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1.
Redox processes of structural Fe in clay minerals play an important role in biogeochemical cycles and for the dynamics of contaminant transformation in soils and aquifers. Reactions of Fe(II)/Fe(III) in clay minerals depend on a variety of mineralogical and environmental factors, which make the assessment of Fe redox reactivity challenging. Here, we use middle and near infrared (IR) spectroscopy to identify reactive structural Fe(II) arrangements in four smectites that differ in total Fe content, octahedral cationic composition, location of the negative excess charge, and configuration of octahedral hydroxyl groups. Additionally, we investigated the mineral properties responsible for the reversibility of structural alterations during Fe reduction and re-oxidation. For Wyoming montmorillonite (SWy-2), a smectite of low structural Fe content (2.8 wt%), we identified octahedral AlFe(II)-OH as the only reactive Fe(II) species, while high structural Fe content (>12 wt%) was prerequisite for the formation of multiple Fe(II)-entities (dioctahedral AlFe(II)-OH, MgFe(II)-OH, Fe(II)Fe(II)-OH, and trioctahedral Fe(II)Fe(II)Fe(II)-OH) in iron-rich smectites Ölberg montmorillonite, and ferruginous smectite (SWa-1), as well as in synthetic nontronite. Depending on the overall cationic composition and the location of excess charge, different reactive Fe(II) species formed during Fe reduction in iron-rich smectites, including tetrahedral Fe(II) groups in synthetic nontronite. Trioctahedral Fe(II) domains were found in tetrahedrally charged ferruginous smectite and synthetic nontronite in their reduced state while these Fe(II) entities were absent in Ölberg montmorillonite, which exhibits an octahedral layer charge. Fe(III) reduction in iron-rich smectites was accompanied by intense dehydroxylation and structural rearrangements, which were only partially reversible through re-oxidation. Re-oxidation of Wyoming montmorillonite, in contrast, restored the original mineral structure. Fe(II) oxidation experiments with nitroaromatic compounds as reactive probes were used to link our spectroscopic evidence to the apparent reactivity of structural Fe(II) in a generalized kinetic model, which takes into account the presence of Fe(II) entities of distinctly different reactivity as well as the dynamics of Fe(II) rearrangements.  相似文献   

2.
Reactive surface area is one of the key parameters for studying the kinetics of mineral dissolution. The common practice in experimental kinetics is to normalize the dissolution rate to the surface area measured by the BET method. The relationship between BET surface area and the reactive surface area is not trivial in minerals such as smectites, which possess both internal and external surface areas, and in which the dissolution is controlled by the chemical attack on the edge surface. The present study examines two proxies for the reactive surface area of the Clay Mineral Society reference smectite SAz-1: BET surface area and the edge surface area measured using AFM.Since smectites are very microporous, their BET surface area is strongly influenced by the degassing procedure. It is demonstrated that outgassing the smectite powder at 135°C in a 15 mL min−1 N2 gas flow for at least 24 hours minimizes contribution from micropores to less than 11% of the BET surface area.Following dissolution experiments in solutions with a low electrolyte concentration, the BET surface area increased from 34 ± 2 m2 g−1 in raw SAz-1 to 127 ± 13 m2 g−1 in SAz-1 sample recovered from dissolution experiments. This increase in BET surface area is explained by a decrease in the average size of the smectite aggregates, and by an increase in microporosity due to the depletion in the major interlayer cation, i.e., Ca2+. As the BET surface area of the raw smectite sample includes considerably less microporosity compared to the BET surface area of the smectite recovered from dissolution experiments, the former is a better approximation of the external surface area of the dried sample powder.AFM measurements show that there is no correlation between the specific external surface area of the sample and its specific edge surface area. This observation is explained by the platy morphology of the smectite particle in which the specific external surface area depends linearly on the height reciprocal, whereas the specific edge surface area is independent of the particles height and depends linearly on the sum of the reciprocals of the length of the axes. Therefore, there is no reason to expect a correlation between the BET and the edge surface area. Our results show that the edge surface area (4.9 ± 0.7 m2 g−1) of the smectite particles cannot be predicted based on its external surface area (136 ± 20 m2 g−1). Therefore, the BET surface area cannot serve as a proxy for the reactive surface area. We suggest using AFM measurements of the specific edge surface area as an alternative proxy for the reactive surface area of smectite.  相似文献   

3.
99Technetium (99Tc) is a fission product of uranium-235 and plutonium-239 and poses a high environmental hazard due to its long half-life (t1/2 = 2.13 × 105 y), abundance in nuclear wastes, and environmental mobility under oxidizing conditions [i.e., Tc(VII)]. Under reducing conditions, Tc(VII) can be reduced to insoluble Tc(IV). Ferrous iron, either in aqueous form (Fe2+) or in mineral form [Fe(II)], has been used to reduce Tc(VII) to Tc(IV). However, the reactivity of Fe(II) from clay minerals, other than nontronite, toward immobilization of Tc(VII) and its role in retention of reduced Tc(IV) has not been investigated. In this study the reactivity of a suite of clay minerals toward Tc(VII) reduction and immobilization was evaluated. The clay minerals chosen for this study included five members in the smectite-illite (S-I) series, (montmorillonite, nontronite, rectorite, mixed layered I-S, and illite), chlorite, and palygorskite. Surface Fe-oxides were removed from these minerals with a modified dithionite-citrate-bicarbonate (DCB) procedure. The total structural Fe content of these clay minerals, after surface Fe-oxide removal, ranged from 0.7% to 30.4% by weight, and the structural Fe(III)/Fe(total) ratio ranged from 45% to 98%. X-ray diffraction (XRD) and Mössbauer spectroscopy results showed that after Fe oxide removal the clay minerals were free of Fe-oxides. Scanning electron microscopy (SEM) revealed that little dissolution occurred during the DCB treatment. Bioreduction experiments were performed in bicarbonate buffer (pH-7) with structural Fe(III) in the clay minerals as the sole electron acceptor, lactate as the sole electron donor, and Shewanella putrefaciens CN32 cells as a mediator. In select tubes, anthraquinone-2,6-disulfate (AQDS) was added as electron shuttle to facilitate electron transfer. In the S-I series, smectite (montmorillonite) was the most reducible (18% and 41% without and with AQDS, respectively) and illite the least (1% for both without and with AQDS). The extent and initial rate of bioreduction were positively correlated with the percent smectite in the S-I series (i.e., layer expandability). Fe(II) in the bioreduced clay minerals subsequently was used to reduce Tc(VII) to Tc(IV) in PIPES buffer. Similar to the trend of bioreduction, in the S-I series, reduced NAu-2 showed the highest reactivity toward Tc(VII), and reduced illite exhibited the least. The initial rate of Tc(VII) reduction, after normalization to clay and Fe(II) concentrations, was positively correlated with the percent smectite in the S-I series. Fe(II) in chlorite and palygorskite was also reactive toward Tc(VII) reduction. These data demonstrate that crystal chemical parameters (layer expandability, Fe and Fe(II) contents, and surface area, etc.) play important roles in controlling the extent and rate of bioreduction and the reactivity toward Tc(VII) reduction. Reduced Tc(IV) resides within clay mineral matrix, and this association could minimize any potential of reoxidation over long term.  相似文献   

4.
To explore the effects of layer-charge distribution on the thermodynamic and microscopic properties of Cs-smectites, classical molecular dynamic simulations are performed to derive the swelling curves, distributions and mobility of interlayer species, and Cs binding structures. Three representative smectites with distinct layer-charge distributions are used as model clay frameworks and interlayer water content is set within a wide range from 0 to 380 mgwater/gclay. All the three smectites swell in a similar way, presenting the characteristic swelling plateaus and similar trends of swelling energetic profiles. The full-monolayer hydrate, corresponding to the global minima of the immersion energy, is the most stable hydrated state of Cs-smectites. The calculated diffusion coefficients of interlayer species disclose the confining effects in all smectites: both water molecules and ions diffuse slower than corresponding bulk cases and they are much more mobile in the direction parallel to the clay surfaces than perpendicular to them. The formed inner-sphere complex structures are very similar in different smectites: ions bind on the H-sites or T-sites and water molecules form cage-like caps covering the ions. Layer-charge distribution is found to have significant influences on the mobility of interlayer species and preference of ion binding sites. A general sequence is proposed to elucidate the preferences of various hexagonal sites (H-sites) and triangular sites (T-sites), that is, tetrahedrally substituted H-sites > nonsubstituted H-sites > tetrahedrally substituted T-sites > nonsubstituted T-sites, but the influence of octahedral substitutions on the preference of the neighboring sites is not obvious. Analysis of mobility indicates that H-sites are more stable Cs-fixation positions than T-sites and smectite with higher fraction of octahedral charges seems to be the most effective barrier material no matter how water content varies although all smectites can immobilize Cs ions in relatively dry conditions. These findings will not only facilitate basic research in geochemistry and material sciences, but also promote the barrier material designing.  相似文献   

5.
Adsorption isotherms and UV-visible and Mossbauer spectroscopic data point to specific interactions between flavomononucleotide (FMN) and Fe(3+)-smectite. The maximum amount of FMN adsorption was 0.3 mmole/g of Fe(3+)-smectite giving a 1:1 molar proportion of Fe3+ and FMN. The results suggest a Fe(3+)-FMN complex residing at the smectite surface. Other homoionic smectites (Cu2+, Zn2+, and Ca2+) exhibited lower levels of adsorption and less apparent specific interaction.  相似文献   

6.
Abstract In well NJ-15 of the Nesjavellir geothermal field, Iceland, the transition of discrete smectite into discrete chlorite has been studied from drill cuttings recovered at depths of less than 1714 m and over a continuous range of temperatures between 60 and 300° C. At temperatures below 180° C, the clay fractions contain mixtures of di- and trioctahedral smectites, whose layer charge increases with depth. Between 200 and 240° C, discrete smectites have transformed into smectite-rich, randomly interstratified chlorite and smecite ( R 0 C/S). Because the abundance of chlorite interlayers in this C/S is generally <20%, its presence can be detected only by electron microprobe techniques and not by X-ray diffraction. Between 245 and 265° C, both regularly ( R 1) and randomly interstratified C/S are the predominant layer silicates. Discrete chlorite first appears at approximately 270° C and coexists with minor amounts of R 0 C/S at higher temperatures.
R 0 and R 1 C/S form a nearly complete compositional series between trioctahedral saponite and discrete chlorite end-members. The interlayer cation and Si content of smectites and C/S decrease with increasing temperature. The Mg/(Mg + Fe) content of smectite, C/S, and chlorite is unrelated to temperature. The percentage of chlorite in C/S, as determined by electron microprobe analyses, increases continuously with increasing temperature, except for occurrences of smectite-rich C/S in fresh basaltic dykes which have not thermally equilibrated with the higher grade country rocks.  相似文献   

7.
The Morrón de Mateo bentonite deposit is being studied as a natural analogue of the thermal and geochemical effects on a bentonite barrier in a deep geological repository of high level radioactive wastes. This bentonite deposit and its host rocks were intruded by a rhyodacitic volcanic dome that induced a hydrothermal metasomatic process affecting the biocalcarenite beds close to the dome. In this work, the mineralogical and chemical features of the clay minerals of the hydrothermally altered pyroclastic (white tuffs) and epiclastic rocks (mass flow), located in the NE sector of the Morrón de Mateo deposit are described. White tuffs have a high content of phyllosilicates, mainly composed of dioctahedral smectites, while mass flow have a higher proportion of inherited minerals, the neoformed phyllosilicates are dioctahedral smectites and an interlayer chlorite/smectite mineral of corrensite type. The chemical composition of smectites reflects the different nature of the parent rocks, in such a way that smectites from white tuffs have a quite homogeneous chemical composition and their structural formulae correspond to montmorillonite type, while smectites from mass flow show more chemical variability, higher Fe and Mg contents and a mean structural formulae corresponding to Fe-Mg-rich beidellite and/or to an intermediate smectite member between beidellite and saponite. In addition, chemical composition and textural features of corrensite-like clay minerals in relation to Fe-Mg-rich smectites in the samples have also been studied, suggesting that the former seems to be formed from Fe-Mg-rich smectites. The presence of corrensite in the epiclastic rocks suggests that in the Morrón de Mateo area a hydrothermal alteration process occurred after bentonite formation, which transformed Fe-Mg-rich smectites into corrensite. This transformation was probably favoured by the intrusion of the Morrón de Mateo volcanic dome, which produced a temperature increase in the geological media and a supply of Fe-Mg-rich solutions. These physicochemical conditions were also responsible for the metasomatic transformations observed in the biocalcarenite beds located on the top of the bentonite deposit. All these data suggest that the Morrón de Mateo natural system could be a good natural analogue of both thermal and chemical effects on a bentonite barrier related to the radioactive decay of fission products and the interaction between the corrosion products of steel over-packs and the bentonite. These circumstances would favour the transformation of the candidate Al-rich smectites into Fe-Mg-rich smectites and corrensite, as steps prior to formation of chlorite. In this case, all the physicochemical and mechanical properties of Al-rich smectites would disappear and the clayey barrier would fail.  相似文献   

8.
 Four smectites with different total Fe contents (two nontronites, one ferruginous smectite, and one montmorillonite) were reduced to obtain a range of Fe(II)/Fe(III) ratios and their magnetic properties measured with a SQUID (superconducting quantum interference device) as a function of applied magnetic field strength at 5 K and as a function of temperature in a field of 0.1 T. The unaltered nontronite and ferruginous smectite specimens showed antiferromagnetic coupling, whereas the coupling in the reduced samples was ferromagnetic; the paramagnetic Curie temperature increased with increasing Fe(II) content. Data collected after cooling samples in both the presence and absence of an external magnetic field of 0.1 T showed that at low temperatures the reduced (ferromagnetic) nontronite and ferruginous smectite samples exhibit a memory effect of previous magnetic field exposure consistent with superparamagnetic or spin glass behavior. The superparamagnetic/ferromagnetic transition temperature, T f , increased linearly with increasing Fe(II) content for each of the nontronites, but the relationship between T f and Fe(II) content differed for different clays, thus demonstrating that T f is sensitive to isomorphous substitutions in the clay structure. The montmorillonite was paramagnetic in both oxidized and reduced forms. Received: 23 March 1999 / Revised, accepted: 27 August 1999  相似文献   

9.
Iheya‐North‐Knoll is one of the small knolls covered with thick sediments in the Okinawa Trough back‐arc basin. At the east slope of Iheya‐North‐Knoll, nine hydrothermal vents with sulfide mounds are present. The Integrated Ocean Drilling Program (IODP) Expedition 331 studied Iheya‐North‐Knoll in September 2010. The expedition provided us with the opportunity to study clay minerals in deep sediments in Iheya‐North‐Knoll. To reveal characteristics of clay minerals in the deep sediments, samples from the drilling cores at three sites close to the most active hydrothermal vent were analyzed by X‐ray diffraction, scanning electron microscope and transmission electron microscope. The sediments are classified into Layer 0 (shallow), Layer 1 (deep), Layer 2 (deeper) and Layer 3 (deepest) on the basis of the assemblage of clay minerals. Layer 0 contains no clay minerals. Layer 1 contains smectite, kaolinite and illite/smectite mixed‐layer mineral. Layer 2 contains chlorite, corrensite and chlorite/smectite mixed‐layer mineral. Layer 3 is grouped into three sub‐layers, 3A, 3B and 3C; Sub‐layer 3A contains chlorite and illite/smectite mixed‐layer mineral, sub‐layer 3B contains chlorite/smectite and illite/smectite mixed‐layer minerals, and sub‐layer 3C contains chlorite and illite. Large amounts of di‐octahedral clay minerals such as smectite, kaolinite, illite and illite/smectite mixed‐layer mineral are found in Iheya‐North‐Knoll, which is rarely observed in hydrothermal fields in mid‐ocean ridges. Tri‐octahedral clay minerals such as chlorite, corrensite and chlorite/smectite mixed‐layer mineral in Iheya‐North‐Knoll have low Fe/(Fe + Mg) ratios compared with those in mid‐ocean ridges. In conclusion, the characteristics of clay minerals in Iheya‐North‐Knoll differ from those in mid‐ocean ridges; di‐octahedral clay minerals and Fe‐poor tri‐octahedral clay minerals occur in Iheya‐North‐Knoll but not in mid‐ocean ridges.  相似文献   

10.
Results of the mineral and chemical study of surface-altered hyaloclastites from the Theistareykir and Nämafjall geothermal zones, the North Iceland rift, are considered. The paper scrutinizes the composition of hydrothermally altered rocks mainly consisting of clay minerals related to the transformation of bedrock hyaloclastites. The clay minerals also make up slope talus or proluvial deltas around highlands. The major clay minerals in areas of the present-day fumarole activity are kaolinite and smectite, while the redeposited talus-proluvial sediments are mainly composed of smectites. The studied rocks contain framboids, globules, rods, and other structures with morphology and size similar to those of mineralized bacteria. The local concentration of Ag in proluvial deposits is attributed to the intense bacterial activity. It is supposed that elevated contents of some trace elements could be related to an intense microbiotic influence.  相似文献   

11.
Sediment samples from the Mid-Atlantic Reykjanes Ridge (59°N) were taken to get information about sediment genesis and to identify different sources during the late Quaternary. Samples were investigated by X-ray diffraction and grain-size analyses. The clay mineral assemblages in sediments of the Reykjanes Ridge reflect paleoceanographic changes during the late Quaternary. Holocene sediments are characterized by high contents of smectite, mainly of less developed crystallinity. In the spatial distribution of clay minerals high smectite concentrations on the eastern flank and slightly decreasing concentrations on the western flank of the Reykjanes Ridge indicate the action of bottom-water transport. The smectite originates mainly from the volcanogenous Icelandic shelf and reflects the influence of Iceland-Scotland Overflow Water (ISOW). Stratigraphic variability in the clay mineral composition reflects predominantly the influence of different sources, resulting from oceanographic and glacial transport processes. During glacial time sediment transport is due mainly to input by icebergs. Increasing amounts of illite, chlorite, and kaolinite characterize ice-rafted sediments of the “Heinrich layers”. In these sediments smectite crystallinity is well developed. In contrast, several other ice-rafted layers contain smectite with low crystallographic order, similar to smectites of Holocene age. The icelandic source was proved by distinct amounts of basaltic glass in the coarse-grained sediment. At approximately 55 ka increasing amounts of chlorite and kaolinite suggest an enhanced influx of warm North Atlantic surface waters. This hypothesis is supported by a high carbonate shell production at this time. Relative low concentrations and the well-developed crystallinity of smectite minerals characterize the Last Glacial Maximum (LGM; 18–16 ka), indicating a reduced supply of fine icelandic material. Shortly after the LGM, at the beginning of termination IA, a distinct increase in fine-grained quartz (<2μm) and smectite are visible, which are proposed to reflect a supply of fine-grained ice-rafted material. At 13 ka linear increasing smectite concentrations of lower crystallographic order indicate increasing supply of fine-grained material from Iceland, linked to reinitiation of bottom currents of the ISOW. Full reinitiation is indicated at around 10 ka, where a strong increase in smectite of low crystallographic order is detected.  相似文献   

12.
The aim of this study is to characterize the pedogenic clay minerals by using simple approach: mixing mineralogical and geochemical findings.The fine clay fractions (< 0.1 μm) of a Vertic Cambisol profile were studied by means of X-ray diffraction (XRD), infrared spectroscopy (FTIR) and cation exchange capacity (CEC).Qualitative and quantitative mineralogical compositions of the clay mixture were determined.Moreover, chemical equilibria and thermodynamic stabilities of minerals (calcite, gypsum, kaolinite, smectites and illites) were studied using results of ionic activities obtained from total concentration of various aqueous species in water extracts from soil-saturated pastes.XRD analysis shows a good homogeneity in the mineralogical composition of the soil material, with depth of soil profiles. The identified clay minerals are mainly illite–smectite mixed layers (I/S) and kaolinite. The chemical analysis of saturated paste extracts with clay minerals shows a slight undersaturation of the illitic phase while smectites and also calcite and gypsum reach the thermodynamic equilibrium along the soil profile.  相似文献   

13.
Sorption of the trihydroxamate siderophores desferrioxamine-B and -D (DFOB and DFOD, respectively) and of the monohydroxamate ligand acetohydroxamic acid (aHA) to smectite were examined in batch sorption studies (pH 5.5, 0.1 M ionic strength) coupled with X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. Both DFOB and DFOD, which have similar molecular structures but different charge properties (cationic versus neutral, respectively) showed a high affinity for smectite. In contrast, the smaller aHA molecule did not sorb appreciably. XRD analysis indicated that DFOB and DFOD each absorbed in the interlamellar region of the clay to give d-spacings of 13.4-13.7 Å at equilibrium solution concentrations <250 μM. FTIR spectra of sorbed DFOB and DFOD indicated that the conformation of each species was distinct from its conformation in the crystalline or dissolved states. At elevated initial solution concentrations of 500-1500 μM, DFOB formed a bilayer in the clay interlayer. Changes in the FTIR spectra of the DFOB-loaded clay samples at these higher surface loadings were consistent with the presence of a metal-siderophore complex in the interlayer. DFOB and DFOD both enhanced Fe and Al release from smectite, but aHA did not. Possible dissolution mechanisms are discussed in light of the FTIR and batch dissolution results.  相似文献   

14.
The fraction of swelling-type clay minerals (smectites) is a first measure to estimate the swelling potential of natural rocks. This swelling potential is only activated if water can be incorporated in the sheet silicates. The samples studied in this work are volcanic rocks from the Southern Andes. According to the petrographic and mineralogical studies, the rocks are characterized as vulcanite with high content of smectite. Undisturbed samples showed minor swelling behaviour in conventional swelling tests, although X-ray diffraction and differential thermal analysis revealed swelling clay contents of more than 70 % in some samples. Powder swelling tests were performed on ground and recompacted rock samples. The results of these tests show a better agreement with those expected according to the mineralogical composition of the samples. The reason for the non-activation of the swelling potential in undisturbed samples was suspected to be the influence of the iron-oxide/hydroxide content, which was on average around 11 %. Scanning electron microscope images showed that the edge terminations of the clay particles are coated with hematite. The hydrophobic properties of hematite impede the access of water between the interlayers of the clay minerals and, in addition, hematite cementation prevents the expansion. In a further series of swelling tests water was replaced by a reducing solution (0.1 molar hydroxylammonium chloride) which removes the Fe-oxide coating. It can be shown that thus the swelling potential of the clay minerals in such undisturbed rocks can be activated.  相似文献   

15.
Smectite suspensions, at low solids contents, are known to be naturally high in volume with diverse structural properties. The changing structural properties of smectite aqueous suspensions in the absence and presence of calcium ions were investigated using an acoustosizer and an advanced cryo-SEM technique to further understand and thereby control their environmental impact.In the absence of Ca(II) ions, smectite particles are present as a colloidally stable sol due to electrical double layer repulsion of the negatively charged platelets. The smectite network is observed to be extended throughout the suspension via clay platelets networking with an edge–edge (EE) orientation due to high basal surface repulsion. After the initial addition of Ca(II) ions, the smectite negative zeta potential reduces and the smectite platelets coagulate forming 2 µm aggregates. The platelets are randomly orientated, lettuce-like, coagulated aggregates with a high presence of both edge–edge (EE) and edge–face (EF) orientations. After equilibration, the smectite platelets forming an orientated honeycomb cellular structure comprised of face–face (FF) multiply sheet aggregates. The voids in the cellular structure are larger than prior to Ca(II) addition, measured at 2–8 µm.The changing structural properties of a smectite suspension in the absence and presence of Ca(II) greatly influence smectite stability and in turn, mineral processing and/or environmental management. Adequate time is required to allow suppression of the initial swelling of the smectite, full Ca(II) exchange and platelet aggregation.  相似文献   

16.
Iron-bearing clay minerals are ubiquitous in the environment and have been shown to play important roles in several biogeochemical processes. Previous efforts to characterize the Fe2+–Fe3+ redox couple in clay minerals using electrochemical techniques have been limited by experimental difficulties due to inadequate reactivity between clay minerals and electrodes. The current work overcomes this limitation by utilizing organic electron transfer mediators that rapidly transfer electrons with both the Fe-bearing clay minerals and electrodes. Here, an Fe-rich source clay mineral (ferruginous smectite, SWa-1) is examined with respect to what fraction of structural Fe participates in oxidation/reduction reactions and the relationship between bulk Fe2+/Fe3+ ratios to the reduction potential (Eh).  相似文献   

17.
Fine-grained fluvial residual channel infillings are likely to reflect systematic compositional changes in response to climate change, owing to changing weathering and geomorphological conditions in the upstream drainage basin. Our research focuses on the bulk sediment and clay geochemistry, laser granulometry and clay mineralogy of Late-glacial and Early Holocene River Meuse (Maas) unexposed residual channel infillings in northern Limburg (The Netherlands). We demonstrate that residual channel infillings register a systematic bulk and clay compositional change related to climate change on a 1–10 k-yr time-scale. Late-glacial and Holocene climatic amelioration stabilised the landscape and facilitated prolonged and intense chemical weathering of phyllosilicates and clay minerals due to soil formation. Clay translocation and subsequent erosion of topsoils on Palaeozoic bedrock and loess deposits increased the supply of smectite and vermiculite within River Meuse sediments. Smectite plus vermiculite contents rose from 30–40% in the Pleniglacial to 60% in the Late Allerød and to 70–80% in the Holocene. Younger Dryas cooling and landscape instability caused almost immediate return to low smectite and vermiculite contents. Following an Early Holocene rise, within about 5000 yr, a steady state supply is reached before 5 ka (Mid-Holocene). Holocene sediments therefore contain higher amounts of clay that are richer in high-Al, low-K and low-Mg vermiculites and smectites compared with Late (Pleni-)glacial sediments. The importance of clay mineral provenance and loess admixture in the River Meuse fluvial sediments is discussed. © 1998 John Wiley & Sons, Ltd.  相似文献   

18.
Ordered illite/smectite is the most abundant and widespread product of argillic alteration associated with the Oligocene, epithermal, Ag-Pb-Zn-Cu-Au Amethyst vein system, southwest Colorado. Hydrothermal illite/smectites exhibit all Reichweite from 1 to 3 and span the composition range from about 25% to about 3% illite.— The composition and Reichweite of illite/smectite vary smoothly with distance from the Amethyst vein. With increasing distance from the vein, percent illite and the Reichweite decrease. When composition-temperature relationships of illite/smectite from modern geothermal systems are applied to the fossil Amethyst system, isotherms describing the thermal regime at the time of argillization can be estimated. Temperatures near 240° C appear to have existed near the Amethyst vein; these temperatures agree with homogenization temperatures obtained from fluid inclusions in vein minerals. The most distal illite/smectites, sampled about 260 m from the vein, indicate temperatures near 110° C. Estimated thermal gradients are on the order of 0.4 to 1° C per meter. — Although illite/smectite composition and structure vary systematically with distance from the Amethyst vein, there are no systematic trends associated with the numerous, smaller veins and veinlets in the hanging wall of the system. This indicates that temperatures of both wallrock and the fluids in all but the major Amethyst vein were nearly the same during clay formation. Apparently, the hydrothermal system had reached a fairly steady, mature, thermal state at the time of argillization.  相似文献   

19.
Clay mineralogy and major-element geochemistry of 35 surface sediment samples collected in 21 major to moderate rivers of Luzon, Philippines are used to evaluate the present chemical weathering process. The clay mineral assemblage consists mainly of smectite (average 86%) with minor kaolinite (9%) and chlorite (5%) and very scarce illite (1%), and does not show strong island-wide differences. The major element results of both bulk and clay-fraction sediments indicate that the formation of clay minerals is accompanied by leaching of Ca and Na first and of Fe and Mn thereafter during the chemical weathering process. A low-moderate chemical weathering degree of bulk sediments and a moderate-intensive degree of clay-fraction sediments are obtained in Luzon rivers based on proxies of chemical index of alteration (CIA) and smectite crystallinity. It is suggested that the majority of andesitic–basaltic volcanic and sedimentary rocks along with the tectonically active geological setting and sub-tropical East Asian monsoon climate are responsible for the predominance of smectite in the clay mineral assemblage.  相似文献   

20.
Integrated geological and geophysical investigation of bottom sediments in the Medvezhii Island region, southwestern margin of the Barents Sea, has made it possible to characterize sediments of diverse types related to the action of hydrocarbon fluids, hemipelagic sedimentation, slope phenomena, and combined influence of all these factors. Relatively homogeneous (in terms of mechanical composition) sediments are subdivided into several lithogenetic types based on the grain size distribution. Relationships of clay minerals, as well as their morphological and structural peculiarities, are described for each type. It is demonstrated that sediments formed under the substantial influence of hydrocarbon fluid fluxes are characterized by a high (relative to hemipelagic sediments) content of smectites and mixed-layer clay minerals of the illite–smectite series. It is assumed that these minerals are authigenic formations in mud volcanic rocks and diapir material. Based on the comparison of clay minerals contents primary source of the material for redeposited sediments has been reconstructed.  相似文献   

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