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1.
岩溶区河流水化学昼夜变化与生物地球化学过程   总被引:6,自引:3,他引:3  
章程 《中国岩溶》2015,34(1):1-8
河流水化学昼夜动态变化的研究有助于揭示水体中相对快速的生物地球化学过程(河流内过程),同时也有助于判别上游补给区流域过程。已有的研究表明生物过程(光合作用与呼吸作用)、地球化学过程(碳酸盐平衡、碳酸钙沉积)是控制河流pH、SpC、Ca2+和HCO3-含量昼夜变化的主要因素。不同级别、类型及河床微环境均会对水化学昼夜变化产生影响,与气温密切相关的光合作用是产生河水pH值和DO昼夜变化的主控因素。在偏碱性与富含钙离子的岩溶河流,有机体的钙化作用与酸分泌可能对光合作用具有重要作用,从而导致水体中Ca2+和HCO3-出现白天下降-夜间回升的昼夜动态变化,下降幅度达20%~30%。水生植物通过光合作用产生DIC(主要为HCO3-)的原位沉降,是真正意义上的净碳汇。昼夜生物地球化学循环及效应研究有助于全面认识岩溶区碳循环特征及岩溶含水层源汇关系,尤其是岩溶碳汇稳定性与净碳汇估算;同时对长时间尺度河流监测计划的制定具有重要意义。   相似文献   

2.
Acid mine drainage was reacted with coal fly ash over a 24 h reaction time and species removal trends evaluated. The evolving process water chemistry was modeled by the geochemical code PHREEQC using WATEQ4 database. Mineralogical analysis of the resulting solid residues was done by X-ray diffraction analysis. Selective sequential extraction was used to evaluate the transfer of species from both acid mine drainage and fly ash to less labile mineral phases that precipitated out. The quantity of fly ash, volume of acid mine drainage in the reaction mixture and reaction time dictated whether the final solution at a given contact time will have a dominant acidic or basic character. Inorganic species removal was dependent on the pH regime generated at a specific reaction time. Sulphate concentration was controlled by precipitation of gypsum, barite, celestite and adsorption on iron-oxy-hydroxides at pH > 5.5. Increase of pH in solution with contact time caused the removal of the metal ions mainly by precipitation, co-precipitation and adsorption. PHREEQC predicted precipitation of iron, aluminium, manganese-bearing phases at pH 5.53–9.12. An amorphous fraction was observed to be the most important in retention of the major and minor species at pH > 6.32. The carbonate fraction was observed to be an important retention pathway at pH 4–5 mainly due to initial local pockets of high alkalinity on surfaces of fly ash particles. Boron was observed to have a strong retention in the carbonate fraction.  相似文献   

3.
Concern about arsenic is increasing throughout the world, including areas of the United States. Elevated levels of arsenic above current drinking-water regulations in ground and surface water can be the result of purely natural phenomena, but often are due to anthropogenic activities, such as mining and agriculture. The current study correlates arsenic speciation in acid mine drainage and mining-influenced water with the important water-chemistry properties Eh, pH, and iron(III) concentration. The results show that arsenic speciation is generally in equilibrium with iron chemistry in low pH AMD, which is often not the case in other natural-water matrices. High pH mine waters and groundwater do not always hold to the redox predictions as well as low pH AMD samples. The oxidation and precipitation of oxyhydroxides deplete iron from some systems, and also affect arsenite and arsenate concentrations through sorption processes.  相似文献   

4.
Quantitative mineralogy correlates with major-, minor- and trace-element chemistry for 387 samples of A-horizon and deeper soils collected from east–west and north–south transects across the USA and Canada, where the deeper soils were collected beneath the A-horizon samples. Concentrations of the major elements correlate with specific mineral phases. Minor- and trace-element concentrations correlate with the same phases as the major elements with which they share similar geochemical behavior. Concentrations of quartz and feldspar correlate with precipitation trends east of the Rocky Mountains, and are independent of the underlying rock type and age, indicating that the weathering of soils in this region may have reached a steady-state mineralogy. Other trends in mineralogy relate to physiographic province. The combination of quantitative mineralogy and chemical analysis yields a much richer portrait of soils than can be gained from chemistry alone, because the origins of chemical trends and the chemical availability of specific elements are related to mineralogy.  相似文献   

5.
Seasonal variations of water chemistry occurred in acid mine drainage receiving mine and leachate water. Sulfate and metal concentrations were low in winter but high in spring and summer. Mine waters were highly acidic (up to pH 3.4) in nature with high concentrations of manganese, copper and zinc but high electrical conductivity and sulfate in leachate. The blue and brownish yellow precipitates were formed under different chemical environments of acid mine drainage. Brownish yellow (Munsell color 7.5YR 8/12), blue (Munsell color 2.5B 9/7) and light blue (Munsell color 2.5B 9/3) precipitates deposited on the stream bottom receiving acid mine water. The brownish yellow precipitates formed in the acid mine water, whereas the blue and light blue precipitates formed in the leachate water. The brownish yellow precipitates consisted mainly of ferrihydrite, whereas the blue and light blue precipitates consisted of glaucocerinite and/or woodwardite.  相似文献   

6.
The study of supergene processes (i.e., secondary processes running in ore deposits and driven by thermodynamic nonequilibrium between ore-and rock-forming minerals and natural waters, gasses, etc.) is important in order to understand the migration of heavy metals from ore into their adjacent surroundings. The contamination of the local environment can be characterized by the composition of pore waters. The Pb-Zn-Cu ore deposits of Zlaté Hory (Czech Republic) have been chosen for a detailed study of pore solutions. A simple model has been created to describe the evolution of supergene processes in the ore deposits. This model is based on the determination of chemical composition of pore solutions. The dilution of pore solutions of such mineral deposits results in acid mine drainage. Pore solutions can have, during specific stages of their evolution, relatively high concentrations of Cu (0.09 mol/kg), Zn (0.1 mol/kg), SO4 (0.8 mol/kg) and an extremely low pH (1.38). The supergene alteration of pyrite is the most important process determining the character of pore water. This reaction causes significant acidification and is a leading source of acid mine drainage. The leached zone originates from the interaction of pyrite and limonite. Increased concentrations of heavy metals and sulfates occur in pore waters. The dynamic composition of pore waters within ore deposits undergoing the supergene process can be used to distinguish: (1) three main zoneslimonite, transition, and primary zone and (2) two areas—an area with the highest intensity of weathering processes and an area of weathering initiation. In these areas the rate of sulfide oxidation is higher as a result of low pH. From the study of these zones and areas we can further our knowledge of ore body, pore solution, acid mine drainage, and contamination of the local environment.  相似文献   

7.
Acid–base accounting (ABA) is a static test used to evaluate pre-mining drainage quality of ores with interpretations based on a reference 3-data point model. The method is often complemented with a kinetic test to ensure certainty of results. The challenges associated with both methods compel companies to rely on only the ABA test, thereby compromising on the long-term drainage quality. This paper validates a proposed 4-data point model that was used to establish a 20% increase in the alkaline amendment of ores at the AngloGold Ashanti Obuasi Mine in Ghana. The validation was done using model limits, the robustness of coefficient of determination and model factor sequence variation. Acidification trends and mineralogical data evaluation of tailings were used to characterise pH buffer trends in mine drainage. The modified 4-data point model, which incorporates a vital kinetic test factor into the ABA model, provides a criterion for the adjustment of carbonate amendment value to improve acid neutralisation in the drainage; this would reduce (1) cost of experimentation, (2) turnaround time for analyses, (3) complexities associated with both test methods. From the XRD data, alunite and goethite are present in tailings to provide sustained pH buffering in drainage beyond the scope of the modified model, while the characterised pH buffer trend could be used for monitoring drainage quality.  相似文献   

8.
The present work describes the process of acid water discharge into the Andévalo Dam (Iberian Pyrite Belt, Huelva-Spain) starting from the interpretation of rainfall data and chemical analyses regarding pH, conductivity, metal and sulphate content in water, from a time series corresponding to the sampling of two confluent channels that discharge water into the referred dam. Statistical data treatment allows us to conclude the existence of acid mine drainage processes in the Chorrito Stream, which are translated into very low pH values and high sulphate and metal concentrations in the water coming from Herrerías Mine. On the other hand, the Higuereta Stream shows, for the same parameters, much lower values that can be interpreted as the channel response to acid rock drainage processes in its drainage basin induced by the rocky outcrops of the Iberian Pyrite Belt.  相似文献   

9.
Evaluation of 12 years of landfill leachate chemical data from a lined cell of municipal waste in south Florida, USA shows an overall declining trend in major ion chemistry. The leachate is dominantly Cl, Na, HCO3 and organic solutes. There are significant short-term variations in concentration that appear to be related to rainfall, rather than fundamental changes to leachate composition. Inorganic parameters related to pH, such as alkalinity, calcium, and magnesium appear to be chemically buffered. Chromium, cobalt, vanadium, zinc, and the metalloid boron display significant short-term co-variance with a decreasing trend. Iron and manganese concentrations increased significantly after capping. Based on the predominance of ammonia, historic methane generation, and increasing trends for iron and manganese after closure, the landfill cell has an anaerobic (reducing) interior environment. The reducing conditions were enhanced by capping and caused the most redox sensitive metals (manganese and iron) to become more mobile.  相似文献   

10.
Metal cycling via physical and chemical weathering of discrete sources (copper mines) and regional (non-point) sources (sulfide-rich shale) is evaluated by examining the mineralogy and chemistry of weathering products in Great Smoky Mountains National Park, Tennessee, and North Carolina, USA. The elements in copper mine waste, secondary minerals, stream sediments, and waters that are most likely to have negative impacts on aquatic ecosystems are aluminum, copper, zinc, and arsenic because these elements locally exceed toxicity guidelines for surface waters or for stream sediments. Acid-mine drainage has not developed in streams draining inactive copper mines. Acid-rock drainage and chemical weathering processes that accompany debris flows or human disturbances of sulfidic rocks are comparable to processes that develop acid-mine drainage elsewhere. Despite the high rainfall in the mountain range, sheltered areas and intermittent dry spells provide local venues for development of secondary weathering products that can impact aquatic ecosystems.Electronic Supplementary Material  Supplementary material is available for this article if you access the article at . A link in the frame on the left on that page takes you directly to the supplementary material.
Jane M. HammarstromEmail: Phone: +1-703-6486165Fax: +1-703-6486252
  相似文献   

11.
Highly reducing and high-pH vent fluids characterize moderately low temperature ultramafic-hosted hydrothermal systems, such as the recently discovered Lost City hydrothermal field at 30°N Mid-Atlantic Ridge Ridge (MAR). To better understand the role of mineral reaction rates on changes in fluid chemistry and mineralization processes in these and similar systems, we conducted an experimental study involving seawater and peridotite at 200 °C, 500 bar. Time series changes in fluid chemistry were monitored and compared with analogous data predicted using experimental and theoretical data for mineral dissolution rates. Although there was qualitative agreement between predicted and measured changes in the chemical evolution of the fluid for some species, the rate and magnitude of increase in pH, dissolved chloride and H2 did not agree well with predictions based on theoretical modeling results. Experimental data indicate that dissolved H2 abruptly and intermittently increased, reaching a value only approximately 20% of that predicted assuming magnetite as the primary Fe-bearing alteration phase. The distribution and valence of Fe in primary and secondary minerals reveal that the most abundant secondary mineral, serpentine, contained significant amounts of both ferric and ferrous Fe, with the less abundant brucite, also being Fe-rich (XFe = 0.3). Surprisingly, magnetite was present in only trace amounts, indicating that H2 generation was largely accommodated by the formation of Fe-chrysotile. Accordingly, the diversity of Fe-bearing secondary minerals together with rates of serpentinization less than theoretically predicted, account best for the relatively low dissolved H2 concentrations produced. Thus, the experimental data can be used to obtain provisional estimates of thermodynamic data for Fe-bearing minerals, enhancing the application of reaction path models depicting mass transfer processes during serpentinization at mid-ocean ridges. Similarly, the observed differences between theoretically predicted and experimentally measured pH values result from constraints imposed by complex patterns of mass transfer inherent to the experimental system. In particular, the experimental observation of a late stage increase in Na/Cl ratio likely results from the dissolution of a Na2O component of clinopyroxene, which causes pH to increase sufficiently to induce precipitation of a Ca-bearing phase, perhaps portlandite. As with the redox variability observed during the experiment, this event could not be predicted, underscoring the need to use caution when modeling alteration processes in the chemically complex ultramafic-hosted hydrothermal systems at elevated temperatures and pressures.  相似文献   

12.
Hydrogeological monitoring was conducted around a pilot cavern for underground cryogenic LNG (Liquefied Natural Gas) storage. The monitoring was mainly focused on the operation of a drainage and recharge system. After the operation of the drainage system commenced, the drainage rate decreased rapidly in the initial stages and then decreased gradually. Hydrogeological monitoring revealed that the rock drainage system operated effectively. During drainage, the water table was maintained below the cavern roof. The recharge for ice-ring formation was performed in two phases. The first phase involved the cessation of pumping in downward-drainage holes and the second involved the closure of upward boreholes. Since the water table was maintained below the cavern roof, artificial recharge was planned at first. However, it was not implemented due to heavy rainfall in the recharge stage. On the basis of hydrogeological monitoring and hydraulic tests, it was found that the fractures above the roof and on the right wall of the pilot cavern mainly affected seepage into the cavern and thermal variation due to the storage of liquid nitrogen. Thermal variation was examined by the thermometers installed around the pilot cavern. The cooling and thawing processes reveal the characteristics of thermal distribution in the rock and the 0 °C isotherm. The cooling phase lasted for six months, and the 0 °C isotherm progressed in time after the injection of liquid nitrogen into the cavern. The isotherm propagated up to about 4 m from the floor and the sidewall of the cavern and about 3 m from the cavern roof. The cooling rate of the rock mass above the cavern roof was lower than that of the other cavern sides due to the gaseous space in the upper part of the containment. The fractures were analyzed and considered for thermal modeling. A two-dimensional finite element analysis was performed to compare the field monitoring at the pilot cavern. The numerical modeling shows the distance between the ice ring and heat transfer pattern of the fractures around the pilot cavern. The propagation of the measured and calculated 0 °C isotherm reveals that the water-conveying joint on the right wall might affect thermal propagation through a thermal pipe.  相似文献   

13.
Water from four north-flowing rivers (Oswegatchie, Grasse, Raquette, and West Branch of the St. Regis) traversing three distinct geologic terranes (Adirondack Highlands, Adirondack Lowlands, St. Lawrence Valley), originating in the acidified northern Adirondack region, display rapid spatial changes in downriver multi-element chemistry and physical parameters. Downriver, most soluble elements increase (Ba, Ca, Cu, K, Mg, Na, Rb, S, and Sr) while statistically significant decreases in insoluble elements (Al, Ce, Dy, Er, Fe, Gd, La, Mn, Nd, Pr, and Y) also occur. Lithium, Si, and Zr did not show a consistent increasing or decreasing trend. Concentrations of most elements measured on June 5, 2008 were greater than 7?weeks later; however, greater discharge and lower pH enhanced Al concentrations occurred during the later sampling date. Elemental ratios track changes in lithology, anthropogenic influence, and pH. The Raquette River shows the least variation in elemental concentrations because of storage in numerous hydropower reservoirs and has non-detectable concentrations of some redox sensitive elements such as Co, Ni, and V. Oswegatchie tributaries display similar geochemical trends dependent upon their location and local bedrock and show geochemical trends along the trunks of major rivers that are also evident in smaller drainage basins. Comparison with analytical results from the Western Adirondack Stream Survey also indicates acidification is prevalent in the Adirondack Highlands, particularly in the Oswegatchie headwaters during periods of high flow, but acidity is rapidly buffered downriver due to interaction with marble in the Adirondack Lowlands.  相似文献   

14.
Perturbation on the simplex is an operation which can be used to numerically describe changes in the composition of, for example, soils, sediments, or rocks. The combination of perturbation and power transformation provides a strong tool for analyzing compositional linear processes in the simplex. When the process is constrained in the sense of a well-known starting (or final) composition, noncentred principal component analysis can be used to estimate the leading perturbation vector of the process. Applying these mathematical tools to chemical major element data from a weathering profile developed on granitoid rocks allows us to model the compositional changes associated with the process of chemical weathering. The comparison of these results with the compositional linear trend defined by erosional products of several of the world's major drainage systems yields close similarities. The latter observation allows for a mathematical formulation of a global mean weathering trend within the system Al2O3–CaO– Na2O– K2O. We further demonstrate the usefulness of the approach for validating processes behind individual trends and for combining the effects of different processes which modify the composition of soils, sediments, and rocks. Alternatives to the Chemical Index of Alteration (CIA) are discussed to obtain a translation-invariant scale for the process of chemical weathering.  相似文献   

15.
Water samples were analyzed for DOC and trace metals from Bagmati River within Kathmandu valley, Nepal, to understand the variation trends of DOC and trace metals and their relationship along the drainage network. The variability in organic matter and wastewater input within the Bagmati drainage basin appeared to control DOC and most of the trace metal concentration. The large input of organic matter and wastewater creates anoxic condition by consuming dissolved oxygen and releasing higher concentrations of DOC, trace elements such as nickel, arsenic, barium, cadmium, and copper with downstream distance. Concentrations of DOC and trace metals like barium and zinc showed strong relationships with human population density and suggest that human activities have strong control on these parameters along the drainage network. The DOC and most of the trace metal concentration increased with downstream distance and appeared to be directly associated with human activities. The variation trends of most of the trace metals appeared to be the same; however, concentration varied widely. Inputs of organic matter and wastewater due to human activities appeared directly to be associated for the variation of DOC and trace metals along the Bagmati drainage network within Kathmandu valley.  相似文献   

16.
Decades of runoff from precious-metal mining operations in the Lake Coeur d’Alene Basin, Idaho, have left the sediments in this lake heavily enriched with toxic metals, most notably Zn, Pb and Cu, together with As. The bioavailability, fate and transport of these metals in the sediments are governed by complex biogeochemical processes. In particular, indigenous microbes are capable of catalyzing reactions that detoxify their environments, and thus constitute an important driving component in the biogeochemical cycling of these metals. Here, the development of a quantitative model to evaluate the transport and fate of Zn, Pb and Cu in Lake Coeur d’Alene sediments is reported. The current focus is on the investigation and understanding of local-scale processes, rather than the larger-scale dynamics of sedimentation and diagenesis, with particular emphasis on metal transport through reductive dissolution of Fe hydroxides. The model includes 1-D inorganic diffusive transport coupled to a biotic reaction network including consortium biodegradation kinetics with multiple terminal electron acceptors and syntrophic consortium biotransformation dynamics of redox front. The model captures the mobilization of metals initially sorbed onto hydrous ferric oxides, through bacterial reduction of Fe(III) near the top of the sediment column, coupled with the precipitation of metal sulfides at depth due to biogenic sulfide production. Key chemical reactions involve the dissolution of ferrihydrite and precipitation of siderite and Fe sulfide. The relative rates of these reactions play an important role in the evolution of the sediment pore-water chemistry, notably pH, and directly depend on the relative activity of Fe and SO4 reducers. The model captures fairly well the observed trends of increased alkalinity, sulfide, Fe and heavy metal concentrations below the sediment–water interface, together with decreasing terminal electron acceptor concentrations with depth, including the development of anoxic conditions within about a centimeter below the lake bottom. This effort provides insights on important biogeochemical processes affecting the cycling of metals in Lake Coeur d’Alene and similar metal-impacted lacustrine environments.  相似文献   

17.
Groundwaters, river and lake waters have been sampled from the semi-arid Siberian Republic of Khakassia. Despite the relatively sparse data set, from a diversity of hydrological environments, clear salinity-related trends emerge that indicate the main hydrochemical evolutionary processes active in the region. Furthermore, the major ion chemistry of the evolution of groundwater baseflow, via rivers, to terminal saline lake water, can be adequately and simply modelled (using PHREEQCI) by invoking: (i) degassing of CO2 from groundwater as it emerges as baseflow in rivers (rise in pH); (ii) progressive evapoconcentration of waters (parallel accumulation of Cl, Na+, SO42−, and increase in pH due to common ion effect); and (iii) precipitation of calcite (depletion of Ca from waters, reduced rate of accumulation of alkalinity). Dolomite precipitation is ineffective at constraining Mg accumulation, due to kinetic factors. Silica saturation appears to control dissolved Si in low salinity waters and groundwaters, while sepiolite saturation and precipitation depletes Si from the more saline surface waters. Gypsum and sodium sulphate saturation are only approached in the most saline environments. Halite remains unsaturated in all waters. Sulphate reduction processes are important in the lower part of lakes.  相似文献   

18.
Acidic, metal-rich waters produced by the oxidative weathering and resulting leaching of major and trace elements from pyritic rocks can adversely affect water quality in receiving streams and riparian ecosystems. Five study areas in the southern Rocky Mountains with naturally acidic waters associated with porphyry mineralization were studied to document variations in water chemistry and processes that control the chemical variations. Study areas include the Upper Animas River watershed, East Alpine Gulch, Mount Emmons, and Handcart Gulch in Colorado and the Red River in New Mexico. Although host-rock lithologies in all these areas range from Precambrian gneisses to Cretaceous sedimentary units to Tertiary volcanic complexes, the mineralization is Tertiary in age and associated with intermediate to felsic composition, porphyritic plutons. Pyrite is ubiquitous, ranging from ∼1 to >5 vol.%. Springs and headwater streams have pH values as low as 2.6, SO4 up to 3700 mg/L and high dissolved metal concentrations (for example: Fe up to 400 mg/L; Cu up to 3.5 mg/L; and Zn up to 14.4 mg/L). Intensity of hydrothermal alteration and presence of sulfides are the primary controls of water chemistry of these naturally acidic waters. Subbasins underlain by intensely hydrothermally altered lithologies are poorly vegetated and quite susceptible to storm-induced surface runoff. Within the Red River study area, results from a storm runoff study documented downstream changes in river chemistry: pH decreased from 7.80 to 4.83, alkalinity decreased from 49.4 to <1 mg/L, SO4 increased from 162 to 314 mg/L, dissolved Fe increased from to 0.011 to 0.596 mg/L, and dissolved Zn increased from 0.056 to 0.607 mg/L. Compared to mine drainage in the same study areas, the chemistry of naturally acidic waters tends to overlap but not reach the extreme concentrations of metals and acidity as some mine waters. The chemistry of waters draining these mineralized but unmined areas can be used to estimate premining conditions at sites with similar geologic and hydrologic conditions. For example, the US Geological Survey was asked to estimate premining ground-water chemistry at the Questa Mo mine, and the proximal analog approach was used because a mineralized but unmined area was located adjacent to the mine property. By comparing and contrasting water chemistry from different porphyry mineralized areas, this study not only documents the range in concentrations of constituents of interest but also provides insight into the primary controls of water chemistry.  相似文献   

19.
The aim of this study was to investigate temporal trends and controlling factors of As and V in running waters throughout Sweden. For this purpose, data on stream water chemistry from 62 streams of varying catchment size and characteristics, included in the Swedish environmental monitoring programmes were evaluated. The geochemical software Visual MINTEQ was used to model the speciation and trend analyses were performed on total concentrations of As and V as well as modelled fractions (dissolved species as well as arsenate and vanadate adsorbed to ferrihydrite). The trend analyses showed increasing total concentrations of As and V in southern Sweden. Concentrations of As and V correlated significantly to Fe concentrations in 59 and 60 of the 62 streams respectively, indicating that Fe is an important determining factor for As and V concentrations in Swedish streams. This was confirmed by the geochemical modelling that indicated that the adsorbed fraction is the dominant form of As and V and that the concentrations of As and V in Swedish streams are thus highly determined by concentrations of colloidal or particulate Fe. It is therefore suggested that the increasing trends of As and V are to a large extent due to increasing concentrations of colloidal Fe, which is stabilised by increasing concentrations of DOC. Further the geochemical modelling indicates that the dissolved fraction of As and V generally is small, with the exception of a few streams with high pH and/or phosphate concentrations.  相似文献   

20.
Relationships between drainage area characteristics and lake water quality   总被引:1,自引:0,他引:1  
The aim of this work is to quantify some of the complex relationships between drainage area characteristics (such as bedrocks and quaternary deposits) and lake water quality (pH, alkalinity, conductivity, and hardness). Seventysix drainage lakes, mainly oligotrophic, are described with respect to drainage area characteristics, morphometry, and water chemistry. The DAZ (drainage area zonation) method has been used to describe the drainage areas. The method utilizes a weighting system to reduce the impact of land types with increasing distance from the lake. The most significant parameter governing the water chemistry parameters seems to be the percentage of open land (cultivated land and/or meadows) in the drainage areas. High percentage leads to high pH, alkalinity, conductivity, and hardness. The correlations concerning alkalinity and pH are improved using the DAZ method. No significant relationships between bedrock geology of the drainage areas and lake water chemistry have been recorded.  相似文献   

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