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1.
Experiments in which cleavage nepheline samples were reacted with aqueous solutions at fixed pH's and temperature were carried out in the laboratory. The chemistry of the solution as a function of time was monitored, as well as the chemistry of the nepheline surfaces.

At 25°C, Al derived from the nepheline stays in solution due to slow precipitation kinetics of Al(OH)3. At 60° and 80°C, precipitation of Al(OH)3 is so rapid that Al concentration in solution is below 0.05 ppm. This indicates that precipitation kinetics favour the formation of bauxite deposits in tropical regions (i.e. T25°C), but not in temperate regions.

Precipitation products on the surface of the nepheline fragments at 60° and 80°C depend on the pH. At pH 3.0, an amorphous aluminium silicate (proto-kaolinite?) is formed. At pH>7.0, the precipitated phase contains, in addition to Al and Si, high amounts of Na and K (proto-muscovite?). The optimum pH for the formation of bauxite is in the range 5–7. These results are in agreement with thermodynamic calculations.  相似文献   


2.
莫高窟崖体可溶盐分布特征研究   总被引：1，自引：0，他引：1       下载免费PDF全文
通过对莫高窟崖面不同高度取样,运用经典溶液化学的研究方法,调查研究莫高窟崖体中所含硫酸钠(Na2SO4)和氯化钠(NaCl)以及中溶盐硫酸钙(CaSO4.2H2O)的分布。经过水化学分析,浸出液的水化学类型主要为SO4.Cl—Ca.Na型,离子为引起壁画疱疹、粉层起甲、颜料层粉化、颜料层片状脱落、壁画地仗酥碱的主要成分。同时,查明了莫高窟崖体物质组成,数据显示,崖面砾岩以大孔隙为主,渗透性变化范围广,有利于盐分溶液渗透。分析结果表明,莫高窟崖体上盐分随高度的分布规律受地表淋滤下渗和历史上风积沙掩埋期的毛细上升等综合因素影响,且后一种作用引起的盐分聚集有可能是底层洞窟壁画病害的主要原因。  相似文献   

3.
This study reports the kinetic experimental results of albite in water and in KCI solution at 22 MPa in the temperature range of 25 to 400℃. Kinetic experiments have been carried out in an open flow-through reaction system (packed bed reactor). Albite dissolution is always incongruent in water at most temperatures, but becomes congruent at 300℃ (close to the critical point 374℃). At temperatures from 25 to 300℃, the incongruent dissolution of albite is reflected by the fact that sodium and aluminum are easily dissolved into water; from 300 to 400℃ it is reflected by silicon being more easily dissolved in water than Al and Na. Maximum albite dissolution rates in the flow hydrothermal systems have been repeatedly observed at 300℃, independent of flow rates.The kinetic experiments of albite dissolution in a KCl aqueous solution (0.1 mol KCl) indicate that the dissolution rate of albite increases with increasing temperature. Maximum silicon release rates of albite have been observed at 400℃, while ma  相似文献   

4.
Previous studies in our laboratory have demonstrated that drinking-water treatment residuals are effective sorbents of arsenic V. However, the effect of soil solution chemistry on arsenic V sorption by drinking-water treatment residuals-amended soils remains to be explored. The current study uses a batch incubation experimental set up to evaluate the effect of soil solution pH, competing ligands, and complexing metal on arsenic V sorption by a sandy soil (Immokalee series) amended with two rates (25 and 50 g kg?1) of aluminum and iron-based drinking-water treatment residuals. Experiments were conducted at three initial arsenic loads (125, 1,875, 3,750 mg kg?1) and a constant solid: solution ratio of 200 g L?1. An optimum equilibration time of 8 days, obtained from kinetic studies, was utilized for sorption experiments with both aluminum and iron drinking-water treatment residual-amended soil. Presence of phosphate decreased arsenic V sorption by both aluminum and iron drinking-water treatment residual amended soils, with a strong dependence on pH, drinking-water treatment residual types, drinking-water treatment residual application rates, and phosphate concentrations. Addition of sulfate had no effect on arsenic V sorption by aluminum or iron drinking-water treatment residual-amended soil. A complementing effect of calcium on arsenic V sorption was observed at higher pH. Results elucidating the effect of soil solution chemistry on the arsenic V sorption will be helpful in calibrating drinking-water treatment residual as a sorbent for remediation of arsenic-contaminated soils.  相似文献   

5.
The adsorption of surfactants from aqueous solution is a phenomenon of major importance in applications ranging from ore flotation and paint technology to enhanced oil recovery. As this paper will illustrate, the process is very complex and of high scientific interest; its results can be extended to the retention of organic compounds (humic and fulvic acids, pollutants...) on solids in the biosphere. For a good understanding of the mechanisms involved in surfactants adsorption at the hydrophilic solid–aqueous solution interface, thermodynamic models have to take into account: (i) the physical chemistry of the surfactant in aqueous solution for choosing the appropriate reference phase, (ii) the surface heterogeneity of the adsorbing solid, (iii) the intensity of normal adsorbate–adsorbent bonds responsible for adsorption, (iv) the intensity of lateral bonds that favour the formation of surface aggregates through cooperative process and finally, (v) suitable theoretical models to describe adsorption phenomena. Once this has been achieved, two systems can be discussed: systems characterised by strong normal adsorbate–adsorbent bonds, currently used in ore flotation, which lead, in the case of heterogeneous surfaces, to the formation of lamellar aggregates at monolayer concentration and bilayer formation for higher concentrations. Systems characterised by weak normal adsorbate–adsorbent bonds, currently used in enhanced oil recovery and hydrocarbon (bio)remediation, which correspond to: (i) formation of globular micelles at the solid surface near the CMC when the temperature is higher than the Krafft point, (ii) formation of bilayered lamellar aggregates in the opposite case, (iii) three-dimensional condensation on substrate (T<TKrafft) if the ionic surfactant interacts with cations in the bulk. To cite this article: J.-M. Cases et al., C. R. Geoscience 334 (2002) 675–688.  相似文献   

6.
Chemical reactions pertinent to karst systems divide broadly into (a) speciation reactions within aqueous solutions, (b) dissolution/precipitation and other acid/base reactions between aqueous solutions and solid minerals, and (c) redox reactions involving various carbon and sulfur-bearing species. As a backdrop against which other chemistry can be evaluated, selected phase diagrams and equilibrium speciation diagrams were calculated for the system Ca—Mg—O—H—C—S. The kinetics of reactions within this system span time scales from milliseconds for homogeneous reactions in solution through hundreds of hours for carbonate mineral dissolution reactions, to geologic time scales for reactions such as the aragonite/calcite inversion or the oxidation/reduction of native sulfur. In purely inorganic systems, kinetic barriers, typically on the order of tens of kJ/mole, are set by nucleation processes and by activated complex formation. Biological processes impact the purely inorganic chemistry by the following mechanisms: (a) Secretions and waste products from biological activity or consumption of CO2 by organisms changes the chemistry in the microenvironments of reaction surfaces. Oxidation potentials, pH, and ion activities may be modified, thus shifting equilibria. (b) Reaction rates may be increased due to modification of activated complexes and thus the activation barriers to reaction. (c) Organic compounds or microorganisms may act as substrates, thus lowering nucleation barriers. The preservation of microorganisms in cave deposits does not necessarily prove a cause and effect relationship.  相似文献   

7.
In order to evaluate the complex interplay between dissolution and precipitation reaction kinetics, we examined the hypothesis of partial equilibria between secondary mineral products and aqueous solutions in feldspar-water systems. Speciation and solubility geochemical modeling was used to compute the saturation indices (SI) for product minerals in batch feldspar dissolution experiments at elevated temperatures and pressures and to trace the reaction paths on activity-activity diagrams. The modeling results demonstrated: (1) the experimental aqueous solutions were supersaturated with respect to product minerals for almost the entire duration of the experiments; (2) the aqueous solution chemistry did not evolve along the phase boundaries but crossed the phase boundaries at oblique angles; and (3) the earlier precipitated product minerals did not dissolve but continued to precipitate even after the solution chemistry had evolved into the stability fields of minerals lower in the paragenesis sequence. These three lines of evidence signify that product mineral precipitation is a slow kinetic process and partial equilibria between aqueous solution and product minerals were not held. In contrast, the experimental evidences are consistent with the hypothesis of strong coupling of mineral dissolution/precipitation kinetics [e.g., Zhu C., Blum A. E. and Veblen D. R. (2004a) Feldspar dissolution rates and clay precipitation in the Navajo aquifer at Black Mesa, Arizona, USA. In Water-Rock Interaction (eds. R. B. Wanty and R. R. I. Seal). A.A. Balkema, Saratoga Springs, New York. pp. 895-899]. In all batch experiments examined, the time of congruent feldspar dissolution was short and supersaturation with respect to the product minerals was reached within a short period of time. The experimental system progressed from a dissolution driven regime to a precipitation limited regime in a short order. The results of this study suggest a complex feedback between dissolution and precipitation reaction kinetics, which needs to be considered in the interpretation of field based dissolution rates.  相似文献   

8.
In three separate experiments, one using a bicarbonate buffered aqueous NaCl solution and two using natural seawater. the solubility of chemically pure X-ray amorphous precipitated silica decreased by approximately 20‰ after aging in contact with solution for several months. The specific surface area of the silica decreased by approximately half during the same experimental time periods. The solubility decrease in buffered NaCl solution occurred at both 2 and 22°C and over the pressure range from 1.01 × 105 to 7.45 × 107 Pa (1–740 atm). The aging process which causes the solubility and surface area decreases may be caused by the formation of a smooth surface silica layer that is more dense than the original surface. No change in the bulk chemistry of the silica could be defined after aging. This short term aging process contributes to the scatter in published solubilities for amorphous silica in seawater.  相似文献   

9.
The relation between aluminum and titanium in the course of bauxite formation is one of the key problems in deciphering the genesis of bauxitic rocks, particularly those occurring in geosynclinal areas. The source of aluminum and titanium in marine geosynclinal bauxites is related directly to the effects of volcanism. Ultra-acidic thermal waters may extensively leach volcanic rocks, resulting in the removal and migration of large amounts of aluminum in solution. These solutions are extremely stable, even when diluted by surface waters, and move to the sea without losing aluminum by precipitation. Primary titanium minerals are also decomposed and displaced in hydrothermally-altered rocks. Titanium is removed primarily as colloidal titanium hydroxide. Aluminum in solution and titanium in the form of colloidal titanium hydroxide films are carried to the sea in acid streams. As the acid streams are neutralized upon mixing with sea water, aluminum forms an amorphous colloidal hydroxide that coagulates and crystallizes. Titanium is extracted by its co-precipitation with aluminum hydroxide by a sorption mechanism. The migration and co-precipitation of these elements in the manner outlined is believed to be responsible for the formation of geosynclinal bauxite deposits in volcanic areas of island arcs. — R.D. DeRudder.  相似文献   

10.
Abstract: The adsorption of gold on iron(III) and aluminum hydroxides from solutions containing Au(III) complexes has been studied as a function of pH and chloride concentration at 30C. Iron(III) hydroxide was more effective in adsorbing gold from solution than aluminum hydroxide. However, both hydroxides controlled the behavior of Au(III) complex with very similar manner. The most effective gold adsorption occurred in aqueous solution with near neutral pH and low Cl concentration. In this solution condition, Au(III) complexes were mainly dissolved as AuCl2(OH)2- and AuCl(OH)3-, and the surface charge for both hydroxides was positive. In addition, the adsorbed Au(III) complexes were spontaneously reduced to elemental gold in spite of the absence of a specific reducing agent.
The results of this study suggest that adsorption and spontaneous reduction of gold complexes on the surface of hydrous metal oxides with positive charge play an important role in gold precipitation in subsurface environment.  相似文献   

11.
Interstitial solution was recovered from core samples of a borehole through 472 m of the Upper Cretaceous Chalk formation in eastern England. The solution has been analysed for major and some minor components and also for oxygen and hydrogen isotopic composition. Samples of the carbonate rock have also been analysed following acid dissolution. The general feature of interstitial solution chemistry is a progressive dilution of dissolved species with decreasing depth, from a near-marine composition found in the deepest samples which are identified as connate water. Departures from the expected dilution trend are interpreted as evidence for diagenetic reactions during burial or as a result of freshwater circulation following subaerial uplift. Sr2+, Li+ and F? have been enriched in interstitial solution and K+ has been slightly depleted. The profile of chalk chemistry with depth shows no conclusive evidence for changes in the Mg and Sr content of the bulk carbonate due to freshwater diagenesis. The δ18O and δD of the interstitial water reflect the same mixing as that shown by dissolved species. However an apparent depletion of 18O and D in the deepest fluids with respect to the expected marine isotopic composition is tentatively explained as a result of the differences in diffusion rates of aqueous oxygen and hydrogen and of ionic solutes.  相似文献   

12.
The extraction of mineral resources requires access through underground workings, or open pit operations, or through drillholes for solution mining. Additionally, mineral processing can generate large quantities of waste, including mill tailings, waste rock and refinery wastes, heap leach pads, and slag. Thus, through mining and mineral processing activities, large surface areas of sulfide minerals can be exposed to oxygen, water, and microbes, resulting in accelerated oxidation of sulfide and other minerals and the potential for the generation of low-quality drainage. The oxidation of sulfide minerals in mine wastes is accelerated by microbial catalysis of the oxidation of aqueous ferrous iron and sulfide. These reactions, particularly when combined with evaporation, can lead to extremely acidic drainage and very high concentrations of dissolved constituents. Although acid mine drainage is the most prevalent and damaging environmental concern associated with mining activities, generation of saline, basic and neutral drainage containing elevated concentrations of dissolved metals, non-metals, and metalloids has recently been recognized as a potential environmental concern. Acid neutralization reactions through the dissolution of carbonate, hydroxide, and silicate minerals and formation of secondary aluminum and ferric hydroxide phases can moderate the effects of acid generation and enhance the formation of secondary hydrated iron and aluminum minerals which may lessen the concentration of dissolved metals. Numerical models provide powerful tools for assessing impacts of these reactions on water quality.  相似文献   

13.
The influence of type and amount of clays present in soils on their properties is well understood. The clays exert their influence through large specific surface area and charges on them. Their effect is mostly exhibited through inter particle bonding and subsequent particle associations. The mineralogical influence of soils in water is well documented. However, the change in soil water system because of presence some of the contaminants can greatly influence the soil behaviour. Some of the changes are due to formation of new compounds due to interactions between the soil and pollutant. The paper reports the effect of interaction of kaolinite mineral with alkali on the index properties of soils from which the geotechnical behaviour can be understood. Detailed X-ray diffraction studies have shown that sodium aluminum silicate hydroxide hydrate (NASH) is formed by clay alkali reactions. The type and amount of formation of the compound is influenced by the concentration of alkali solution. While the compound formed is in smaller quantities with 1 N NaOH solution, significantly high quantity is formed with 4 N NaOH solution. Presence of alumina is shown to play a significant role. It was observed that the formation of sodium aluminum silicate hydroxide hydrate is reduced in the presence of alumina. Specific gravity of contaminated clay soil was reduced which confirms the formation of new compounds. Water adsorption and specific surface area of soil are also influenced due to soil alkali interaction. The changes in the free swell and index properties of soil in the presence of alkali have been explained by the changes in soil fabric and the formation of new compound.  相似文献   

14.
水悬浮体系中凹凸棒石与Cu2+作用机理   总被引：12，自引：0，他引：12  
研究矿物吸附重金属性能和机理,对正确认识矿物吸附性质、环境矿物材料应用研究以及重金属环境化学行为具有重要理论和实际意义。凹凸棒石是重要粘土矿物之一,也是重要的环境矿物材料,其吸附净化功能潜在应用受到广泛关注。在制备凹凸棒石纯样基础上,进行了凹凸棒石吸附Cu^2 单因素实验,吸附前后溶液pH值变化观测和吸附Cu^2 后凹凸棒石表面结构高分辨透射电镜调查。结果表明,从表面来看,凹凸棒石对Cu^2 的吸附性能主要受振荡速度、吸附时间、初始溶液pH值、吸附剂用量等因素影响,但实际上,凹凸棒石对Cu^2 的吸附作用主要是凹凸棒石诱导的Cu^2 水解沉淀作用以及凹凸棒石(带负电荷)与氢氧化铜(带正电荷)正负电荷胶体颗粒的互相作用,这有别于严格意义的矿物界面吸附作用。产生这种作用的机制在于凹凸棒石属于天然纳米矿物材料,具有较高的表面化学活性,凹凸棒石一水悬浮体系中凹凸棒石表面水解呈现出碱性,结果导致吸附平衡水溶液pH值较初始水溶液有较大程度的升高,达到Cu^2 水解基本完全的pH条件.  相似文献   

15.
以特殊的紫红色土为研究对象,采取三峡地区黄腊石滑坡临江松散土进行室内饱水试验,根据能量最低原则建立热力学反应模型,通过线性规划求解,分析不同饱水环境下随时间积累过程中紫红色松散土矿物反应特征及规律。研究表明:松散土在不同溶液浸泡条件下化学反应类型不同,江水和弱碱性溶液中主要发生白云石矿物的溶解,自来水、纯水和弱酸性溶液中主要发生方解石矿物的溶解和Ca2+与K+的交换吸附。另外,不同浸泡环境中不同时间的水-土化学作用活跃程度明显差异,弱酸性溶液与松散土的化学反应在饱水1~7 d最为强烈,其他四种溶液与松散土的化学反应在饱水7~16 d最为强烈。饱水后期,不同溶液浸泡条件下的水-土化学作用都减弱并最终趋向于平衡。  相似文献   

16.
Energy related industrial development, municipal waste treatment processes and some natural sources, contribute to B (being present) in the environment in elevated concentrations. Boron forms numerous aqueous ion pairs and complexes, some of which would not normally exist in significant concentrations under typical baseline environmental conditions. A complete understanding of the aqueous chemistry of B depends on an accurate evaluation of the thermodynamic data for these species.Equilibrium constants for 29 inorganic complexes, ion pairs, and polyanions of B have been critically evaluated. Apparent equilibrium constants have been extrapolated to zero ionic strength, and the selected thermodynamic values are tabulated. Gibbs free energies of formation for the aqueous species have been computed; these are presented with entropy and enthalpy values where available  相似文献   

17.
A parameter called ΔO2? is defined as the difference between the Gibbs energy of formation from the elements of a crystalline oxide and the Gibbs energy of formation from the elements of its cation in aqueous solution (per O2? in the oxide). Another parameter called Δ hydroxide is defined as the difference between the Gibbs energies of formation of an hydroxide and its constituent oxides, H2O oxide being considered as ice. A linear equation for 32 hydroxides, using these two parameters is: Δhydroxide = ?0.210 (ΔO2? cation ? ΔO2? H+). This relation can also be expressed in terms of solution energies. The solution energy of an hydroxide is a linear function of the solution energy of the corresponding oxide. The equation above can be used to predict values for Gibbs energies of formation of hydroxides, oxides or aqueous cations and to test the consistency of existing Gibbs energy values.  相似文献   

18.
The zinc-lead separation from a chloride solution in the form of a synthetic leach liquor has been studied using tertiary aliphatic amines and tetra-alkylammonium salts. Larger extractions, and hence distribution coefficients, are observed with ammonium salts. However, the best separation factors occur when employing tertiary amines. The results show that it is possible to leave the lead in the aqueous solution whilst the zinc is transferred to the organic phase by a proper choice of the hydrochloric acid and extractant concentrations. An approach to coordination chemistry is suitable to explain the extraction mechanism.  相似文献   

19.
Non-conservative behavior of dissolved inorganic phosphate (DIP) in estuaries is generally ascribed to desorption from iron and aluminum (hydr)oxides with increasing salinity. Here, we assess this hypothesis by simulating the reversible adsorption of phosphate onto a model oxide (goethite) along physico-chemical gradients representative of surface and subsurface estuaries. The simulations are carried out using a surface complexation model (SCM), which represents the main aqueous speciation and adsorption reactions of DIP, plus the ionic strength-dependent coulombic interactions in solution and at the mineral-solution interface. According to the model calculations, variations in pH and salinity alone are unlikely to explain the often reported production of DIP in surface estuaries. In particular, increased aqueous complexation of phosphate by Mg2+ and Ca2+ ions with increasing salinity is offset by the formation of ternary Mg-phosphate surface complexes and the drop in electrical potential at the mineral-water interface. However, when taking into account the downstream decrease in the abundance of sorption sites, the model correctly simulates the observed release of DIP in the Scheldt estuary. The sharp increase in pH accompanying the admixing of seawater to fresh groundwater should also cause desorption of phosphate from iron oxyhydroxides during seawater intrusion in coastal aquifers. As for surface estuaries, the model calculations indicate that significant DIP release additionally requires a reduction in the phosphate sorption site density. In anoxic aquifers, this can result from the supply of seawater sulfate and the subsequent reductive dissolution of iron oxyhydroxides coupled to microbial sulfate reduction.  相似文献   

20.
Contemporary ‘acid rain’ in the Hubbard Brook ecosystem has induced a series of geochemical responses. Neutralization is accomplished in essentially a 2-step process. Initially, hydrogen ion acidity is neutralized by the dissolution of reactive alumina primarilly found in the soil zone. In the Hubbard Brook area this reactive alumina has solution properties much like natural gibbsite. Aluminum-rich surface waters with a pH of 4.7 5.2 are typical of this neutralization stage. In a second step, both hydrogen ion acidity and aluminum acidity are neutralized by the chemical weathering of primary silicate minerals, i.e. by the alkali and alkaline earths contained in the bedrock and glacial till of the watershed. The chemical weathering reaction is much slower than the alumina dissolution reaction, so that the aluminum acidity stage (pH 4.7 5.2) may persist for substantial periods. Typically, however, in the Hubbard Brook area the aluminum acidity has been neutralized and a pH > 5.2 is obtained before surface waters reach a third-over stream channel. Because of the relatively low pH's throughout the soil zone and in the streamwater, carbonic acid reactions are essentially absent at the present time in the Hubbard Brook system. Water pathlength (or residence time) in the soil zone is the crucial factor in the state of acid rain neutralization, aluminum chemistry and chemical weathering. As measured by the losses of alkali and alkaline earths from the ecosystem, chemical weathering rate in the Hubhard Brook area at the present time is not especially high relative to other areas.  相似文献   

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