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1.
The results of experimental studies of ion exchange properties of Co-bearing ferromanganese crusts in the Magellan Seamounts (Pacific Ocean) are discussed. Maximum reactivity in reactions with the participation of manganese minerals (Fe-vernadite, vernadite) is typical of Na+, K+, and Ca2+ cations, whereas minimum activity is recorded for cations Pb2+ and Co2+. The exchange complex of ore minerals in crusts is composed of Na+, K+, Ca2+, Mg2+, and Mn2+ cations. The exchange capacity of manganese minerals increases from the alkali metal cations to rare and heavy metal cations. Peculiarities of the affiliation of Co2+, Mn2+, and Mg2+ cations in manganese minerals of crusts are discussed. In manganese minerals, Co occurs as Co2+ and Co3+ cations. Metal cations in manganese minerals occur in different chemical forms: sorbed (Na+, K+, Ca2+, Mn2+, Co2+, Cu2+, Zn2+, Cd2+, and Pb2+); sorbed and chemically bound (Mg2+, Ni2+, Y3+, La3+, and Mo6+); and only chemically bound (Co3+). It is shown that the age of crust, its preservation time in the air-dry state, and type of host substrate do not affect the ion exchange indicators of manganese minerals. It has been established that alkali metal cations are characterized by completely reversible equivalent sorption, whereas heavy metal cations are sorbed by a complex mechanism: equivalent ion exchange for all metal cations; superequivalent, partly reversible sorption for Ba2+, Pb2+, Co2+, and Cu2+ cations, relative to exchange cations of manganese minerals. The obtained results refine the role of ion exchange processes during the hydrogenic formation of Co-bearing ferromanganese crusts.  相似文献   

2.
The results of experimental studies of ion exchange properties of manganese and iron minerals in micronodules (MN) from diverse bioproductive zones of the World Ocean are considered. It was found that the sorption behavior of these minerals is similar to that of ore minerals from ferromanganese nodules (FMN) and low-temperature hydrothermal crusts. The exchange complex of minerals in the MN includes the major (Na+, K+, Ca2+, Mg2+, and Mn2+) and the subordinate (Ni2+, Cu2+, Co2+, Pb2+, and others) cations. Reactivity of theses cations increases from Pb2+ and Co2+ to Na+ and Ca2+. Exchange capacity of MN minerals increases from the alkali to heavy metal cations. Capacity of iron and manganese minerals in the oceanic MN increases in the following series: goethite < goethite + birnessite < todorokite + asbolane-buserite + birnessite < asbolane-buserite + birnessite < birnessite + asbolane-buserite < birnessite + vernadite Fe-vernadite + Mn-feroxyhyte. The data obtained supplement the available information on the ion exchange properties of oceanic ferromanganese sediments and refine the role of sorption processes in the redistribution of metal cations at the bottom (ooze) water-sediment interface during the MN formation and growth.  相似文献   

3.
Cation exchange reactions with participation of heavy metals Mn, Co, Ni, Cu, Zn, Cd, Ba, and Pb were studed in oceanic low-temperature hydrothermal deposits of various mineral compositions and in hydrogenic Fe-Mn crusts. Individual minerals and their assemblages differ significantly in absorptive capacity, which increases in the following order: hematite ? Si-protoferrihydrite < protoferrihydrite < geothite < nontronite ? Fe-vernadite + Mn-feroxyhyte < Fe-free vernadite < bernessite + Fe-free vernadite < bernessite; i.e., it successively increases from the mineral with a coordination type of lattice to minerals with a layer-type structure. The exchange complex of all minerals includes Na+, K+, Ca2+, and Mg2+, i.e., the main cations of seawater. In Mn minerals, Mn2+ is the main exchange component. The contribution of all the mentioned cations to the exchange capacity of minerals is as high as 90–98%. The highest absorptive capacity among the examined low-temperature oceanic deposits is characteristic of hydrothermal Mn minerals. Their capacity exceeds substantially that of hydrothermal oxides, hydroxides, Fe-aluminosilicates, and hydrogenic Fe-Mn minerals. The absorptive capacity of all examined Mn minerals relative to heavy metals increases in the same order: Ni < Zn < Cd < Mn < Co < Pb < Cu.  相似文献   

4.
Fe(II)–Ca(II), Fe(II)–Na(I), and Fe(II)–Ca(II)–Na(I) exchange experiments on montmorillonite were performed in chloride background. These experiments show the possible sorption of Fe2+ and FeCl+ ion pairs in exchange site positions, a result confirmed with 77 K 57Fe Mössbauer experiments. The sorption data were modeled and the cation exchange selectivity for Fe(II) were found to be nearly equal to that of Ca(II). Vanselow selectivity coefficients, for Na–Fe2+ and Na–FeCl+ reactions, were found to be equal to 0.4 (0.5 for Ca2+) and 2.3 (2.5 for CaCl+) respectively. High affinity of montmorillonite for chloride ion pairs seems to be a common mechanism as first stated by Sposito et al., (Soil Sci. Soc. Am. J. 47, 51–56, 1983a), and should have implications e.g., on the chemistry of suspended particles in seawater. Exchange selectivity coefficients derived from this study and others were used to model experimental data on river water and seawater equilibrated particles. The agreement between simulations and experimental data is very good. The simulation shows the predominance of monovalent ion (Na+ and chloride ion pairs) sorption on clay particles in seawater. This sorption of monovalent ions leads to the dispersion of particles in seawater and to the extension of a plume of particles spreading away from river deltas, such as that of the River Amazon.  相似文献   

5.
The rate of silica removal from two montmorillonites (Chambers and Polkville) has been measured as a function of time, temperature, solution composition, and exchange ion on the clay. Silica removal rate increased with temperature from 200 to 350°C, decreased with time, and could be approximated initially by a parabolic rate law. Solution composition influenced silica removal rate by determining the exchange population of the clay; silica removal is most rapid when K-exchange ions are present. Thus increasing the concentration of K+ accelerated silica removal, whereas increasing the concentration of Na+, Ca2+, and Mg2+ inhibited silica removal. Activation energies for silica removal range from 5 to 10 kcal/mol. The largest values are associated with the largest concentrations of inhibitor ions in solution. Activation energies of this magnitude suggest that the rate-limiting step for silica removal is transport through a hydrated, expanded interlayer space. Application of experimental results to diagenesis in moderately to deeply buried sediments suggests that K+ uptake by montmorillonite may precede and accelerate illite formation.  相似文献   

6.
We study the origin of the ionic exchange enthalpy in montmorillonite clays using microcalorimetry measurements and molecular simulation. We first determine the standard reaction enthalpy for well-defined interlayer water contents. We then show by a detailed analysis based on thermodynamic cycles that replacing Na+ ions by Cs+ in the interlayer of montmorillonite clays is an endothermic process, and that the overall exchange is exothermic only because it is dominated by the exothermic replacement of Cs+ by Na+ in the aqueous phase. This conclusion from ionic exchange enthalpies supports the one of a recent study of the ionic exchange free energy by Teppen and Miller [Teppen B. J. and Miller D. M. (2006) Hydration energy determines isovalent cation exchange selectivity by clay minerals. Soil Sci. Soc. Am. J.70(1), 31-40] and contradicts long-held views on the role of ion-clay interactions in determining the ionic exchange thermodynamics. This calls for a paradigm shift for the origin of this exchange: The driving force is the “hydrophobicity” of Cs+ compared to Na+ and not its affinity for clay surfaces.  相似文献   

7.
Experimental studies of the reactions of Cu(II), Pb(II), and Zn(II) in aqueous solutions with organic matter derived from fresh samples of the green filamentous algae Ulothrix spp. and the green unicellular algae Chlamydomonas spp. and Chlorella vulgaris show that, under suitable conditions, a significant proportion of the metals is removed from solution by sorption onto the particulate organic matter of the algal suspension.The metal sorption is strongly suppressed by H+ but is only marginally influenced by the proportion of whole cells in the suspension and by complexing of metals in solution by the soluble organic matter. The presence of relatively small amounts of the cations Na+ and Mg2+ in solution reduces the sorption of Zn(II) to near zero, but Pb(II) and Cu(II) sorption occurs to an appreciable extent even in strong brines. This may be a means for the selective precipitation of Pb(II) from brines rich in Pb(II) and Zn(II).Metal “saturation” values indicate that particulate algal matter of the type used in these experiments could sorb sufficient quantities of metal to form an ore deposit if a weight of organic matter of similar order of magnitude to that of the inorganic sediments in the deposits was available. However, the metal sorption is an equilibrium reaction, and the experimentally determined “enrichment factors” suggest that the “saturation” values could be approached only in solutions whose metal contents were initially at least two orders of magnitude above those of normal seawater.  相似文献   

8.
The 2-site protolysis no electrostatics surface complexation and cation exchange (2SPNE/CE) model used in previous work to model the sorption of Ni and Zn on Na- and Ca-montmorillonites was applied to sorption edges and isotherms measured for Eu on these two montmorillonite forms. The aim was to further test the applicability of the sorption model on a trivalent element with a more complex aqueous chemistry. An additional reason for choosing Eu was that it is considered to be a good chemical analogue for other lanthanides and trivalent actinides. With site types, site capacities, and protolysis constants fixed at the values in the Ni/Zn studies, all of the measured sorption edge data could be modelled using cation exchange and the monodentate surface species, ≡SSOEu2+, ≡SSOEuOH+ and ≡SSOEu(OH)3−, on the strong site type. However, an additional modelling study showed that the same data were almost equally well described by considering bidentate surface complexes, (≡SSO)2Eu+ and (≡SSO)2Eu(OH)2−, and cation exchange. To model the sorption isotherm measurements up to pH = 7.2, only one additional weak site surface complex was required, ≡SW1OEu2+ for the monodentate case and (≡SW1O)2Eu+ for the bidentate case. Selectivity coefficients are given for Eu3+- Ca2+ and Eu3+- Na+ exchange on the planar sites and surface complexation constants for monodentate and bidentate Eu surface species on the edge sites of montmorillonite.  相似文献   

9.
Sorption edges and isotherms for Eu(III) uptake on Ca-montmorillonite and Na-illite in 0.066 mol/L Ca(ClO4)2 and 0.1 mol/L NaClO4 background electrolytes, respectively, were modelled using a quasi-mechanistic sorption model (the two site protolysis non electrostatic surface complexation and cation exchange (2SPNE SC/CE) model). For both clay minerals the Eu sorption edges could be quantitatively modelled in the pH range ∼3 to ∼10 using cation exchange reactions for Eu3+/Na+ and Eu3+/Ca2+ and three surface complexation reactions on the strong sorption sites forming ≡SSOEu2+, ≡SSOEuOH+ and ≡SSOEu(OH)2° inner sphere complexes which appear successively with increasing pH. Time resolved laser fluorescence spectroscopy (TRLFS) measurements of Cm(III) loaded Ca-montmorillonite and Na-illite were available from Part 1 of this work. De-convolution of the normalised fluorescence spectra measured at different pH values indicated three distinct Cm surface complexes, Cm complexes 1, 2 and 3 for both clay minerals, in agreement with model predictions, but with different distribution functions for the individual species. Under the assumption that Eu and Cm exhibit essentially the same hydrolysis and sorption behaviour, the Eu surface complexation constants were used to predict surface species distribution functions for Cm under the same experimental conditions used in the TRLFS measurements. Comparison of modelled and experimentally deduced species distributions indicated that for both clay minerals peak heights and widths of the three peaks did not correspond particularly well. It is shown that the calculated species distribution functions are sensitive to the values of the hydrolysis constants used in the calculations, whereas modelling the sorption edge measurements by applying the 2SPNE SC/CE approach is much less sensitive. By modifying the values of the hydrolysis constants within their uncertainty range and re-modelling the sorption edges, considerably better correspondence between the modelled and TRLFS species distribution functions was found. In particular, peak positions, heights and widths for the model predicted peaks for the ≡SSOCm2+ and ≡SSOCmOH+ species distribution, and those for Cm complexes 1 and 2 derived from TRLFS, were found to be very close for both clay minerals. However, discrepancies were still apparent between the profile for the calculated ≡SSOEu(OH)2° surface species and the Cm complex 3 species, especially in the case of Na-illite.  相似文献   

10.
Results of the experimental study of ion exchange properties of deep-sea pelagic sediments and related ferromanganese nodules (FMN) are considered. The exchange complex of sediments and nodules includes Na+, K+, Ca2+, and Mg2+ cations. The FMNs also include Mn2+ cations. Series of reactivity of metal cations during exchange reactions in different types of pelagic clayey sediments and diagenetic-sedimentary FMN are compiled. Series of exchange capacity of the sediments and FMN for alkali and heavy metal cations are also presented. The exchange capacity of FMN is always higher than that of enclosing sediments. Sediments are characterized by reversible equivalent sorption of cations of both alkali and heavy metals. Irrespective of the mineral composition, the FMNs are characterized by the reversible equivalent sorption of alkali metal cations, whereas sorption of heavy metal cations is only partly reversible. More over, alkali metal cations do not replace heavy metal cations. The results obtained refine the role of ion exchange processes in the redistribution of heavy metal cations at the water-bottom sediment interface during the diagenetic-sedimentary formation of ferromanganese nodules.  相似文献   

11.
The total mineralization of solutions squeezed out of montmorillonite clay saturated in sea water was determined at different overburden pressures. The subsequent fractions of expelled solutions were also analysed for various anions (Cl?, SO2-4, HCO?3, F?) and cations (Na+, K+, Mg2+, Ca2+, B3+). The results indicate that the concentrations of squeezed-out solutions during the initial stages of compaction (at pressures up to 35 kg/cm2) are slightly higher than that of interstitial solution present initially. The concentration of squeezed-out solution goes through a maximum, or at least remains constant, before starting to decrease with increasing overburden pressure.  相似文献   

12.
Sorption of Ni(II) onto chlorite surfaces was studied as a function of pH (5–10), ionic strength (0.01–0.5 M) and Ni concentration (10−8–10−6 M) in an Ar atmosphere using batch sorption with radioactive 63Ni as tracer. Such studies are important since Ni(II) is one of the major activation products in spent nuclear fuel and sorption data on minerals such as chlorite are lacking. The sorption of Ni(II) onto chlorite was dependent on pH but not ionic strength, which indicates that the process primarily comprises sorption by surface complexation. The maximum sorption was at pH ∼ 8 (Kd = ∼10−3 cm3/g). Desorption studies over a period of 1–2 weeks involving replacement of the aqueous solution indicated a low degree of desorption. The acid–base properties of the chlorite mineral were determined by titration and described using a non-electrostatic surface complexation model in FITEQL. A 2-pK NEM model and three surface complexes, Chl_OHNi2+, Chl_OHNi(OH)+ and Chl_OHNi(OH)2, gave the best fit to the sorption results using FITEQL. The high Kd values and low degree of desorption observed indicate that under expected groundwater conditions, a large fraction of Ni(II) that is potentially leachable from spent nuclear fuel may be prevented from migrating by sorption onto chlorite surfaces.  相似文献   

13.
It is shown that the reaction ability of metal cations of ore minerals in Fe–Mn crusts of the Marcus Wake Rise increases in the following manner: (Co2+ < Cu2+ < Ni2+) < (Mg2+ < Mn2+ < K+ ≈ Ca2+ ≈ Na+). The composition of the exchange complex of the ore minerals is constant and includes these metal cations. Ca2+ and Na+ are major contributors to the exchange capacity of the ore minerals. The capacity of the ore minerals by cations of alkali and base metals is 0.43–0.60 and 2.08–2.70 mg-equiv/g, respectively. The exchange capacity of the ore minerals by cations of base metals increases linearly with the increase in the MnO2 content of the crust and does not depend on the geographical locations of the Marcus Wake guyots.  相似文献   

14.
An exploratory study was carried out at 22 sampling stations along the Langat River, Selangor in order to investigate on the vitality of cation exchange capacity (CEC) in sediment (0–5 cm). Parameters such as pH, Eh, salinity, and electrical conductivity (EC) were determined. The CEC in sediment has been calculated by the determination of Ca2+, Na+, Mg2+, and K+ using the flame atomic absorption spectrophotometer, while the organic matter content in sediment was ascertained using the loss on ignition method. The characteristic of the sediment shows that pH (3.09–7.46), salinity (0.02–10.71 ppt), EC (3.39–517 μS/cm) and Eh (?16.20–253.10 mV) were substantially high in variation. This study also revealed that exchangeable Ca2+ and Mg2+ were controlled by organic matter contents, while exchangeable Na+ and K+ were influenced by salinity. Salinity was observed to play a major part in controlling all the exchangeable cations, as it gives strong significant correlations with Na+, K+, Mg2+, CEC, and organic matter at p?<?0.01. The presence of seawater, clay mineralogy, and organic matter proves that it does play an important role in determining the CEC and soon relates to the pollution magnitude in the sediment.  相似文献   

15.
作为高放废物处置罐候选金属材料,低碳钢在处置库服役期间,其腐蚀产物侵入缓冲屏障,导致缓冲材料矿物相变与性能变异,威胁多重屏障体系的长期安全稳定。本文详细综述了国内外处置库深部还原环境所处的弱碱性化学场与中低温度场的变化趋势,认为处置库深部化学-温度还原条件可导致处置罐Fe腐蚀释放Fe~(2+)。在处置库长期运行过程中,蒙脱石与Fe~(2+)接触发生矿物相变,一方面Fe~(2+)置换蒙脱石八面体晶格中的Al~(3+)和Mg~(2+),还原Fe~(3+)或直接占据空位,生成次生矿物;另一方面Fe~(2+)交换蒙脱石层间的Na~+、K~+和Ca~(2+),转化为铁基蒙脱石。矿物相变可诱发缓冲屏障性能变异甚至退化。基于"抗矿物转化"理念,提出了下一阶段缓冲材料矿物相变研究方向,为地下实验室碳素钢选型、缓冲屏障验证试验设计以及屏障体系安全评价提供科学依据。  相似文献   

16.
Diffusion experiments with HTO, 36Cl−, Br−, I−, 22Na+, 85Sr2+ and 134Cs+ at trace concentrations in a single sample of Opalinus Clay are modeled with PHREEQC’s multicomponent diffusion module. The model is used first in a classical approach to derive accessible porosities, geometrical factors (the ratio of pore tortuosity and constrictivity) and sorption behavior of the individual tracers assuming that the clay is homogeneous. The accessible porosity for neutral species and cations is obtained from HTO, the anion exclusion volume from 36Cl− and Br−, and the cation exchange capacity from 22Na+. The homogeneous model works well for tritium, the anions and 22Na+. However, the 85Sr2+ and 134Cs+ experiments show an early arrival of the tracer and a front-form that suggest a dual porosity structure. A model with 10% dead-end pores, containing 19% of the total exchange capacity, can satisfactorily calculate all the experimental data. The Cs+ diffusion model builds on a 3-site exchange model, constructed from batch sorption data. The excellent agreement of modeled and measured data contradicts earlier reports that the exchange capacity for Cs+ would be smaller in diffusion than in batch experiments.The geometrical factors for the anions are 1.5 times larger than for HTO, and for the cations 2-4 times smaller than for HTO. The different behavior is explained by a tripartite division of the porespace in free porewater, diffuse double layer (DDL) water, and interlayer water in montmorillonite. Differences between estimated and observed geometrical factors for cations are attributed to increased ion-pairing of the divalent cations in DDL water as a result of the low relative dielectric permittivity. Interlayer and/or surface diffusion contributes significantly to the diffusive flux of Cs+ but is negligible for the other solutes. The geometrical factors for anions are higher than estimated, because pore constrictions with overlapping double layers force the anions to take longer routes than HTO and the cations. Small differences among the anions can also be attributed to different ion-pairing in DDL water.  相似文献   

17.
The influence of clay dispersion method on dewatering behaviour of a run-of-mine bentonite was examined to better understand the roles of calcium–sodium ion exchange and overall electrolyte concentration on the suppression of swelling and subsequent stabilisation of the clay. As with previous work, controlled dispersion of the clay directly into a swelling suppressing environment was observed to yield order of magnitude improvements in dewatering behaviour [de Kretser, R.G., Scales, P.J. and Boger, D.V., 1997. Improving clay-based tailings disposal: a case study on coal tailings. AIChE Journal. 43 (7), 1894–1903.]. The calcium ion, even after normalisation for its valence, yielded significantly better clay stabilisation performance than the sodium ion indicating the greater benefit afforded via divalent ion-exchange driven controlled dispersion. However the results also highlighted a synergistic effect of the double layer suppression effect on the efficacy of ion-exchange mediated controlled dispersion through simultaneous swelling suppression and structure preservation during the transient process of ion exchange on hydration. Studies of controlled dispersion in dual ion, Na+ and Ca2+, systems illustrated that although the efficacy of controlled dispersion deteriorated with an increase in the Na+ to Ca2+ ratio, even small amounts of calcium character could generate significant improvements in dewaterability over the pure sodium case. This result was relevant in terms of defining an operational window for the commonly used, but sparingly soluble calcium source, gypsum where the low deliverable calcium level could be more than offset by the controlled dispersion benefits of maintaining a higher overall salinity level. Based on the results presented, the potential impact of practical implementation of a controlled dispersion framework within a mineral processing operation was illustrated via numerical modelling of the operation of a steady state thickener.  相似文献   

18.
Groundwater of the unconfined aquifer (1,100 sq. km) of a two-tier coastal aquifer located in the Amol–Ghaemshahr plain, Mazandaran Province, Northern Iran, is classified into fresh and brackish water types. Fresh groundwater (FGW) samples (n = 36) are characterized by Ca2+ > Na+ > Mg2+ > K+ and HCO3 ? > Cl? > SO4 2? > NO3 ?. Spearman’s rank correlation coefficient matrices, factor analysis data, values of the C-ratio (av. = 0.89) and CAI and values of the molar ratios of Ca2+/HCO3 ?, Ca2+/SO4 2?, Mg2+/HCO3 ? and Mg2+/SO4 2? indicate that the ionic load in the FGW is derived essentially from carbonic acid-aided weathering of carbonates and aluminosilicates, saline/sea water trapped in the aquifer sediments (now admixed with the groundwater) and ion exchange reactions. Values of the CAI and Na+/Cl? molar ratio suggest that the part of the Ca2+ (±Mg2+) content in 23 FGW samples is derived from clay minerals of the aquifer matrix, and part of the Na+ content in 20, 12, and 3 FGW samples is derived, respectively, from alkali feldspar weathering, clay minerals of the aquifer matrix and rain water and/or halite. Brackish groundwater (BGW) samples (n = 4) contain Cl? as the dominant anion and their average total ionic concentration (38.65 meq/L) is 1.79 times higher than that of the FGW samples (21.50 meq/L). BGW pockets were generated by non-conservative mixing of FGW with the upconed saline water from the underlying saline groundwater zone of the semi-confined aquifer along bore wells involved in excessive extraction of groundwater from the unconfined aquifer. Groundwater belongs essentially to “high salinity, low sodium” irrigation water class.  相似文献   

19.
The cation-exchange characteristics of Amazon River suspended sediment have been studied in order to determine the contribution of exchangeable cations to the geochemical fluxes from the river. Sediment samples were obtained throughout most of the Amazon Basin. The range of exchangeable cation compositions is very narrow in the river and in seawater as well. In river water, the exchangeable cation complement (equivalent basis, exclusive of H+) is 80% Ca2+, 17% Mg2+, 3% Na+ plus K+. In seawater Na+ and Mg2+ are about equal (38%) while Ca2+ ~ 15% and K+ ~ 9%.On reaction with seawater, river suspended sediment took up an amount of Na+ equal to nearly one-third of the dissolved river load, as well as amounts corresponding to 15–20% of the dissolved fluvial K+ and Mg2+. These estimates reflect an unusually high suspended-sediment:dissolved-solids ratio of 6.4 at the time of sampling. At a more representative world average ratio of four, the uptake of Na+ would be 20% of the dissolved fluvial load, and that for K+ and Mg2+ about 10%. Over the annual cycle of the Amazon, it is estimated that ion exchange has a still smaller effect, as a consequence of the low average suspended-solids:dissolved-solids ratio of 1.7.Variations in the ratio XCaXMg, the equivalent fraction of exchangeable Ca2+ and Mg2+, throughout the river, can be described by a single isotherm. This same isotherm accurately describes the distribution of exchangeable Ca2+ and Mg2+ on sediment equilibrated with seawater, despite that a high proportion of exchange sites is occupied by Na+ and K+.  相似文献   

20.
Groundwater sampling was accomplished in the basaltic sequence of the Rh?n mountain range, Germany, in order to investigate hydrochemical groundwater evolution and to delineate mineral alteration reactions involved in natural weathering. The hydrochemical compositions of near-surface groundwaters indicate a Ca/Mg–HCO3 type with near-neutral pH and evolve to a Na–HCO3 type with high pH at greater depth. Column experiments were performed with basaltic and phonolitic rock samples to determine individual mineral alteration reactions. The basic reactions could be related to the alteration of olivine, Ca-pyroxene, plagioclase, pyrrhotite, and feldspathoids under formation of secondary clay minerals (smectites, illite) and goethite. The mineral alteration reactions deduced from the leaching experiments by inverse modelling were found to be consistent with the mineral reactions associated with the natural groundwaters. The reactions calculated for groundwater evolution involve the alteration of primary and secondary minerals to produce low-T mineral phase. The conversion of secondary Na-beidellite to illite occurs at a later stage of groundwater evolution, reducing the concentrations of K+ and Mg2+. Near-surface groundwaters do not indicate significant cation exchange. Initial cation exchange requires elevated pH values, with Mg2+ removed from solution preferred to Ca2+. Na-alkalisation of the groundwaters at greater depth suggests the exchange of Na+ for Mg2+ and Ca2+ on Na-beidellite, supported by cation exchange on coatings of iron hydroxides as alteration products. Among the mature high-pH groundwater at greater depth, the dissolution of anorthite and albite has significant effect on groundwater composition.  相似文献   

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