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1.
We have measured with an electron microprobe the Mg, Al, Si, Ca, Ti, Mn, and Fe contents of five strongly heated stony cosmic spherules (sCS) from the South Pole water well. We have also measured the isotopic compositions of Si, and when possible of Mg and of Fe in these objects by ion microprobe. Except for iron, the measured elemental compositions are chondritic within a factor of 2. In four samples, the ratio of 57Fe/56Fe exceeds the terrestrial value by 3.5‰ to 48‰. Mass-dependent fractionation of the isotopes of Si ranges from ∼2 to ∼8 ‰/AMU in three samples. Mg is clearly fractionated in only one sample, for which δ25Mg = ∼8 ‰. The extent of mass-dependent fractionation of the isotopes and, by implication, of evaporative loss generally follows a trend Mg < Si < Fe. The trend is similar to that found in laboratory heating experiments of charges with solar composition. Although the observed isotopic inhomogeneities within some samples call into question the strict validity of the Rayleigh equation for the sCS, its approximate application to our new and to previously published results for Mg suggests that evaporative losses of greater than 40 wt.% occur rarely from sCS, and that the precursor grains of the sCS had a CM-carbonaceous-chondrite-like complement of Mg, Si, Ca, and Al. Low Fe contents relative to CM abundances could reflect an unusual precursor composition, or, more probably, losses by processes that did not fractionate isotopes, i.e., ejection of immiscible FeS and FeNi beads from the melt or rapid, complete separation and decomposition of FeS at the surface.  相似文献   

2.
Fifteen samples of (Mg,Fe)SiO3 majorite with varying Fe/Mg composition and one sample of (Mg,Fe)(Si,Al)O3 majorite were synthesized at high pressure and temperature under different conditions of oxygen fugacity using a multianvil press, and examined ex situ using X-ray diffraction and Mössbauer and optical absorption spectroscopy. The relative concentration of Fe3+ increases both with total iron content and increasing oxygen fugacity, but not with Al concentration. Optical absorption spectra indicate the presence of Fe2+–Fe3+ charge transfer, where band intensity increases with increasing Fe3+ concentration. Mössbauer data were used in conjunction with electron microprobe analyses to determine the site distribution of all cations. Both Al and Fe3+ substitute on the octahedral site, and charge balance occurs through the removal of Si. The degree of Mg/Si ordering on the octahedral sites in (Mg,Fe)SiO3 majorite, which affects both the c/a ratio and the unit cell volume, is influenced by the thermal history of the sample. The Fe3+ concentration of (Mg,Fe)(Si,Al)O3 majorite in the mantle will reflect prevailing redox conditions, which are believed to be relatively reducing in the transition zone. Exchange of material across the transition boundary to (Mg,Fe) (Si,Al)O3 perovskite would then require a mechanism to oxidize sufficient iron to satisfy crystal-chemical requirements of the lower-mantle perovskite phase.  相似文献   

3.
(Mg,Fe)(Si,Al)O3 perovskite samples with varying Fe and Al concentration were synthesised at high pressure and temperature at varying conditions of oxygen fugacity using a multianvil press, and were characterised using ex?situ X-ray diffraction, electron microprobe, Mössbauer spectroscopy and analytical transmission electron microscopy. The Fe3+/ΣFe ratio was determined from Mössbauer spectra recorded at 293 and 80?K, and shows a nearly linear dependence of Fe3+/ΣFe with Al composition of (Mg,Fe)(Si,Al)O3 perovskite. The Fe3+/ΣFe values were obtained for selected samples of (Mg,Fe)(Si,Al)O3 perovskite using electron energy-loss near-edge structure (ELNES) spectroscopy, and are in excellent agreement with Mössbauer data, demonstrating that Fe3+/ΣFe can be determined with a spatial resolution on the order of nm. Oxygen concentrations were determined by combining bulk chemical data with Fe3+/ΣFe data determined by Mössbauer spectroscopy, and show a significant concentration of oxygen vacancies in (Mg,Fe)(Si,Al)O3 perovskite.  相似文献   

4.
A charge-consistent numerical model for the joint (regular and stochastic) acceleration of iron by a spherical shock wave propagating in the solar corona is proposed. Large-scale irregularities of the plasma density and the nonisothermal injection of ions are taken into account. For the case of iron, the energy dependence of the mean charge qFe(E) is determined by the relationships between the characteristic acceleration time, the charge-variation time for the accelerated ions, and the time for their trapping in regions of high plasma density. Due to the global inhomogeneity of the medium, these relationships depend on the shock speed. Our calculations indicate that photoionization by soft X-rays from flare regions can substantially change the charge states of heavy ions only in the most powerful solar events (both impulsive and gradual).  相似文献   

5.
Using approximation of a uniform background (the jellium model) for a condensed dispersed phase, the analytical expressions describing a spatial distribution of the potential of the electric field and electron concentration in the low-temperature plasma at equilibrium which contains hollow spherical microparticles are obtained. The influence of heating temperature of plasma on the above distributions is studied, and the dependencies of the charge on microparticle radius, the size of the microparticle cavity and the absolute temperature of plasma are calculated. It is shown that electrons can be emitted not only into the surrounding plasma but also into the cavity of the particles.  相似文献   

6.
The formation of the energy spectra of heavy ions at the front of a parallel shock is considered taking into account ionization and recombination during the acceleration. An analytic solution for ions with three possible charge states is obtained and applied to the acceleration of the anomalous cosmic-ray component at the boundary of the heliosphere. In addition, a more general numerical model for such acceleration at a spherical shock front is developed and used to obtain the energy dependence of the mean charges for C, N, O, Ne, Si, S, Ar, and Fe ions. The model implies that highly excited ions begin to dominate over ions with low charges at energies above 1 MeV/nucleon, in agreement with observational data.  相似文献   

7.
甘肃庄浪全新世黄土-古土壤序列元素分布特征及意义   总被引：6，自引：1，他引：5  
通过对渭河上游XJN全新世剖面的Fe、Al、Si、K、Ca、Mg、Na、Ti和Sr元素含量的分析,发现这些元素的分布与气候密切相关。在剖面中表现为:迁移序列是Ca>Sr>Na>Mg,Fe、Al、Si、K和Ti则相对富集;Ca-Sr关系呈两段式分布,指示全新世早期的一次环境变化;Ki残积系数增大,Ca/Mg比值减小,指示化学风化作用增强。  相似文献   

8.
Bulk compositions and mineral analyses for forty-one, large, garnet- and spinel-facies peridotite xenoliths from the Udachnaya kimberlite in the central Siberian platform have many similarities to those of well-studied peridotites from the Kaapvaal craton in southern Africa. Coarse Mg-rich lherzolites and harzburgites with equilibration temperatures below 1000 °C are abundant and are believed to form the principal rock type in the Siberian lithosphere. The low-temperature Udachnaya peridotites have an average mg number [Mg/(Mg+Fe)] of 92.6 with a wide dispersion in modal enstatite, ranging to over 40 wt%. High-temperature peridotites are relatively richer in Fe and Ti and are commonly deformed, with porphyroclastic or mosaic-porphyroclastic textures, some of the latter having fluidized enstatite. The Udachnaya peridotites have experienced late-stage metasomatism before, during and after eruption. Garnets and pyroxenes in many of the high-temperature rocks are zoned, probably by reaction with melt prior to eruption. Virtually all the peridotites contain secondary diopside, inhomogeneous on a micron scale, that mantles primary orthopyroxene. It is believed to have crystallized along with lesser amounts of intergranular calcite and monticellite during eruption. Bulk analyses for total Fe in many specimens are higher than whole-rock Fe calculated from the electron probe analyses and the modes. The magnitude of the difference between the two measurements of total Fe correlates with loss-on-ignition, suggesting that Fe has been introduced during serpentinization following eruption. These late metasomatic processes have thus affected some major as well minor and trace element compositions. The similarities in bulk composition of peridotites from Udachnaya and the Kaapvaal are evidence of a common origin. Low-temperature cratonic peridotites differ from oceanic peridotites in having higher mg numbers (>92) and in having relatively high but wide-ranging modal enstatite (Mg/Si = 1.06–1.49 weight fraction). The Udachnaya low-temperature peridotites have an inverse correlation between FeO (calculated from the probe analyses and modes) and SiO2. This correlation is also present in the Kaapvaal data but is complicated by a greater range in fertility that produces a positive variation of Fe with Si. A negative trend for Fe/Si can be seen within a portion of the Kaapvaal data, that for low-Ca harzburgites, in which the variation in fertility is restricted. The negative trends for Fe/Si can be interpreted as a consequence of either segregation of olivine and orthopyroxene by metamorphic differentiation or partial sorting during cumulate formation. Received: 18 June 1996  / Accepted: 11 February 1997  相似文献   

9.
《Applied Geochemistry》1997,12(1):83-95
In a column experiment, acidic groundwater from Pinal Creek Arizona, a Cu mining area, was eluted through a composited alluvial sample obtained from a core that had been removed from a well downgradient of the acidic groundwater. The minerals present in typical grains and flakes in the alluvium before and after the elution were determined by X-ray diffraction (XRD), scanning electron microscopy, and energy dispersive multichannel analyses (EDX). The concentrations of Fe, Ti, Mn, Si, Al, Na, Ca, K, Mg and S in these grains and flakes and in their microcrystalline surface coatings were measured by EDX.In addition to magnetite, hematite, and Fe-Ti oxides, Fe was most concentrated in micas (especially biotite-like flakes) and in the microcrystalline coatings. The measured elements in these microcrystalline coatings were primarily K, Fe, Al, and Si. The microcrystalline coatings on the mica flakes also contained Mg. The approximate l:3 Mg:Si atomic ratios (ARs)_of the biotite-life flake both before and after the elution would suggest that the Fe deposited during the elution had not substituted for Mg in these flakes. As a result of the elution, assuming no loss of Si, the averaged recorded Fe:Si AR of the microcrystalline coatings increased from (0.46 to 0.58):3.00.Iron deposition on the typical grains and flakes may relate to the presence of Fe in the particle on which it is deposited or to the presence of Fe in the microcrystalline surface coatings before elution. The data here are not sufficient for a statistical evaluation, but elution caused the following trends: (l) The Fe:Si AR increased in the (K,Fe,Al,Si)-microcrystalline surface coatings; (2) For the mica flakes, there was more than a 2-fold increase in the Fe:Si AR for the microcrystalline surface coatings of the Fe-rich biotite-like flakes but no measurable increase of the Fe:Si AR for the microcrystalline surface coatings of the muscovite-like flakes that contained 3–5 times less Fe; (3) Also for the biotite-like flakes, the increase in Fe:Si AR was greater in the flakes that had a higher Fe:Si AR; (4) The Fe deposition on the Fe-rich microcrystalline surface coatings of the feldspar was much greater than on the Fe-poor, beige quartz and feldspar grains that, prior to elution, had only CaS04 microcrystalline coatings; and (5) No Fe was deposited on Fe-poor grains with no microcrystalline surface coating.  相似文献   

10.
 A 2-D periodic ab initio Hartree–Fock LCAO study was performed on Fe-substituted 1:1 sheet silicate, lizardite. The atomic orbitals were described by large-core pseudopotentials (Fe atoms) and a sp basis set (the other atoms). Calculated atomic charges and the results of bond population analysis indicate that the Fe-O bond was as ionic as the Mg-O. This hypothesis was supported by calculated density of states and electron density maps. Increasing Fe for Mg substitution changed the shape of projected density of states (PDOS) of O(p) orbitals. Received: 27 January 2000 / Accepted: 21 May 2000  相似文献   

11.
大麻坪地区二辉橄榄岩部分熔融实验研究   总被引：1，自引：0，他引：1  
本文以采自大麻坪地区汉诺坝玄武岩中的二辉橄榄岩包体为初始实验物料,在压力1.0～3.0 GPa、温度1350～1550℃条件下进行了部分熔融实验,对实验产物进行了岩相学研究和电子探针成分分析。二辉橄榄岩在1350℃开始熔融,在实验的温度压力范围内,熔融程度为10%～30%。随熔融程度的升高,部分熔融后残余岩石倾向于向富镁、低铁、低钙、低硅的趋势演化,而部分熔融产生的熔体则倾向于富镁、富铁、低铝、低硅的趋势演化。在岩石化学图解上本次实验中二辉橄榄岩部分熔融产生的熔体化学组成与汉诺坝地区拉斑玄武岩的组成相近。随熔融程度升高,熔体具有从苦橄质→玄武质演化的趋势。  相似文献   

12.
The elemental abundances of lunar surface are the important clues to study the formation and evolution history of the Moon. In 2010, China＇s Chang＇E-2 （CE-2） lunar orbiter carried a set of X-ray spectrometer （XRS） to investigate the elemental abundances of the lunar surface. During CE-2＇s life span around the Moon, the XRS ex- perienced several events of solar flare. The X-ray solar monitor onboard recorded the spectra of solar X-rays at the same time. In this paper, we introduced the XRS instrument and data product. We analyzed the characteristics of the XRS data. Using the data obtained during an M solar flare event which had occurred on Feb. 16, 201 l, we derived the elemental abundances ofMg, A1, Si, Ca and Fe of the lunar surface in the Oceanus Procellarum. Finally, we dis- cussed the factors that influence the accuracy of the inversion.  相似文献   

13.
Reidar G. Trnnes 《Lithos》2000,53(3-4):233-245
Melting experiments were performed on an FeO-rich bulk Earth model composition in the CMFAS system in order to investigate the partitioning of major elements between coexisting minerals and melts. The starting material (34.2% SiO2, 3.86% Al2O3, 35.2% FeO, 25.0% MgO and 1.88% CaO), contained in Re-capsules, was a mixture of crystalline forsterite and fayalite, and a glass containing SiO2, Al2O3, and CaO. Olivine is the first liquidus phase at 10 GPa but is replaced by majoritic garnet (ga) in the 15–26 GPa range. Magnesiowüstite (mw) crystallizes close to the liquidus and is joined by perovskite (pv) at 26 GPa.

The quenched melt compositions are homogeneous throughout the melt region of the charges and are only slightly enriched in Si, Ca and Fe, and depleted in Mg, relative to the starting composition. The Fe/Mg and Ca/Al ratios in all of the minerals increase rapidly below the liquidus to become compatible with the bulk composition at the solidus. At 26 GPa, a relative density sequence of mw>pv>melt>ga is observed. This indicates that majorite floating, combined with the sinking of magnesiowüstite and perovskite can be expected during the solidification of a Hadean magma ocean and in hot mantle plumes early in the Earth's history. The mineral–melt partitioning relations indicate that fractional crystallization or partial melting in the transition zone and the upper part of the lower mantle would increase the Fe/Mg and Ca/Al ratios of the melt, even if magnesiowüstite was predominant in the solid fraction. A significant contribution of accumulated mw to the segregation of the protocore is therefore unlikely. The suggested process of perovskite fractionation to the lower mantle is not capable of increasing the Mg/Si ratio in the residual melt, and the combined fractionation of perovskite and magnesiowüstite produces a melt with elevated ratios of Si/Mg, Ca/Al and Fe/Mg.  相似文献   


14.
X-PEEM images and XPS were collected on isolated layers of three synthetic swelling clays, one hectorite and two saponites with various charge, recording the Si(2p), Al(2p) and Mg(2p) core level spectra from the clay sheets. Spectra were fitted to determine the different components of the core levels. Due to their large full width at half maximum, Si XPS spectra were fitted using two to three doublets. It appears that, for a given clay mineral, Si, Al and Mg binding energies (BE) were constant, for all the observed layers. However, variations of the Si BE were observed depending on the nature of the mineral investigated. The various components obtained from the fit of Si spectra could be assigned to different substitution rates; binding energy shifting to lower values with substitution increase in the layer. Furthermore, variations in Si BE according to charge location were assigned to the influence of exchangeable cation.  相似文献   

15.
The atomic fractions Mg/(Mg + Fe) and the Mg-Fe distribution coefficient $$K_{{\text{D}}{\text{.Mg - Fe}}}^{{\text{Ca - am - Cum}}} \left( { = \tfrac{{[{\text{Mg/Fe]}}_{{\text{Ca - am}}} }}{{{\text{[Mg/Fe]}}_{{\text{Cum}}} }}} \right)$$ are calculated for 31 metamorphic cummingtonite-hornblende pairs. Data on 21 pairs are taken from the litterature, and new electron microprobe analyses and structural formulae are presented of nine pairs from Tydal, Sör-Tröndelag, Norway, and of one pair from Cooma, N.S.W., Australia (cf. Kisch, 1969). The electron microprobe methods used are described, particularly the use of mineral standards, and the variation of the mass absorption in substitution series. The hornblendes from the Tydal pairs are markedly pargasitic in composition, and contain minor proportions of the cummingtonite “molecule”. The Mg-Fe distributions in the cummingtonite-hornblende pairs — as plotted on a [Mg/(Mg + Fe)]Ca-am vs. [Mg/(Mg + Fe)]Cum diagram (Fig. 3) — differ significantly from the Mg-Fe distribution curve for cummingtonite-actinolite pairs from Quebec (Mueller, 1961). Whereas the actinolites have markedly higher Mg/Fe ratios than the co-existing cummingtonites (K D.Mg-Fe Ca-am-Cum ≈ 1.5–2.0), the cummingtonite-hornblende pairs diverge towards lower values from the distribution coefficient. In most of the metamorphic cummingtonite-hornblende pairs — including the nine pairs from Tydal — the Mg/Fe ratio of the hornblende is lower than in the co-existing cummingtonite, i.e K D.Mg-Fe Ca-am-Cum <1. A relation appears to exist between the Mg-Fe distribution and the Al content of the calcic amphibole phase. This is believed to be due to the non-random distribution of AlY among the octahedral lattice sites: in hornblende AlVI enters the M 1+M3 positions, in which Mg is preferred over Fe, rather than M 2, in which Fe is preferred (Ghose, 1965). Since the cummingtonites remain Al-poor, the over-all Mg/Fe ratio in the hornblende is reduced relative to the co-existing cummingtonite as a result. The variations of the Mg-Fe distribution in the cummingtonite-hornblende pairs can also be related directly to the presence and composition of the plagioclase and other Al-rich phases in the metamorphic mineral assemblage. In any range of Mg/Fe ratios, the cummingtonite-hornblende pairs associated with oligoclase have lower distribution coefficients (0.61–0.81; 12 pairs) than those associated with calcic plagioclase or plagioclase-free assemblages (0.97 to 1.89; 6 pairs); the pairs associated with andesine have intermediate Mg-Fe distributions (0.74–1.15; 6 pairs).  相似文献   

16.
The topological properties of the electron density distributions for more than 20 hydroxyacid, geometry optimized molecules with SiO and GeO bonds with 3-, 4-, 6- and 8-coordinate Si and Ge cations were calculated. Electronegativities calculated with the bond critical point (bcp) properties of the distributions indicate, for a given coordination number, that the electronegativity of Ge (∼1.85) is slightly larger than that of Si (∼1.80) with the electronegativities of both atoms increasing with decreasing bond length. With an increase in the electron density, the curvatures and the Laplacian of the electron density at the critical point of each bond increase with decreasing bond length. The covalent character of the bonds are assessed, using bond critical point properties and electronegativity values calculated from the electron density distributions. A mapping of the (3, −3) critical points of the valence shell concentrations of the oxide anions for bridging SiOSi and GeOGe dimers reveals a location and disposition of localized nonbonding electron pairs that is consistent with the bridging angles observed for silicates and germanates. The bcp properties of electron density distributions of the SiO bonds calculated for representative molecular models of the coesite structure agree with average values obtained in X-ray diffraction studies of coesite and danburite to within ∼5%. Received: 18 August 1997 / Revised, accepted: 19 February 1998  相似文献   

17.
Structural energetics of the alkali feldspars have been studied using a “lattice” or structure energy model. Electrostatic energies, U e,for 20 well-refined, non-intergrown alkali feldspars were calculated using Bertaut's (1952) summation procedure and average about ?13,400 kcal/mol; the repulsive energies of the alkali site in each structure (～15 kcal/mol) were calculated using repulsive parameters for K-O and Na-O interactions estimated from bulk modulus data for NaF and KF and the exponential form of the repulsive potential. Using a procedure in which the position of the alkali cation was varied while the oxygen cage was kept fixed, structure energy gradients for the alkali sites of high albite and a hypersolvus Ab42Or58 structure were computed. In both cases, a broad structure energy well, elongated approximately parallel to c and subparallel to the observed split Na positions, was found. In both structures there is a single energy minimum corresponding closely with the observed single alkali positions. Comparison of U e values for the alkali feldspars with different K/Na ratios shows that intermediate compositions are predicted to be less “stable” than either endmember and that the potassic end-member is predicted to be less “stable” than the sodic one, assuming that all other factors contributiong to the free energies of each phase are approximately the same. Comparison of U e values for the high albite and low sanidine structures with different Al/Si distributions and a fixed tetrahedral framework indicates that the ordered charge distributions are 63.0 and 54.8 kcal/mol, respectively, more “stable” than the disordered distributions. Smaller, more realistic energy differences were obtained by using U evalues averaged from four separate calculations with a +3 charge on a different T site in each and with +4 charges on the other T sites. If, in addition, the charges on cations and oxygen are reduced to half their nominal formal charges, in agreement with Pauling's electroneutrality principle and the results of recent molecular orbital calculations on silicates, the predicted electrostatic energy differences are reduced to 3.6 and 1.6 kcal/mol, respectively. These calculations also indicate that the T1O site in the high albite structure energetically favors Al and that the Al/Si distribution determines the Na position within the alkali site.  相似文献   

18.
Solid solution in vesuvianite is elucidated by examining chemical trends and cation abundances in 22 microprobe analyses of samples from the Big Maria Mountains, southeastern California. Two recent structure refinements indicate 50 filled cation sites per formula, providing the basis for data normalization. Previous optical absorption and Mössbauer studies help clarify site occupancies. Stoichiometric abundances of Si and Ca + Na indicate 18 and 19 per formula, filling all 4- and 8-fold sites respectively. The four 6-fold A-sites are filled with Al. The solid solution occurs mainly within the eight 6-fold AlFe-sites (Al, Mg, Fe2+, Fe3+, Ti) and one 5-fold B-site (Mg, Fe2+, Fe3+). Chemical trends and crystal chemical constraints delineate eight independent substitutions.An extensive solid solution in the elements Mg, Fe, Al, and Ti suggests considerable potential as a petrogenetic indicator. In order to treat equilibria involving vesuvianite thermodynamically, a reference composition must be chosen and activity-composition relations modeled. For a reference composition, Mg-vesuvianite (Fe, Ti, Na-free) was chosen because of its chemical simplicity, but problems in ascertaining its stoichiometry have led previous workers to propose at least six different formulas. In this study, its formula is determined from the microprobe analyses by applying exchange vectors to substitute components of pure Mg-vesuvianite for Fe and Ti. This yields Ca19Mg2Al11-Si18 O69(OH)9, with AlFe-sites=MgAl7, and B-sites=Mg. Subdivision of the AlFe-sites into at least two distinct sites is suggested by observed chemical trends which are explanable only when different substitutions are considered to operate within different AlFe-sites.A thermodynamic mole fraction is formulated for Mg-vesuvianite based on an ideal mixing-on-sites solution model. A method is provided for estimating the distribution of Fe between the AlFe- and B-sites. Thermodynamic mole fractions calculated using Fe site distributions estimated from microprobe data yield results similar to those calulated using Fe site distributions determined from Mössbauer analysis.  相似文献   

19.
The dissolution rate of illite, a common clay mineral in Australian soils, was studied in saline-acidic solutions under far from equilibrium conditions. The clay fraction of Na-saturated Silver Hill illite (K1.38Na0.05)(Al2.87Mg0.46Fe3+0.39Fe2+0.28Ti0.07)[Si7.02Al0.98]O20(OH)4 was used for this study. The dissolution rates were measured using flow-through reactors at 25 ± 1 °C, solution pH range of 1.0-4.25 (H2SO4) and at two ionic strengths (0.01 and 0.25 M) maintained using NaCl solution. Illite dissolution rates were calculated from the steady state release rates of Al and Si. The dissolution stoichiometry was determined from Al/Si, K/Si, Mg/Si and Fe/Si ratios. The release rates of cations were highly incongruent during the initial stage of experiments, with a preferential release of Al and K over Si in majority of the experiments. An Al/Si ratio >1 was observed at pH 2 and 3 while a ratio close to the stoichiometric composition was observed at pH 1 and 4 at the higher ionic strength. A relatively higher K+ release rate was observed at I = 0.25 in 2-4 pH range than at I = 0.01, possibly due to ion exchange reaction between Na+ from the solution and K+ from interlayer sites of illite. The steady state release rates of K, Fe and Mg were higher than Si over the entire pH range investigated in the study. From the point of view of the dominant structural cations (Si and Al), stoichiometric dissolution of illite occurred at pH 1-4 in the higher ionic strength experiments and at pH ?3 for the lower ionic strength experiments. The experiment at pH 4.25 and at the lower ionic strength exhibited lower RAl (dissolution rate calculated from steady state Al release) than RSi (dissolution rate calculated from steady state Si release), possibly due to the adsorption of dissolved Al as the output solutions were undersaturated with respect to gibbsite. The dissolution of illite appears to proceed with the removal of interlayer K followed by the dissolution of octahedral cations (Fe, Mg and Al), the dissolution of Si is the limiting step in the illite dissolution process. A dissolution rate law showing the dependence of illite dissolution rate on proton concentration in the acid-sulfate solutions was derived from the steady state dissolution rates and can be used in predicting the impact of illite dissolution in saline acid-sulfate environments. The fractional reaction orders of 0.32 (I = 0.25) and 0.36 (I = 0.01) obtained in the study for illite dissolution are similar to the values reported for smectite. The dissolution rate of illite is mainly controlled by solution pH and no effect of ionic strength was observed on the dissolution rates.  相似文献   

20.
The distributions of Al 3+/Mg 2+ and Al 3+/ Fe 3+ were studied in the octahedral sheet of illites and smectites. Cation exchange interaction parameters J i, as first, second, third and fourth neighbours were calculated by means of empirical interatomic potentials. Several compositions with different interlayer cations and tetrahedral charge were studied in both Al/Mg and Al/Fe systems. The values of J i parameters were similar in all Al/Mg samples. From these J i values, a strong trend to form AlMg pairs was observed in the Al/Mg system. In the Al/Fe system, the values of J i are very small, indicating no preference for Al/Fe mixing. From these J i parameters, Monte Carlo simulations of octahedral cation ordering were performed. In the Al/Mg system, an order/disorder phase transition was observed obtaining a fully ordered distribution without presence of an MgMg pair, according to experimental data. Similar phase transitions were observed for the octahedral compositions Al/Mg 1/1 and 3/1. In the Al/Fe system an order/disorder phase transition was also detected but at very low temperature for illite and smectite. Complete Al/Fe mixing is observed in the most stable ordered distribution. This is consistent with experimental results for synthetic Fe/Al smectites.  相似文献   

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