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1.
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   

2.
Most sulphur diagenesis models predict that SO42- concentrations decrease exponentially with increasing sediment depth and are lower than that of the overlying water throughout the sediments. Low SO42- concentrations (less than 0.2 mM) are common in the sediments of Lake Anna that receive acid mine drainage; however, sediment with as much as 20 mM SO42- at about 20cm below the sediment surface is also seen in this section of the lake. A decision tree was proposed to investigate the cause of the high SO42- concentrations at depth (HSD) in the sediment. The first possibility proposed was that an increase in the quantity of groundwater flowing through Lake Anna sediments may increase groundwater advection of SO42- or oxygen which would induce sulphide oxidation. This hypothesis was tested by measuring groundwater flow. HSD profiles were found in a discrete region of the lake; however, stations having these profiles did not have higher groundwater flow than other sites sampled. Alternate explanations for the HSD profiles were that the region in which they occurred had: (1) unusual sediment chemical compositions; (2) a different source of regional groundwater, or (3) a lateral intrusion of high SO42- groundwater. There were no differences in sulphide and organic matter concentrations between the two regions. The area which has HSD in the sediment covers a large area in the middle of the lake, so it is unlikely that it has a unique source of regional groundwater. The third alternative was supported by the fact that in all three sample years, HSD stations were located in the preimpoundment stream channel, which is a likely lateral flow path for groundwater containing high SO42- concentrations.  相似文献   

3.
Waters were sampled from 17 boreholes at Haut Glacier d'Arolla during the 1993 and 1994 ablation seasons. Three types of concentrated subglacial water were identified, based on the relative proportions of Ca2+, HCO3? and SO42? to Si. Type A waters are the most solute rich and have the lowest relative proportion of Si. They are believed to form in hydrologically inefficient areas of a distributed drainage system. Most solute is obtained from coupled sulphide oxidation and carbonate dissolution (SO–CD). It is possible that there is a subglacial source of O2, perhaps from gas bubbles released during regelation, because the high SO42? levels found (up to 1200 µeq/L) are greater than could be achieved if sulphides are oxidized by oxygen in saturated water at 0 °C (c.414 µeq/L). A more likely alternative is that sulphide is oxidized by Fe3+ in anoxic environments. If this is the case, exchange reactions involving FeIII and FeII from silicates are possible. These have the potential to generate relatively high concentrations of HCO3? with respect to SO42?. Formation of secondary weathering products, such as clays, may explain the low Si concentrations of Type A waters. Type B waters were the most frequently sampled subglacial water. They are believed to be representative of waters flowing in more efficient parts of a distributed drainage system. Residence time and reaction kinetics help determine the solute composition of these waters. The initial water–rock reactions are carbonate and silicate hydrolysis, and there is exchange of divalent cations from solution for monovalent cations held on surface exchange sites. Hydrolysis is followed by SO–CD. The SO42? concentrations usually are <414 µeq/L, although some range up to 580 µeq/L, which suggests that elements of the distributed drainage system may become anoxic. Type C waters were the most dilute, yet they were very turbid. Their chemical composition is characterized by low SO42? : HCO3? ratios and high pH. Type C waters were usually artefacts of the borehole chemical weathering environment. True Type C waters are believed to flow through sulphide‐poor basal debris, particularly in the channel marginal zone. The composition of bulk runoff was most similar to diluted Type B waters at high discharge, and was similar to a mixture of Type B and C waters at lower discharge. These observations suggest that some supraglacial meltwaters input to the bed are stored temporarily in the channel marginal zone during rising discharge and are released during declining flow. Little of the subglacial chemical weathering we infer is associated with the sequestration of atmospheric CO2. The progression of reactions is from carbonate and silicate hydrolysis, through sulphide oxidation by first oxygen and then FeIII, which drives further carbonate and silicate weathering. A crude estimate of the ratio of carbonate to silicate weathering following hydrolysis is 4 : 1. We speculate that microbial oxidation of organic carbon also may occur. Both sulphide oxidation and microbial oxidation of organic carbon are likely to drive the bed towards suboxic conditions. Hence, we believe that subglacial chemical weathering does not sequester significant quantities of atmospheric CO2 and that one of the key controls on the rate and magnitude of solute acquisition is microbial activity, which catalyses the reduction of FeIII and the oxidation of FeS2. Copyright © 2002 John Wiley & Sons, Ltd.  相似文献   

4.
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   

5.
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   

6.
南极洲万达盐湖为饱和方解石湖水。计算出的方解石饱和指数随水深增加而变化。在Ca2+及HCO3-活度值均一的上部氧化环境湖水中,pH及溶解氧(DO)是控制该变化的主要因素,在下部还原环境湖水中,Ca2+及HCO3-的活度对方解石的饱和指数SI的变化起主要作用。这充分揭示了湖底部近代沉积物中分布较多方解石矿物的原因。  相似文献   

7.
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   

8.
A heterogeneous chemical model is developed by coupling aerosol, gas-phase and liquid-phase chemical model. SO2 oxidation rates on the aerosol surface are calculated and the influence of some factors is discussed. Model simulations indicate that SO2 heterogeneous oxidation rates are sensitive to the mass concentration and chemical composition of aerosols, relative humidity, initial values of SO2 and H2O2. The heterogeneous chemical model is coupled with a Eulerian deposition model. Model results show that oxidation of SO2 on the aerosol surface is found to reduce SO2 levels by 5%–33%, to increase SO 4 2- - concentrations by 8%–50% in the surface layer. Project supported by the National “85-912” Key Science and Technology Project.  相似文献   

9.
Multiple sulfur and oxygen isotope compositions in Beijing aerosol   总被引：1，自引：0，他引：1  
Multiple sulfur isotopes(32S, 33 S, 34 S, 36S) and oxygen isotopes(16O, 18O) in Beijing aerosols were measured with MAT-253 isotope mass spectrometer. The δ34S values of Beijing aerosol samples range from 1.68‰ to 12.57‰ with an average value of 5.86‰, indicating that the major sulfur source is from direct emission during coal combustion. The δ18O values vary from 5.29‰ to 9.02‰ with an average value of 5.17‰, revealing that the sulfate in Beijing aerosols is mainly composed of the secondary sulfate. The main heterogeneous oxidation of SO2 in atmosphere is related to H2O2 in July and August, whereas H2O2 oxidation and Fe3+ catalytic oxidation with SO2 exist simultaneously in September and October. Remarkable sulfur isotope mass-independent fractionation effect is found in Beijing aerosols, which is commonly attributed to the photochemical oxidation of SO2 in the stratosphere. In addition, thermochemical reactions of sulfur-bearing compounds might be also a source of sulfur isotope anomalies based on the correlation between ?33S and CAPE.  相似文献   

10.
The use of the sulphate mass balance (SMB) between precipitation and soil water as a supplementary method to estimate the diffuse recharge rate assumes that the sulphate in soil water originated entirely from atmospheric deposition; however, the origin of sulphate in soil and groundwater is often unclear, especially in loess aquifers. This study analysed the sulphur (δ34S-SO4) and oxygen (δ18O-SO4) isotopes of sulphate in precipitation, water-extractable soil water, and shallow groundwater samples and used these data along with hydrochemical data to determine the sources of sulphate in the thick unsaturated zone and groundwater of a loess aquifer. The results suggest that sulphate in groundwater mainly originated from old precipitation. When precipitation percolates through the unsaturated zone to recharge groundwater, sulphates were rarely dissolved due to the formation of CaCO3 film on the surface of sulphate minerals. The water-extractable sulphate in the deep unsaturated zone (>10 m) was mainly derived from the dissolution of evaporite minerals and there was no oxidation of sulphide minerals during the extraction of soil water by elutriating soil samples with deionized water. The water-extractable concentration of SO4 was not representative of the actual SO4 concentration in mobile soil water. Therefore, the recharge rate cannot be estimated by the SMB method using the water-extractable concentration of SO4 in the loess areas. This study is important for identifying sulphate sources and clarifying the proper method for estimating the recharge rate in loess aquifers.  相似文献   

11.
The method after Strickland and Parsons is modified for fresh water as follows: filtration on glass-fibre paper, oxidation with K2Cr2O7 in cone. H2SO4 for 2 h at 130 °C, dilution to 2.5 times the volume by aqua dest., centrifuging-off of the turbidity and extinction measurement at 445 nm against the blank value, the sample solution being balanced to the transmission of 100% (extinction = 0). Here, the following calibration line holds for the concentration C and the quantity of oxidation solution Ox: C = E1cmc · 0.162 · Ox, C in mg filter. The oxidation solution contains 4.8 g K2Cr2O7 as dissolved in 20 ml aqua dest. and made up with conc. H2SO4 to 11. With 5 ml of this solution one is able to determine 0.05 … 1 mg C/filter. Calibration is performed with 125 mg/l glucose solution. Comparative investigations have shown a good agreement with elementary-analytically obtained measured values. The occurring errors have been determined mainly by sampling. In the range of very small values we have to take into account a blank value of the filter due to the adsorption of dissolved organic substances on the filter.  相似文献   

12.
淮北临涣矿采煤沉陷区不同水体水化学特征及其影响因素   总被引：3，自引：0，他引：3  
为研究淮北临涣矿采煤沉陷区不同水体的补给水源及溶质来源,在现场调查的基础上,系统采集丰水期、平水期、枯水期沉陷区积水、地表河水和浅层地下水样进行测试分析,采用Piper三线图、Gibbs图和因子分析方法,对不同水体水化学特征及其影响因素进行讨论.结果表明:地表水水体总溶解性固体(TDS)质量浓度表现为枯水期丰水期平水期,浅层地下水表现为枯水期平水期丰水期,地表水TDS质量浓度明显高于浅层地下水.地表水中主要阴阳离子为Na~+、Cl~-和SO_4~(2-),水化学类型主要为SO_4~(2-)-Cl~--Na~+型;浅层地下水离子以HCO_3~-、Ca~(2+)和Mg~(2+)为主,表现为HCO_3~--Ca~(2+)-Mg~(2+)型.结合Gibbs图和因子分析可知,地表水受蒸发作用、地表径流以及采煤活动等因素影响,浅层地下水在一定程度上体现出大气降水和地表水补给的特点,受岩石风化作用影响较为明显.  相似文献   

13.
Samples from Kawah Ijen crater lake, spring and fumarole discharges were collected between 1990 and 1996 for chemical and isotopic analysis. An extremely low pH (<0.3) lake contains SO4–Cl waters produced during absorption of magmatic volatiles into shallow ground water. The acidic waters dissolve the rock isochemically to produce “immature” solutions. The strong D and 18O enrichment of the lake is mainly due to enhanced evaporation at elevated temperature, but involvement of a magmatic component with heavy isotopic ratios also modifies the lake D and 18O content. The large ΔSO4–S0 (23.8–26.4‰) measured in the lake suggest that dissolved SO4 forms during disproportionation of magmatic SO2 in the hydrothermal conduit at temperatures of 250280°C. The lake δ18OSO4 and δ18OH2O values may reflect equilibration during subsurface circulation of the water at temperatures near 150°C. Significant variations in the lake's bulk composition from 1990 to 1996 were not detected. However, we interpret a change in the distribution and concentration of polythionate species in 1996 as a result of increased SO2-rich gas input to the lake system.Thermal springs at Kawah Ijen consist of acidic SO4–Cl waters on the lakeshore and neutral pH HCO3–SO4–Cl–Na waters in Blawan village, 17 km from the crater. The cation contents of these discharges are diluted compared to the crater lake but still do not represent equilibrium with the rock. The SO4/Cl ratios and water and sulfur isotopic compositions support the idea that these springs are mixtures of summit acidic SO4–Cl water and ground water.The lakeshore fumarole discharges (T=170245°C) have both a magmatic and a hydrothermal component and are supersaturated with respect to elemental sulfur. The apparent equilibrium temperature of the gas is 260°C. The proportions of the oxidized, SO2-dominated magmatic vapor and of the reduced, H2S-dominated hydrothermal vapor in the fumaroles varied between 1979 and 1996. This may be the result of interaction of SO2-bearing magmatic vapors with the summit acidic hydrothermal reservoir. This idea is supported by the lower H2S/SO2 ratio deduced for the gas producing the SO4–Cl reservoir feeding the lake compared with that observed in the subaerial gas discharges. The condensing gas may have equilibrated in a liquid–vapor zone at about 350°C.Elemental sulfur occurs in the crater lake environment as banded sediments exposed on the lakeshore and as a subaqueous molten body on the crater floor. The sediments were precipitated in the past during inorganic oxidation of H2S in the lake water. This process was not continuous, but was interrupted by periods of massive silica (poorly crystallized) precipitation, similar to the present-day lake conditions. We suggest that the factor controlling the type of deposition is related to whether H2S- or silica-rich volcanic discharges enter the lake. This could depend on the efficiency with which the lake water circulates in the hydrothermal cell beneath the crater. Quenched liquid sulfur products show δ34S values similar to those found in the banded deposits, suggesting that the subaqueous molten body simply consists of melted sediments previously accumulated at the lake bottom.  相似文献   

14.
韩翠红  孙海龙  魏榆  鲍乾  晏浩 《湖泊科学》2020,32(6):1683-1694
耦联水生光合作用的碳酸盐风化碳汇是全球碳循环的重要组成部分,而生物碳泵效应是稳定碳酸盐风化碳汇的关键机制.河流筑坝后,生物碳泵效应的变化、控制因素及对水化学影响的研究甚少.本研究对2个喀斯特筑坝河流平寨水库和红枫湖进行系统采样,以研究河流筑坝后生物碳泵效应的变化、控制因素及对水化学的影响.研究结果表明,入库河流的水化学变化不明显,而2个水库的水化学则表现出显著的季节变化特征,具体表现为水库的水温和pH均呈现出夏季高、冬季低的变化特征,而电导率（EC）、HCO3-浓度和pCO2则表现出夏季低、冬季高的季节变化特征.以叶绿素a（Chl.a）浓度和溶解氧（DO）饱和度指代的生物碳泵效应则是在夏季最强、冬季最弱.生物碳泵效应利用溶解性无机碳（DIC）,形成有机质并释放出氧气,是造成夏季水库pH值和DO饱和度升高,电导率（EC）、HCO3-浓度和pCO2降低的主要因素.空间上,水库的Chl.a浓度及DO饱和度均大于河水,EC、HCO3-浓度和pCO2均小于河水,这表明河流筑坝后,由于水库的“湖泊化”导致水库的生物碳泵效应显著提高.通过对Chl.a与碳、氮和磷浓度及化学计量比的相关性分析发现,平寨水库和红枫湖的生物碳泵效应受到碳施肥的影响.平寨水库和红枫湖水库生物碳泵效应碳施肥机制的发现,表明在喀斯特地区,生物碳泵效应不仅受到氮磷元素的控制,也受到碳元素的控制,因此在富营养化湖泊治理时,也应考虑碳的影响.  相似文献   

15.
Ambient concentrations of sulfur dioxide (SO2), nitrogen dioxide (NO2), and ozone (O3) were measured at 51 sampling points by passive sampling technique in Kocaeli, an important industrial city in Turkey. Samples were analyzed by UV‐spectrophotometry for NO2 and O3 and by ion chromatography for SO2, respectively. Concentrations of SO2, NO2, and O3 were determined to investigate their spatial distribution and source characterization. The sampling campaigns revealed an average concentration of 8 µg/m3 (max. 82 µg/m3) for SO2, and 14 µg/m3 (max. 40 µg/m3) for NO2, in summer; while average winter concentrations were 25 µg/m3 (max. 61 µg/m3) for SO2, and 50 µg/m3 (max. 100 µg/m3) for NO2. The maximum ozone concentrations were determined to be 86 µg/m3 in summer and 61 µg/m3 in winter downwind of the source areas of the precursor pollutant emissions. The results showed that NO2 and SO2 concentrations in industrial and urban areas were two to four times higher compared with rural areas in the summer and winter. In the light of the information obtained from the spatial interpolation of the pollutant concentrations, a selection of appropriate locations for continuous monitoring was suggested according to the European Community (EU) directives.  相似文献   

16.
邓焕广  张智博  刘涛  殷山红  董杰  张菊  姚昕 《湖泊科学》2019,31(4):1055-1063
为了解城市湖泊不同水生植被区水体温室气体的溶存浓度及其影响因素,于2015年4-11月按每月2次的频率采用顶空平衡法对聊城市铃铛湖典型植被区——菹草区、莲藕区和睡莲区表层水中CO2、CH4和N2O的溶存浓度进行监测,计算水中温室气体的饱和度和排放通量,并测定水温（T）、pH、溶解氧（DO）、叶绿素a及营养盐浓度等理化指标,以探究水体环境因子对温室气体溶存浓度的影响.结果表明,铃铛湖各植被区水体温室气体均处于过饱和状态,是大气温室气体的"源";莲藕区CH4浓度、饱和度和排放通量均显著高于菹草区,而各植被区N2O和CO2均无显著性差异;不同植被区湖水中DO、总氮（TN）、总磷（TP）和硝态氮（NO3--N）浓度具有显著差异,其中DO、TN和NO3--N浓度均表现为菹草区最高,莲藕区最低,而TP浓度则正好相反;各植被区温室气体浓度和水环境参数间的相关分析和多元回归分析的结果表明,水生植物可通过影响水体的理化性质对温室气体的产生和排放产生显著差异影响,在菹草区亚硝态氮（NO2--N）、NO3--N、T和DO是控制水体温室气体浓度的主要因子;睡莲区为TP和pH;莲藕区则为pH、NO2--N和DO.  相似文献   

17.
通过模拟沙湖沉积物-水系统,以沙湖原水氟离子（F-）浓度为1倍浓度（0.69 mg/L）,设置0.5倍浓度、1倍浓度、1倍浓度灭菌、2倍浓度和4倍浓度共5个实验组,探究不同上覆水F-浓度背景下沙湖沉积物中F-的迁移.结果表明,沉积物F-的释放量随上覆水F-浓度的增加而呈下降的趋势,其中2倍和4倍浓度组的沉积物由释放F-转变为吸附F-.碱性水体有利于沉积物F-的释放,即随着pH增大,F-释放量也会增加.微生物的Beta多样性层次聚类分析表明,F-会抑制Paenisporosarcina与Thiobacillus的相对丰度,但对Fusibacter的生命活动具有促进作用.根据各浓度组间优势菌属相对丰度与环境因子的冗余分析可得,Acinetobacter、Thiobacillus相对丰度与pH呈负相关;Fusibacter相对丰度与F-浓度呈显著正相关,而Thiobacillus的相对丰度则与F-表现出弱负相关.通过对各浓度组中重要离子的分析发现,0.5倍组和4倍组中F-的迁移受Ca2+、HCO3-和SO42-浓度影响较大;相关性分析表明0.5倍浓度组的Ca2+、HCO3-浓度与F-浓度呈极显著正相关,而4倍组中F-浓度和Ca2+、HCO3-浓度呈负相关,SO42-浓度和F-浓度的相关性则是0.5倍组呈负相关,4倍组呈极显著正相关.本文在不同上覆水F-浓度背景下全面探究了沙湖沉积物中F-释放和迁移机理,为沙湖及其他含氟地表水的氟污染防治提供理论支持.  相似文献   

18.
A detailed geochemical-petrological examination of layer 2 basalts recovered during Leg 37 of the DSDP has revealed that the original distribution, form and abundance of igneous sulfide have been profoundly altered during low-grade oxidative diagenesis. The net result appears to have been a rather pervasive remobilization of igneous sulfide to form secondary pyrite accompanied by a bulk loss of sulfur equivalent to about 50–60% of the original igneous value, assuming initial saturation. It is suggested that during infiltration of seawater into the massive crystal-line rock, igneous sulfide has experienced pervasive oxidation, under conditions of limited oxidation potential, to form a series of unstable, soluble sulfur species, primarily in the form of SO32? and S2O32?. Spontaneous decomposition of these intermediate compounds through disproportionation has resulted in partial reconstitution of the sulfur as secondary pyrite and the generation of SO42? ion, which, due to its kinetic stability, has been lost from the basalt system and ultimately transferred to the ocean. This model not only satisfies the geochemical and petrological observations but also provides a suitable explanation for the highly variable δ34S values which characterize secondary sulfides in deep ocean floor basalts.  相似文献   

19.
自2005年以来,程海水体的化学需氧量(COD)持续升高,而生化需氧量(BOD)却维持不变,高锰酸盐指数(COD_(Mn))升高也较缓慢.为研究程海COD持续升高的原因,选取程海水体中具有代表性的无机阴离子(Cl~-、F~-、S~(2-)、HCO_3~-)和溶解性有机质(DOM)中不同浓度的胡敏酸(HA)、富里酸(FA)和商品化腐殖酸(SHA),研究其对COD和COD_(Mn)测定的影响,探讨Cl~-和DOM共同存在下对COD测定的影响.结果表明:程海水体中Cl~-浓度对COD存在显著影响,产生的COD值为5.42 mg/L,S~(2-)、F~-和HCO_3~-对COD影响较小;各离子对COD_(Mn)的影响很小;不同浓度梯度的HA、FA和SHA与COD测定结果呈显著线性相关,氧化1 mg C HA、FA和SHA所产生的COD值分别为2.164、1.964和2.362 mg;氧化1 mg C HA和FA所产生的COD_(Mn)值分别为0.646和0.344 mg;DOM对COD测定值的影响显著大于对COD_(Mn)测定值的影响;且一定浓度Cl~-的存在增强了FA与HA对COD测定的影响.该研究为进一步阐明程海COD逐步升高,COD_(Mn)值缓慢升高的内在原因奠定了基础.  相似文献   

20.
The origin and the chemical and isotopic evolution of dissolved inorganic carbon (DIC) in groundwater of the Okavango Delta in semi-arid Botswana were investigated using DIC and major ion concentrations and stable oxygen, hydrogen and carbon isotopes (δD, δ18O and δ13CDIC). The δD and δ18O indicated that groundwater was recharged by evaporated river water and unevaporated rain. The river water and shallow (<10 m) groundwater are Ca–Na–HCO3 type and the deep (≥10 m) groundwater is Na–K–HCO3 to HCO3–Cl–SO4 to Cl–SO4–HCO3. Compared to river water, the mean DIC concentrations were 2 times higher in shallow groundwater, 7 times higher in deep groundwater and 24 times higher in island groundwater. The δ13CDIC indicate that DIC production in groundwater is from organic matter oxidation and in island groundwater from organic matter oxidation and dissolution of sodium carbonate salts. The ionic and isotopic evolution of the groundwater relative to evaporated river water indicates two independent pools of DIC.  相似文献   

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