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1.
Traditionally, land subsidence that results from groundwater over-pumping has often been described by the theory of consolidation. The mechanism of land subsidence due to the dehydration of clay minerals is not well addressed. A model of the “hydration state of smectite”, and a “solid solution model of smectite dehydration”, incorporating a thermodynamic solid solution model and laboratory results concerning clay-water systems of swelling pressure, hydration state and basal spacing in smectite interlayer, are employed to examine the effect of the release of water from the smectite interlayer on land subsidence in the coastal area of the Chou-Shui River alluvial fan and the Yun Lin offshore industrial infrastructure complex in Taiwan. The results indicate that 9.56–22.80% of the total cumulative land subsidence to a depth of 300 m is consistent with smectite dehydration following the over-pumping of groundwater. This dehydration-related land subsidence occurred to a depth of 0–60 m, with subsidence due to smectite dehydration accounting for 6.20–13.32% of the primary consolidation. Additionally, the total amount of subsidence resulting from both smectite dehydration and primary consolidation is consistent with the subsidence observed in the field. This study reveals that smectite dehydration appears to be important in assessing and predicting land subsidence in shallow aquifer systems.  相似文献   

2.
We propose a thermodynamic approach to model the stepwise dehydration with increasing temperature or decreasing H2O activity of K, Na, Ca and Mg-smectite. The approach relies on the relative stability of the different solid-solutions that describe the hydration of di- or trioctahedral-smectites containing 0, 1, 2 or 3 interlayer water layers. The inclusion of anhydrous mica end-members makes it possible to cover, with the same solid-solution model, the entire range of composition from low-charge smectite to mica, through high-charge smectite and illite. Non-ideal Margules parameters were used to describe the non-ideality of the solid solutions between the hydrated and dehydrated smectite end-members. Standard state properties of all smectite end-members as well as Ca- and Mg-muscovite and -phlogopite were initially estimated by oxide summation. These values were then refined and the other non-ideal interactions were estimated on the basis of different experimental data. The stepwise dehydration of smectite, and its stability and compatibility relations were calculated by Gibbs free energy minimising. Our results account for the progressive evolution of smectite to interlayered illite/smectite and then to mica, as observed in nature and experiments, and our model provides an explanation for the thermodynamic stability of smectite and illite/smectite compared to mica + kaolinite or pyrophyllite assemblages. The results suggest that the enthalpic contribution of interlayer water is a function of the ionic potential of the interlayer cation and the number of interlayer water molecules. This evolution makes possible to estimate the standard-state thermodynamic parameters and hydration-temperature behaviour of smectite of virtually all possible compositions. For the four-interlayer cations considered in the study, our model reproduces the 3 → 2 → 1 water-layer transitions that accompany a reduction of water activity or an increase of temperature at ambient pressure. The range of water content and interlayer distance calculated for the 3w, 2w and 1w states are also in fair agreement with the experimental values at ambient pressure.  相似文献   

3.
Isothermal thermogravimetric experiments have been carried out to determine the reaction kinetics of the dehydration processes in fuller's earth, a natural Ca-montmorillonite. Dehydration in swelling clays is a complex reaction, and analysis of the thermogravimetric data using empirical rate equations and time-transformation analysis reveals that the nature of the rate controlling mechanism is dependent upon both the temperature regime of the sample as well as the extent of reaction. For fuller's earth, we find that the dehydration kinetics are dominated by a nucleation and growth mechanism at low temperatures and fractions transformed (stage I), but above 90 °C the last stages of the reaction are diffusion controlled (stage II). The activation energy for dehydration during stage I is around 35 kJ · mol−1, whereas the removal of water during stage II requires an activation energy of around 50 kJ · mol−1. These two stages of dehydration are associated with primary collapse of the interlayer (stage I) and movement of water that is hydrated to cations within the interlayer (stage II). Received: 28 August 1998 / Revised, accepted: 27 January 1999  相似文献   

4.
Clay minerals associated with intra-volcanic bole horizons of varied colours and thicknesses contain montmorillonite, halloysite and kaolinite, show distinct microstructures and microaggregates. In kaolinite, Fe3+ ions substitute for Al3+ at octahedral sites. Most of these clays are dioctahedral type, show balance between net layer and interlayer charges. The interstratified illite — smectite (I/S) mixed layers containing variable proportions of montmorillonite. Illite contains sheet-like, well oriented microaggregates. The parallel stacks of chlorite sheets show chlorite/smectite (C/S) mixed layers. Progressive enrichment of Fe and depletion of Al ions with the advancement of kaolinization process is observed. High order of structural and compositional maturity observed in these bole clays, indicate long hiatus between the two volcanic episodes.  相似文献   

5.
Clay minerals of about 600 samples from drill cores in the Tertiary shales of the Rhinegraben, were analysed by X-ray diffraction methods. It was found that the abundance of smectite decreases with increasing amounts of mixed layer clays and illites, suggesting a diagenetic alteration of smectite with increasing temperatures of the sediments as was also observed in other sedimentary basins. As for the relation between smectite alteration and temperatures as measured in sample depths, in the marine Graue Schichtenfolge (Middle Oligocene) when temperatures reach 70°C and over, smectite no longer is to be found. In the limnic Bunte Niederröderner Schichten (Upper Oligocene) the maximum temperature of smectite occurrence is about 80°C. These temperatures also fit the results of former field studies of the thermal stability of smectite. In the brackish to limnic Obere and Untere Hydrobienschichten (Lower Miocene) however, smectite seems to have disappeared already at a temperature of over 30°C. Although the smectite distribution in the latter formations may depend partly on its inhomogenous deposition there is also evidence for the diagenetic alteration of smectite in these formations. The rapid disappearance of smectite in these formations was possibly caused by a greater availability of potassium ions since high permeability of these strata provide extraordinarily good mobility of the pore solutions. In the older Lymnäenmergel formation (Upper Eocene) a more advanced stage of smectite alteration is found as compared to the other formations at corresponding temperatures. This is considered to be the consequence of the longer duration of diagenesis and the rock salt inclusions of this saline formation which might have enriched the pore solutions with potassium ions.  相似文献   

6.
The results of the study of clay mineral alterations in Upper Pleistocene sediments of the southern trough in the Guaymas Basin (Gulf of California) due to the influence of hydrothermal solutions and heat produced by sill intrusions are discussed. Core samples from DSDP Holes 477 and 477A were taken for the analysis of clay minerals. Application of the method of modeling X-ray diffraction patterns of oriented specimens of the finely dispersed particles made it possible to establish the phase composition of clay minerals, determine their structural parameters, and obtain reliable quantitative estimates of their contents in natural mixtures. The modeling data allowed us to characterize reliably the transformation of clay minerals in sediments of the hydrothermally active southern trough in the Guaymas Basin. In Upper Pleistocene sandy–clayey sediments of the southern trough, changes in the composition of clay minerals occurred under the influence of a long-living hydrothermal system. Its lower part (interval 170.0–257.5 m) with maximum temperatures (~300°C) was marked by the formation of chlorite. Terrigenous clay minerals are not preserved here. Saponite appears at a depth of 248 m in the chlorite formation zone. Higher in the sedimentary section, the interval 146–170 m is also barren of terrigenous clay minerals. Sediments of this interval yielded two newly formed clay minerals (chlorite and illite), which were formed at lower temperatures (above 180°C and below 300°C, approximately up to ~250°C), while the relatively low-temperature upper part (110–146 m) of the hydrothermal system (from ~140°C to ~180°C) includes the mixture of terrigenous and newly formed clay minerals. Terrigenous illite is preserved here. Illitization of the mixed-layer illite–smectite was subjected to illitization. The terrigenous montmorillonite disappeared, and chlorite–smectite with 5–10% of smectite layers were formed. In the upper interval (down to approximately 110 mbsf), the composition of terrigenous clay minerals remains unchanged. They are composed of the predominant mixed-layer illite–smectite and montmorillonite, the subordinate illite, mixed-layer chlorite–smectite with 5% of smectite layers, mixed-layer kaolinite–smectite with 30% of smectite layers, and kaolinite. This composition of clay minerals changed under the influence of sill intrusions into the sedimentary cover at 58–105 m in the section of Hole 477. The most significant changes are noted in the 8-m-thick member above the sill at 50–58 m. The upper part of this interval is barren of the terrigenous mixed-layer illite–smectite, which is replaced by the newly formed trioctahedral smectite (saponite). At the same time, the terrigenous dioctahedral smectite (montmorillonite) is preserved. The composition of terrigenous clay minerals remains unchanged at the top of the unit underlying the sill base.  相似文献   

7.
K-Ar ages of illite alteration associated with Middle Proterozoic Athabasca unconformity-type U deposits in Saskatchewan range from 414 to 1493 Ma. The K-Ar ages correlate with water contents and δD values such that illites with young K-Ar ages have δD values as low as −169 and water contents as high as 7.7 wt.% whereas illites with older ages have δD values near −70 and water contents near 4 wt.%. Water extracted at 400°C from illites with low δD values and high water contents has low δD and δ18O values similar to those of modern meteoric water suggesting that some of the illites associated with the original deposition of the ore underwent varying degrees of retrograde alteration. The alteration is initiated by hydration of sites in the interlayer region of the illite which results in the partial resetting of the K-Ar ages and introduction of excess structural water in the form of interlamellar water. The interlamellar water is enriched in 18O by about 7 per mil relative to the water that physically surrounded the clay particle. Further alteration decreases the δD value and increases the δ18O value of the illite by isotopic exchange between the mineral and the interlamellar water. Although the chemical compositions and XRD patterns of the altered illites indicate that no detectable smectite component is present in the samples, the isotopic results suggest that the altered illites may be an early precursor in the formation of mixed-layer illite/smectite by retrograde alteration of pure illite. The wide variation of δD values of chlorite and kaolinite from these U deposits is analogous to that of the illite suggesting that retrograde alteration of clays by meteoric water can be substantial. The general association of altered clays with areas containing the highest concentrations of U is probably related to localized permeability within the ore zone.  相似文献   

8.
Neutron powder diffraction measurements on lithium and cesium saturated montmorillonite samples before and after heat treatment at 300°C are studied, in order to undertake a complete refinement of crystal structure and unravel the migration mechanism for the interlayer cations of Li or Cs. Rietveld analysis of the corresponding diffraction patterns finds that montmorillonite crystallizes in the C2/m space group with unit cell dimensions consistent with the size of the specific interlayer cation. We show that thermal treatment affects the two types of samples in a different way. This is with respect to their unit cell dimensions and the migration of Li from the 2b to the 2c clay lattice site, in constrast to the Cs positioning which remains effectively unchanged.  相似文献   

9.
The smectite-to-chlorite conversion is investigated through long-duration experiments (up to 9 years) conducted at 300 °C. The starting products were the Wyoming bentonite MX80 (79 % smectite), metallic iron and magnetite in contact with a Na–Ca chloride solution. The predominant minerals in the run products were an iron-rich chlorite (chamosite like) and interstratified clays interpreted to be chlorite/smectite and/or corrensite/smectite, accompanied by euhedral crystals of quartz, albite and zeolite. The formation of pure corrensite was not observed in the long-duration experiments. The conversion of smectite into chlorite over time appears to take place in several steps and through several successive mechanisms: a solid-state transformation, significant dissolution of the smectite and direct precipitation from the solution, which is over-saturated with respect to chlorite, allowing the formation of a chamosite-like mineral. The reaction mechanisms are confirmed by X-ray patterns and data obtained on the experimental solutions (pH, contents of Si, Mg, Na and Ca). Because of the availability of some nutrients in the solution, total dissolution of the starting smectite does not lead to 100 % crystallization of chlorite but to a mixture of two dominant clays: chamosite and interstratified chlorite/smectite and/or corrensite/smectite poor in smectite. The role of Fe/(Fe + Mg) in the experimental medium is highlighted by chemical data obtained on newly formed clay particles alongside previously published data. The newly formed iron-rich chlorite has the same composition as that predicted by the geothermometer for diagenetic to low-grade metamorphic conditions, and the quartz + Fe-chlorite + albite experimental assemblage in the 9-year experiment is close to that fixed by water–rock equilibrium.  相似文献   

10.
 The smectite dehydration theory developed by Ransom and Helgeson was applied for simulation of land subsidence in the Yun-Lin coastal area, Taiwan. The volumetric reduction of smectite clay at equilibrium state was computed by assuming that the dehydration of interlayer water in smectite clay can be described with a regular solid solution reaction. By using the in situ stratigraphic data collected from the subsidence monitoring wells in the simulated area, the amounts of land subsidence caused by smectite dehydration in three scenarios with pressure variation were calculated. The results indicate that significant amounts of land subsidence can be attributed to smectite dehydration. This finding reveals that smectite dehydration is of importance for assessment and prediction of land subsidence. Additionally, the results also indicate the overburden weight has a larger effect on clay dehydration than the effective stress change resulting from over-pumping, although both of them induce relatively minor variations on land subsidence. Received: 23 February 2000 · Accepted: 23 March 2000  相似文献   

11.
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   

12.
The Oued Belif 48 and Koudiat El Halfa 5 borehole samples have been analysed in order to reveal the mineralogical composition of the Triassic successions and their burial history within the geological evolution of the Tethysian southern margin. Oued Belif 48 borehole belongs to Nefza district which is a part of the “Nappe zone” (Tellian unit, north-western Tunisia). Koudiat El Halfa 5 borehole crosses the Koudiat El Halfa diapir (north–west of the north–south axis, Central Atlas). In this paper, the burial degree of evaporitic Triassic samples was determined by the “illite crystallinity” index and by the evolution of the other phyllosilicates, essentially chlorite, talc and illite/chlorite and illite/smectite mixed layers. The studied samples of the two boreholes are characterized by the presence of abundant clay minerals. The <2-μm grain-size fraction of the samples is mostly composed of illite, chlorite and smectite and may contain a slight percentage of swelling layers (illite/smectite and illite/chlorite). The illite crystallinity value measured on ethylene glycol solvated oriented mounts of the Oued Belif 48 samples oscillates globally between 1 and 2.5 characterizing the epizonal zone with a range of 300–400 °C temperatures. The measures of Koudiat El Halfa 5 samples crystallinity index show a value ranging from 2 to 4, which indicates the anchizone and early epizone burial stage (temperatures around 200 °C). These data can be explained by Miocene magmatic activities characterizing the Triassic material of Nefza district and also by burial phenomena effects.  相似文献   

13.
The aim of the present work was to study the thermodynamic equilibria between water and a homo-ionic montmorillonite SWy-1 saturated by different cations. The choice of this smectite is justified by the large set of experimental data available from the literature for eight different interlayer cations: Na+, K+, Rb+, Cs+, Mg2+, Ca2+, Sr2+, and Ba2+. In particular, studies by [Cases et al., 1992], [Cases et al., 1997] and [Bérend et al., 1995] are providing heat of adsorption data, pairs of desorption-adsorption isotherms, and information about the partition of adsorption-desorption water molecules between external surfaces and internal spaces. By calculating the effective amount of hydration water as the difference between the so-called gravimetric water and the surface covering water, a thermodynamic model was then developed, based on the concept of Ransom and Helgeson (1994) considering an asymmetric subregular binary solid solution between a fully hydrated and a anhydrous smectite. A set of six thermodynamic parameters ( and four Margules parameters) was extracted by a least square method from measurements of enthalpies of adsorption and paired adsorption-desorption isotherms for each interlayer cation. These six initial parameters were then used to determine a complete set of standard thermodynamic hydration parameters (, heat capacity, molar volume, and number of interlayer H2O) and quantify, for each cation, the number of moles of hydration water molecules as a function of relative humidity and temperature. The validation of the standard state thermodynamic properties of hydration for each end member was carried out using three approaches: (1) a comparison with experimental isotherms obtained on hetero-ionic and homo-ionic SWy-1 smectite at different temperatures; (2) a comparison with the experimental integral enthalpy and entropy of hydration of the SWy-1 smectite; and (3) a comparison with experimental isotherms acquired on various smectites (Upton, MX80, Arizona) with different layer charges.Eventually, the present work demonstrates that, from a limited number of measurements, it is possible to provide the hydration thermodynamic parameters for hydrated smectites with different compositions and under different conditions of temperature and relative humidity, using the newly developed predictive model.  相似文献   

14.
The dehydration of a natural goethite to hematite is accompanied by a systematic hydrogen isotope fractionation. Closed system dehydration at, and below, 250°C results in a significantly greater degree of isotopic fractionation than does open system dehydration. This relationship is apparently reversed at 300°C. Both processes produce a progressive decrease in the DH ratio of the mineral hydrogen with increasing degree of dehydration. At temperatures of 160°C to 250°C the closed system mineralvapor fractionation factor is independent of temperature, while above 250°C, it varies strongly with temperature. The mineral-vapor fractionation factor associated with open system dehydration appears to be independent of temperature over the interval 160°C to 300°C. The closed system DH fractionation suggests that natural goethite undergoing dehydration in the presence of water can isotopically exchange with that water.CO2 loss from goethite during dehydration is correlated with the loss of H2O. The CO3 is thought to be present in carbonates which exist as impurities in the goethite. Loss of both H2O and CO2 appears to be diffusion-controlled.  相似文献   

15.
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16.
Aluminous, high-temperature clay minerals form from alteration of tholeiitic basaltic glass and calcic plagioclase during hydrothermal venting on the crest of the East Pacific Rise at 21°N. The clay alteration assemblages are layered crusts (up to 1 mm thick) completely replacing glass and calcic plagioclase adjacent to surfaces exposed to hydrothermal fluids. The interiors of the affected basalt samples have unaltered appearances and oxygen isotopic compositions just slightly heavier than that of MORB. The surficial alteration crusts are mixtures of beidellitic smectite (aluminous, dioctahedral), randomly interstratified mixed-layer Al-rich chlorite/smectite, minor chlorite, an x-ray amorphous aluminosilicate material, and possible minor serpentine (amesite). A δ18O value of +4.1 ± 0.2%. (SMOW) is determined for the beidellitic smectite. Assuming that this smectite equilibrated with hydrothermal fluid having an oxygen isotope value between that of seawater (0%.) and 350°C hydrothermal fluid from EPR, 21°N vents (+1.6%.), an equilibration temperature between 290°C and 360°C is calculated for the beidellitic smectite. This is substantially higher than any previously reported temperature for an oceanic smectite. The mixed-layer Al-rich chlorite/smectite has a δ18O value of +3.5%., which corresponds to equilibration at 295°–360°C. The aluminous composition of the alteration assemblage is uncommon for clay minerals produced by submarine hydrothermal basalt alteration. We suggest that this assemblage is largely the product of high-temperature interaction between basalt glass + plagioclase and Mg-poor, acidic hydrothermal fluids, with possibly some contribution of Mg from bottom seawater, and that the aluminous clays either incorporate Al3+ remobilized from basalt by lowpH hydrothermal fluids, or are residual phases remaining after intense alteration of basaltic glass + plagioclase.  相似文献   

17.
The Wadi Badaa (WB) Upper Miocene clays, Cairo-Suez district, Egypt, represent materials for the ceramic production. The clay raw materials are composed mainly of smectite and kaolinite with minor quartz, calcite, and rare feldspar. The plasticity indices vary between 24 and 30%, suggesting that these clays are plastic raw materials. IR bands of the investigated clays were observed at 3695, 3619, 1032, 916, 794, 690, 534, 466, and 423 cm?1 for kaolinite; at 3436, 1635, 916, and 466 cm?1 for smectite; and at 1179, 1104, 794, 690, and 466 cm?1 for quartz. The <2 μm particle sizes of samples are relatively abundant in clays (～33%), which is adequate for uses of the ceramic products because of containing fine particle sizes. The studied WB clays contain 7.95 and 12.35% moisture water and interlayer water, respectively, with a maximum drying shrinkage of 7.87% at room temperature; therefore, the WB clays could be used in the ceramic manufacture.  相似文献   

18.
We propose a solid-solution model for dioctahedral aluminous phyllosilicates accounting for the main compositional variations, including hydration, observed in natural smectites, interlayered illite/smectite, illites, and phengites from diagenetic to high-grade metamorphic conditions. The suggested formalism involves dehydrated micas and hydrated pyrophyllite-like thermodynamic end-members. With these end-members, the equilibrium conditions of quartz + water + K-bearing mica-like phyllosilicates of fixed 2:1 composition are represented by a line in P–T space along which the interlayer water content varies. The relevant thermodynamic properties required for the calculation of equilibrium conditions were derived using a set of 250 natural data of known maximal temperature and pressure conditions, which covers a range between 25°C and few MPa to 800°C and 5 GPa. The temperatures calculated at fixed pressure with our model are in fair agreement with those reported in the literature for the 250 natural data. At low temperature and pressure, the amount of interlayer water in K-deficient phengite and illite is predicted to reach 100% of the apparent vacancies, which is consistent with previous values reported in the literature. Although the amount of interlayer water is predicted to decrease with pressure and temperature, it is calculated to be significant in K-deficient phengite from LT–HP pelites metamorphosed at about 350°C, 10 kbar. The presence of molecular water in the interlayer site of such phengites has been confirmed by FTIR mapping. Its implications for P–T estimates are discussed.  相似文献   

19.
The Liverpool Plains in northern New South Wales contain some of the best agricultural land in Australia and are underlain by extensive smectite clay-dominated soils sourced from weathering the alkali basalts of the Liverpool Ranges. It had been thought that a relatively simple geological model explained the underlying Cenozoic sequence with salt-rich clays of the Narrabri Formation overlying sands and gravel aquifers comprising the Gunnedah Formation. Extensive groundwater modelling based upon this simple conceptualisation has been used in management plans proposed by the mining and agricultural industries. A 31.5 m core has been recovered using minimally disturbed triple-tube coring methods at Cattle Lane (Latitude –31.52° S, Longitude 150.47° E) to resolve uncertainty concerning the aquitard status of the upper layer. Recovered core has been examined and tested to determine grainsize, cation-exchange capacity, X-ray diffraction, X-ray fluorescence and microscopic examination of granular components. These measurements complement surface and borehole geophysical techniques, hydrogeological data and hydrochemical analysis of water samples recovered from a series of specially constructed piezometers adjacent to the cored hole. The sequence overlies a Late Cretaceous channel cut into Permian bedrock at 91 m depth with sands and clays below 31.5 m considered to represent various alluvial fill events mostly occurring since the Early Pliocene. Erosion of Late Eocene alkali basalts on the Liverpool Ranges, with the formation of smectite clays, pedogenic carbonates and with the addition of quartz from both eolian sources and locally derived from adjacent Triassic sandstone hills, provides the great majority of the sediment recovered from the cores. Late Pleistocene (114 ka) to Holocene ages were determined for the core from three optically stimulated luminescence (OSL) measurements on fine sands (13, 23 and 29 m BG). Detailed examination has failed to detect any evidence of a boundary between Narrabri and Gunnedah formations revealing rather a gradual change in dominance of clays and silts over sands and gravels embedded in a clay-rich matrix. This result challenges the conceptualisation used to conduct groundwater modelling on the Liverpool Plains.  相似文献   

20.
Lath-shaped and highly crystalline trioctahedral smectites were synthesized under hydrothermal conditions. The quenched glasses with stoichiometrically dehydrated Na-smectite compositions were treated at （a） 500℃ and 100 MPa for 1 and 11 days; and （b） 300℃ and 100 MPa for 7 days. The crystallinity and particle size of products were dependent on the chemical composition of the starting glass, synthetic temperature and duration of hydrothermal treatment. The high structural ordering and large dimensions of the products were confirmed from the sharpness of XRD peaks; and hydration behavior under controlled relative humidity. Transmission electron microscopy was also performed for the characterization of the particle size of product. Particle sizes vary from ca. 10 nm to a few pm by changing the chemical compositions of the starting materials. The product with the highest structural ordering and largest dimension was obtained from Nao.33（Mg1.83Al0.67）Si4O11 glass treated at 500℃ and 100 MPa for 1 day. The obtained results also confirmed the metastability and compositional dependency in the formation of highly crystalline trioctahedral smectite at hydrothermal conditions.  相似文献   

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