pond, respectively). From 15 September to 31 October 2002, there was a substantial increase in precipitation totals (212, 246 and 198 mm, respectively) with increased discharge. Archer Creek was characterized by a large range of SO42? concentrations (152 to 389 µeq L?1, mean = 273 µeq L?1) and also exhibited the greatest range in δ34S values of SO42? (?1·4 to 8·8 ‰ ). Sleepers River's SO42? concentrations ranged from 136 to 243 µeq L?1 (mean = 167 µeq L?1) and δ34S values of SO42? ranged from 4·0 to 9·0 ‰ . Cone Pond's SO42? concentrations (126–187 µeq L?1, mean = 154 µeq L?1) and δ34S values (2·4 to 4·3 ‰ ) had the smallest ranges of the three watersheds. The range and mean of δ18O‐SO42? values for Archer Creek and Cone Pond were similar (3·0 to 8·9 ‰ , mean = 4·5 ‰ ; 3·9 to 6·3 ‰ , mean = 4·9 ‰ ; respectively) while δ18O‐SO42? values for Sleepers River covered a larger range with a lower mean (1·2 to 10·0 ‰ , mean = 2·5). The difference in Sleepers River chemical and isotopic responses was attributed to weathering reactions contributing SO42?. For Archer Creek wetland areas containing previously reduced S compounds that were reoxidized to SO42? probably provided a substantial source of S. Cone Pond had limited internal S sources and less chemical or isotopic response to storms. Differences among the three watersheds in S biogeochemical responses during these storm events were attributed to differences in S mineral weathering contributions, hydrological pathways and landscape features. Further evaluations of differences and similarities in biogeochemical and hydrological responses among watersheds are needed to predict the impacts of climate change. Copyright © 2008 John Wiley & Sons, Ltd.  相似文献   

8.
Mass balance studies in forested catchments in the northeastern USA show that S losses via streamwater SO42? exceed measured atmospheric S inputs. Possible sources of the excess S loss include underestimated dry deposition, mineralization of organic S in soils, desorption of soil sulphate, oxidation of recently formed sulphides and mineral weathering. Evaluating the relative contribution of these sources and processes to SO42? export is important to our understanding of S cycling as well as to policy makers in their evaluation of the efficacy of S emission controls. In order to evaluate the potential for mineral weathering contributions to SO42? export, we measured concentration and isotopic composition (δ34S and δ18O) of SO42? in stream water, and concentration and δ34S values of four S fractions in bedrock and soil parent material in catchments of varying geological composition. Geological substrates with low S concentrations were represented by catchments underlain by quartzite and granite, whereas geological substrates with high S concentrations were represented by catchments underlain by sulphidic slate, schist and metavolcanic rocks. Catchments with S‐poor bedrock had stream‐water SO42? concentrations <100 µeq L?1 and isotopic values consistent with those of atmospheric SO42? that had been cycled through the organic soil pool. Catchments with S‐rich bedrock had stream‐water SO42? concentrations ranging from 56 to 229 µeq L?1. Isotopic values deviated from those of SO42? in atmospheric deposition, clearly indicating a mineral weathering source in some cases, whereas in others spatial variability of mineral δ34S values precluded the isotopic detection of a weathering contribution. These results, along with evidence suggesting formation of secondary sulphate minerals in bedrock weathering rinds, indicate that mineral weathering may be an important source of S in the surface waters of some forested catchments in the northeastern USA. Copyright © 2004 John Wiley & Sons, Ltd.  相似文献   

9.
Jun Xiao  Fei Zhang  Zhangdong Jin 《水文研究》2016,30(25):4855-4869
Hydrochemistry methods were used to decipher the weathering and geochemical processes controlling solute acquisition of river waters in the dry season in the middle Loess Plateau (MLP), one of the most severely eroded areas and turbid riverine systems in the world. River waters were neutral to slightly alkaline with pH varying from 7.6 to 9.6. The total dissolved solids decreased from northwest to southeast with a mean value of 804 mg/l, much higher than the global average and other large rivers in China. Ternary diagram showed that river waters were dominated by Na+, HCO3?, and Cl? with the main water‐type of HCO3?–Cl?–Na+. Saturation index values, Mg2+, Ca2+, and HCO3? analyses indicated the preferential Ca2+ removal by calcite precipitation. Gibbs plots and stoichiometry plots indicated that the dissolved solutes were mainly derived from rock weathering with minor anthropogenic and atmospheric inputs. Samples in the northwestern basin are also influenced by evaporation. A forward model of mass budget calculation showed that, owing to high soluble characteristics, evaporite dissolution was a major feature of river waters and contributed 41% to the total dissolved cations on average, while carbonate and silicate weathering contributed 28%,and 25% on average, respectively. Besides evaporite dissolution, cation exchange is also responsible for the high concentrations of Na+ in river water. Spatial variations showed that evaporite dissolution and silicate weathering were higher in the northern basin, whereas carbonate weathering was higher in the southern basin. Different from most rivers in the world, the physical erosion rates (varying from 117.7 to 4116.6 t/km2y) are much higher than the chemical weathering rates (varying from 3.54 to 6.76 t/km2y) in the MLP because of the loose structure of loess and poor vegetation in the basin. In the future, studies on comparison of water geochemistry in different seasons and on influence of different types of land use and soil salinization on water geochemistry, denudation rates, and water quality should be strengthened in the MLP. These results shed some lights on processes responsible for modern loess weathering and also indicate the importance of time‐series sampling strategy for river water chemistry. Copyright © 2016 John Wiley & Sons, Ltd.  相似文献   

10.
Snowmelt‐fed springs and small (0.5 km2) upland catchments in alpine areas of the western United States contribute significantly to the quantity and inorganic chemistry of water delivered to downstream basins but have not been studied extensively. Mineral weathering, transit time, and hydrologic mixing control the solute chemistry of waters that drain the upland zone of Niwot Ridge, Colorado Front Range, and adjacent areas in the granitic core of the Southern Rocky Mountains. Water in 37 springs sampled in this study flows in generally short steep paths (~0.3 km) through shallow regolith with mean transit times (MTT) of weeks to months, producing solutions dominated by Si, Ca2+, Na+, and HCO3?, locally SO42?. Rock type is a significant control on spring, surface, and shallow groundwater chemistry, and plagioclase (oligoclase) is the major source of dissolved Na+ and Si. Concentrations of Ca2+ exceed stoichiometric predictions of oligoclase weathering by ~3.5×; excess Ca2+ likely represents weathering of aeolian material, vein calcite, or trace minerals. Concentrations of base cations and Si increase slowly with estimated MTT of 0.2 years for Niwot Ridge spring waters, and several years for shallow groundwater sampled by wells. Chemical weathering of silicate minerals is slow with estimated rates of ~2.0 and 0.2 pmol·m?2·s?1 for oligoclase and microcline, respectively; the most mineralized spring waters are saturated only with respect to kaolinite and montmorillonite. More than 50% of the dissolved base cations + Si measured in Boulder Creek at Orodell (~25 km downstream) accumulate before water emerges from alpine springs on Niwot Ridge. Warming global temperatures are shifting more high‐elevation precipitation to rain, potentially changing run‐off patterns, transit time, and solute loads. Acquisition of solutes by alpine waters thus has implications far beyond small upland catchments.  相似文献   

11.
Solute and runoff time-series at Finsterwalderbreen, Svalbard, provide evidence for considerable basal routing of water and the existence of at least two contrasting subglacial chemical weathering environments. The hydrochemistry of a subglacial upwelling provides evidence for a snowmelt-fed subglacial reservoir that dominates bulk runoff during recession flow. High concentrations of Cl− and crustal ions, high pCO2 and ratios of [*SO2−4/(*SO2−4+HCO−3)] close to 0·5 indicate the passage of snowmelt through a subglacial weathering environment characterized by high rock:water ratios, prolonged residence times and restricted access to the atmosphere. At higher discharges, bulk runoff becomes dominated by icemelt from the lower part of the glacier that is conveyed through a chemical weathering environment characterized by low rock:water ratios, short residence times and free contact with atmospheric gases. These observations suggest that icemelt is routed via a hydrological system composed of basal/ice-marginal, englacial and supraglacial components and is directed to the glacier margins by the ice surface slope. Upwelling water flows relatively independently of icemelt to the terminus via a subglacial drainage system, possibly constituting flow through a sediment layer. Cold basal ice at the terminus forces it to take a subterranean routing in its latter stages. The existence of spatially discrete flow paths conveying icemelt and subglacial snowmelt to the terminus may be the norm for polythermal-based glaciers on Svalbard. Proglacial mixing of these components to form the bulk meltwaters gives rise to hydrochemical trends that resemble those of warm-based glaciers. These hydrochemical characteristics of bulk runoff have not been documented on any other glacier on Svalbard to date and have significance for understanding interactions between thermal regime and glacier hydrology. © 1998 John Wiley & Sons, Ltd.  相似文献   

12.
Oxygen isotopic data are presented for bulk glacial meltwaters draining the Haut Glacier d'Arolla, Valais, Switzerland and for the sulphate contained within them in an attempt to assess the redox status of the subglacial chemical weathering environment. The sulphate derived from subglacial chemical weathering is so depleted in 18O that it must have formed, at least partially, in an anoxic environment. Under these conditions, Fe3+ can act as an oxidizing agent and oxygen atoms incorporated into sulphate are derived from 18O‐depleted water molecules (by contrast, dissolved O2 is strongly enriched in 18O). These data therefore support the hypothesis that sectors of the glacier bed are anoxic and that Fe3+ may act as a significant oxidizing agent under these conditions. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

13.
The hydrochemistry of naled and upwelling water sampled from the forefields of Finsterwalderbreen, Svalbard, during spring are used for the first time to infer the hydrology of overwinter meltwaters at a polythermal‐based glacier. Hydrochemical variations in naled are explained in terms of different water sources and their chemical alteration during freezing. Two water sources to naled are identified: surficially routed snowmelt and subglacial water. Naled that results from the freezing of the former is enriched in atmospherically derived ions such as Na+ and Cl−, and is believed to be formed during winter warm periods. Naled of subglacial origin contains relatively high proportions of crustally derived solute. It reflects the freezing of subglacial meltwaters that continue to issue from a subterranean upwellling during winter. An increasing dominance of SO2−4 Mg2+, Na+ and Cl− in subglacial naled with increasing distance from the upwelling reflects the progressive freezing of this water body and the associated removal of Ca2+ and HCO by calcite precipitation. These spatial trends are accentuated by the leaching of soluble ions from the naled close to its source by subsequent upwelling waters. The chemistry of spring upwelling waters, also of subglacial origin, strongly reflects this process. Meltwater produced by geothermal heating of glacier basal ice is believed to be the principal source of water to the subglacial drainage system during winter. Solute acquisition by this meltwater is limited by a scarcity of proton suppliers. Evolution of this dilute meltwater carries an imprint of ion exchange processes. Some stored subglacial water from the end of the previous ablation season may supplement the basal meltwater component in early winter. Copyright © 2000 John Wiley & Sons, Ltd.  相似文献   

14.
The aluminium (Al) cycle in glacierised basins has not received a great deal of attention in studies of biogeochemical cycles. As Al may be toxic for biota, it is important to investigate the processes leading to its release into the environment. It has not yet been ascertained whether filterable Al (passing through a pore size of 0.45 μm) is incorporated into biogeochemical cycles in glacierised basins. Our study aims to determine the relationship between the processes bringing filterable Al and glacier‐derived filterable nutrients (particularly Fe and Si) into glacierised basins. We investigated the Werenskiöldbreen basin (44.1 km2, 60% glacierised) situated in SW Spitsbergen, Svalbard. In 2011, we collected meltwater from a subglacial portal at the glacier front and at a downstream hydrometric station throughout the ablation season. The Al concentration, unchanged between the subglacial system and proglacial zone, reveals that aluminosilicate weathering is a dominant source of filterable Al under subglacial conditions. By examining the Al:Fe ratio compared with pH and the sulphate mass fraction index, we found that the proton source for subglacial aluminosilicate weathering is mainly associated with sulphide oxidation and, to a lesser degree, with hydrolysis and carbonation. In subglacial outflows and in the glacial river, Al and Fe are primarily in the forms of Al(OH)4‐ and Fe(OH)3. The annual filterable Al yield (2.7 mmol m‐2) was of a magnitude similar to that of nutrients such as filterable Fe (3.0 mmol m‐2) and lower than that of dissolved Si (18.5 mmol m‐2). Our results show that filterable Al concentrations in meltwater are significantly correlated to filterable and dissolved glacier‐derived nutrients (Fe and Si, respectively) concentrations in glaciers worldwide. We conclude that a potential bioavailable Al pool derived from glacierised basins may be incorporated in biogeochemical cycles, as it is strongly related to the concentrations and yields of glacier‐derived nutrients.  相似文献   

15.
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16.
The Agua Negra drainage system (30 12′S, 69 50′ W), in the Argentine Andes holds several ice‐ and rock‐glaciers, which are distributed from 4200 up to 6300 m a.s.l. The geochemical study of meltwaters reveals that ice‐glaciers deliver a HCO3?? Ca2+ solution and rock‐glaciers a SO42?? HCO3?? Ca2+ solution. The site is presumably strongly influenced by sublimation and dry deposition. The main processes supplying solutes to meltwater are sulphide oxidation (i.e. abundant hydrothermal manifestations), and hydrolysis and dissolution of carbonates and silicates. Marine aerosols are the main source of NaCl. The fine‐grained products of glacial comminution play a significant role in the control of dissolved minor and trace elements: transition metals (e.g. Mn, Zr, Cu, and Co) appear to be selectively removed from solution, whereas some LIL (large ion lithophile) elements, such as Sr, Cs, and major cations, are more concentrated in the lowermost reach. Daily concentration variation of dissolved rare earth elements (REE) tends to increase with discharge. Through PHREEQC inverse modelling, it is shown that gypsum dissolution (i.e. sulphide oxidation) is the most important geochemical mechanism delivering solutes to the Agua Negra drainage system, particularly in rock‐glaciers. At the lowermost reach, the chemical signature appears to change depending on the relative significance of different meltwater sources: silicate weathering seems to be more important when meltwater has a longer residence time, and calcite and gypsum dissolution is more conspicuous in recently melted waters. A comparison with a non‐glacierized semiarid drainage of comparable size shows that the glacierized basin has a higher specific denudation, but it is mostly accounted for by relatively soluble phases (i.e. gypsum and calcite). Meltwater chemistry in glacierized arid areas appears strongly influenced by sublimation/evaporation, in contrast with its humid counterparts. Copyright © 2007 John Wiley & Sons, Ltd.  相似文献   

17.
A critical evaluation of literature values for the solubility products, K sp NBS = [Fe2+][HS–] Fe2+ HS– (H NBS + )–1, of various iron sulphide phases results in consensus values for the pKs of 2.95 ± 0.1 for amorphous ferrous sulphide, 3.6 ± 0.2 for mackinawite, 4.4 ± 0.1 for greigite, 5.1 ± 0.1 for pyrrhotite, 5.25 ± 0.2 for troilite and 16.4 ± 1.2 for pyrite.Where the analogous ion activity products have been measured in anoxic freshwaters in which there is evidence for the presence of solid phase FeS, the values lie within the range of 2.6–3.22, indicating that amorphous iron sulphide is the controlling phase. The single value for a groundwater of 2.65 (2.98 considering carbonate complexation) agrees. In seawater four values range between 3.85 to 4.2, indicating that mackinawite or greigite may be the controlling phase. The single low value of 2.94 is in a situation where particularly high fluxes of Fe (II) and S (–II) may result in the preferential precipitation of amorphous iron sulphide. Formation of framboidal pyrite in these sulphidic environments may occur in micro-niches and does not appear to influence bulk concentrations. Calculations show that the formation of Fe2S2 species probably accounts for very little of the iron or sulphide in most natural waters. Previously reported stability constants for the formation of Fe (HS)2 and (Fe (HS)3)– are shown to be suspect, and these species are also thought to be negligible in natural waters. In completely anoxic pore waters polysulphides also have a negligible effect on speciation, but in tidal sediments they may reach appreciable concentrations and lead to the direct formation of pyrite. Concentrations of iron and sulphide in pore waters can be controlled by the more soluble iron sulphide phase. The change in the IAP with depth within the sediment may reflect ageing of the solid phase or a greater flux of Fe (II) and S (–II) nearer the sediment surface. This possible kinetic influence on the value of IAPs has implications for their use in geochemical studies involving phase formation.  相似文献   

18.
Abstract

A time series survey was carried out in 2002 to understand the hydrogeochemical processes taking place in the Achankovil River of the Western Ghats Range. The water is neutral with pH and EC ranges from 6.32 to 7.56 and 24–54 µS cm?1, respectively. Chloride and sodium are the dominant anion and cation in the water respectively. Correlation analysis of the chemical parameters of the water shows that few ions have additional sources. The majority of carbonate is derived from carbonate weathering followed by silicate weathering. Cation concentrations show decreasing trend from upstream to downstream in contrast to the increasing trend in the major world rivers. Dissolved silica in pre-monsoon water is low. The river chemistry is dominated by rock weathering induced by precipitation. Thermodynamic plots show that dolomite, kaolinite, albite and chlorite are in equilibrium with the river water. Chemical weathering is predominant here compared to physical weathering. The overall material transport seems to be lower compared to the other Indian rivers; nevertheless, the solute loads are comparable to certain large rivers such as the River Cauvery in southern India. The solute flux including the nutrient flux is very high among the Western Ghats rivers in relation to its size, which will certainly supplement the productivity of the lake/estuary and the coastal waters. Since this study is restricted to a one-year period, long-term data procurement and analysis along with micro nutrients studies are needed, which are lacking in the present study, to gain insight into the material flux by this river into the Arabian Sea.  相似文献   

19.
Nearly 200 analyses of meltwaters, ice and snow from three alpine glacial sites in carbonate terrain are summarized and discussed in terms of sources of solutes and kinetic controls on the progress of weathering reactions. Most data derive from the Swiss Glacier de Tsanfleuron which is based on Cretaceous and Tertiary pure and impure limestones. Two other sites (Marmolada, Italian Dolomites and the Saskatchewan Glacier, Alberta) are based on a mixed calcitic-dolomitic substrate. Most solutes originate from carbonate dissolution; moreover, where pyrite is present its oxidation supplies significant sulphate and forces more dissolution of carbonate. The ratios Sr2+/Ca2+ and Mg2+/Ca2+ are much higher in Tsanfleuron melt-waters than local bedrock, a phenomenon that can be reproduced in the laboratory at small percentages of dissolution. These anomalous ratios are attributed to incongruent dissolution of traces of the metastable carbonates Mg-calcite and aragonite. These phases also provide Na+ to solution. K+ is argued to originate mainly by ion-exchange on clays with solute Ca2+. Quartz and very minor feldspar dissolution are also inferred. Locally enhanced input from atmospheric sources is recognized by high Cl? and associated Na+. The progress of weathering reactions has been evaluated by the trends in the data, computer modelling and some simple laboratory experiments. The most dilute samples show a trend towards removal of CO2 to low partial pressures (c. 10?5.5 atmospheres), reflecting initially rapid carbonate dissolution and relatively slow dissolution of gaseous CO2. Later addition of atmospheric CO2 or acid from pyrite oxidation allows further carbonate dissolution, but solutions show a wide range of saturations, and CO2 pressures as high as 10?2.2 where pyrite oxidation is important. In a carbonate terrain, measurement of electroconductivity (corrected to 25°C) and alkalinity in the field allows the following preliminary deductions (where meq stands for milliequivalents): where S is the minimum meq(Ca2+ + Mg2+) produced by simple dissolution of carbonate unconnected with pyrite oxidation. As with any proxy method, these deductions do not remove the need for chemical analysis of waters in a given study area.  相似文献   

20.
This paper presents new estimates of solute fluxes from five high Arctic glacier basins in Svalbard. These estimates are combined with data from two other glacier basins to assess the effectiveness of chemical denudation on Svalbard and to estimate rates of temporary (or transient) CO2 drawdown. We use a solute provenance model to partition solutes into marine, aerosol, atmospheric and crustal components and to estimate their annual fluxes. Crustally derived solute fluxes are equivalent to a mean chemical denudation rate of 350 Σmeq+ m−2 a−1 for Svalbard (range: 160–560 Σmeq+ m−2 a−1), which lies within the global range of 94–4200 Σmeq+ m−2 a−1 for 21 glacier basins in the northern hemisphere, and is close to the continental average of 390 Σmeq+ m−2 a−1. Specific annual discharge is the most significant control upon chemical denudation in the glacierized basins, and basin lithology is an important secondary control, with carbonate‐rich and basaltic lithologies currently showing the greatest chemical denudation rates. Estimates of transient CO2 drawdown are also directly associated with specific annual discharge and rock type. On Svalbard transient CO2 drawdown lies in the range 110–3000 kg C km−2 a−1, whilst the range is 110–13000 kg C km−2 a−1 for the northern hemisphere glacial data set. Transient CO2 drawdown is therefore usually low in the Svalbard basins unless carbonate or basalt rocks are abundant. The analysis shows that a large area of uncertainty in the transient CO2 drawdown estimates exists due to the non‐stoichiometric release of solute during silicate hydrolysis. Silicate hydrolysis is particularly non‐stoichiometric in basins where the extent of glacierization is high, which is most probably an artefact of high flushing rates through ice‐marginal and subglacial environments where K‐feldspars are undergoing mechanical comminution. Copyright © 2000 John Wiley & Sons, Ltd.  相似文献   

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