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1.
This paper presents mineralogical and geochemical data from several continental sequences located in Central (Ain Ghréwiss and Kébar) and Central-Southern Tunisia (Selja, Kef Schefeir, Shib, Oum El Kcheb and Haidoudi). These sequences vary in age from Late Palaeocene to Early Oligocene and contain considerable quantities of fibrous clays (up to 75% palygorskite and 90% sepiolite). These clays appear in assocation with carbonates (mainly dolomite), detrital aluminosilicates (illite, Al smectites, mixed-layers illite–smectite and kaolinite), quartz and lesser quantities of gypsum and halite. The textural characteristics observed by electron microscopy, the trace and rare earth elements contents and their distribution in the various mineral phases, together with the isotopic composition of dolomite and fibrous clays, provide good clues as to the genesis of the neoformed minerals. Thus, the sepiolite would have precipitated directly in lacustrine, playa-lake or sebka environments under alkaline conditions, high Si and Mg and low Al activity, and arid to semiarid climate. On the other hand, the palygorskite would have formed by transformation of already existing illite and/or smectite type aluminosilicates in solutions in equilibrium with isotopically heavier and, therefore, more evaporated solutions than the sepiolite.  相似文献   

2.
This study examines textural inhomogeneity and variable chemical composition of Upper Jurassic glaucony in relation to small‐scale synsedimentary and postsedimentary authigenic processes controlled by the palaeonvironmental and palaeogeographical context. Four glaucony types with complex textural and compositional features have been recognized in cores of the Georgiev Formation of the West Siberian Basin. Samples exclusively made of light green type 1 glaucony (K2O < 6·5%: the less mature type, richer in glauconite–smectite mixed layer) formed under dysoxic conditions in the deepest distal marine environments of the northern sectors of the West Siberian Basin. Dark green type 2 glaucony is the most mature (richest in glauconitic mica: K2O up to 8·5%), is sometimes associated with type 1 glaucony, and is typical of high bottom areas with a low sedimentation rate within the central sectors of the basin. Type 3 glaucony is formed by brown grains, poorer in K and Fe but richer in Al and Si than type 2 glaucony, and is only present in strongly condensed successions of the central‐eastern sectors of the West Siberian Basin. Type 4 glaucony is much richer in Fe than any other type, shows fresh yellowish green cores slightly less mature than type 2 glaucony, and brown rims and cracks with composition similar to that of type 3 grains; it was formed in western sectors of the West Siberian Basin, close to Urals. Weathering under a subtropical to temperate climate, and erosion of badly drained peneplaned lowland areas around the basin, provided Al‐rich terrigenous clays as substratum for glauconitization, which explains Al and Si enrichment in Siberian glaucony. Maturation from glauconite–smectite to glauconitic mica is monitored by a change from light to dark green colour related to decrease in Al, Si, Mg, Ca and Na, and to increase in K and Fe. Brown rims of type 4 glaucony, and brown type 3 grains formed after leaching of Fe and K from mature glauconite, with formation of clays and Fe oxyhydroxides as reaction products, as a result of free oxygen exposure related to a hydrodynamic regime and temporary sea‐level fall. Glauconitization stopped and diagenetic pyrite formed due to basin deepening and burial under black shales during the latest Jurassic–earliest Cretaceous transgression. This study demonstrates that, due to the complex nature of glaucony, the authigenesis of glauconitic minerals in the rock record cannot be correctly understood if the palaeoenvironmental context and the palaeogeographical context of glaucony‐bearing sediments are not considered.  相似文献   

3.
Experimental batch and miscible-flow cultures were studied in order to determine the mechanistic pathways of microbial Fe(III) respiration in ferruginous smectite clay, NAu-1. The primary purpose was to resolve if alteration of smectite and release of Fe precedes microbial respiration. Alteration of NAu-1, represented by the morphological and mineralogical changes, occurred regardless of the extent of microbial Fe(III) reduction in all of our experimental systems, including those that contained heat-killed bacteria and those in which O2, rather than Fe(III), was the primary terminal electron acceptor. The solid alteration products observed under transmission electron microscopy included poorly crystalline smectite with diffuse electron diffraction signals, discrete grains of Fe-free amorphous aluminosilicate with increased Al/Si ratio, Fe-rich grains, and amorphous Si globules in the immediate vicinity of bacterial cells and extracellular polymeric substances. In reducing systems, Fe was also found as siderite. The small amount of Fe partitioned to the aqueous phase was primarily in the form of dissolved Fe(III) species even in the systems in which Fe(III) was the primary terminal electron acceptor for microbial respiration. From these observations, we conclude that microbial respiration of Fe(III) in our laboratory systems proceeded through the following: (1) alteration of NAu-1 and concurrent release of Fe(III) from the octahedral sheets of NAu-1; and (2) subsequent microbial respiration of Fe(III).  相似文献   

4.
Apatites occurring in lateritic residues derived from high-grade metamorphic rocks from Sri Lanka are hydroxy-apatite as indicated by EPMA and XRD. Weathered phosphates and weathered crystalline products are composed of carbonate fluorapatite, crandallite, wardite, fluellite, kaolinite, goethite and gibbsite. EDAX, DTA and SIMS show the presence of amorphous materials, such as oxides of Fe, Al, Si, Al+Si, and S, on the surface of weathered phosphate. Using SEM, TEM, EDAX and electron diffraction techniques, the presence of these amorphous and crystalline materials with several transitions has been clearly identified in weathered phosphate. Recrystallization of phosphate occurred during weathering by dissolution, nucleation and precipitation. The lattice images of hydroxyapatite are gradually increased from 8.3-A basal spacings by weathering, and form mosaic bound fragments. Chondrite-, shale- and phosphorite concretion-normalized REE patterns of these apatites, known to have sedimentary origins, suggest enrichment and remobilisation during post-depositional reworking.  相似文献   

5.
Stoichiometry of smectite dissolution reaction   总被引：1，自引：0，他引：1  
The dissolution stoichiometry of smectite-rich bentonites SAz-1, STx-1 and SWy-1 was studied at 50°C and pH 2 and 3 using flow-through reactors. In addition to smectite, these samples contain considerable amounts of silica phases (quartz, cristobalite and/or amorphous silica). As a result, the molar Al/Si ratios of the bulk samples are significantly lower than those of the pure smectite.Smectite dissolution was highly incongruent during the first few hundred to few thousand hours of the experiments. Release rates of Si, Mg, Ca and Na underwent a distinct transition from an initial period of rapid release to significantly lower release rate at steady state. A reversed trend was observed for release of Al, which gradually increased from very low starting release rate to higher release rate at steady state. At steady state the ratio of released Al to released Si was found to be constant and independent of the experimental conditions. We suggest that this ratio represents the Al/Si ratio of the smectite itself, and it is not influenced by the presence of accessory phases in the sample.The rapid release of calcium, sodium and magnesium from the interlayer sites is explained by ion-exchange reactions, whereas the fast release of silicon is explained by dissolution of amorphous silica. We interpret the initial slow release of Al as the result of inhibition of smectite dissolution due to coating or cementation of the smectite aggregates by amorphous silica. As the silica is dissolved, the aggregates fall apart and more smectite surfaces are exposed, resulting in an increase in the smectite dissolution rate. Thereafter, the system approaches steady state, in which the major tetrahedral and octahedral cations of smectite are released congruently.  相似文献   

6.
Phyllosilicates occurring as replacements of olivine, clinopyroxene and interstitial materials and as veins or fracture-fillings in hydrothermally altered basalts from DSDP Hole 504B, Leg 83 have been studied using transmission and analytical electron microscopy. The parageneses of phyllosilicates generally change systematically with depth and with the degree of alteration, which in turn is related to permeability of basalts. Saponite and some mixed-layer chlorite/smectite are the dominant phyllosilicates at the top of the transition zone. Chlorite, corrensite, and mixed-layer chlorite/corrensite occur mainly in the lower transition zone and upper levels of the sheeted dike zone. Chlorite, talc, and mixed-layer talc/chlorite are the major phyllosilicates in the sheeted dike zone, although replacement of talc or ohvine by saponite is observed. The phyllosilicates consist of parallel or subparallel discrete packets of coherent layers with packet thicknesses generally ranging from< 100 Å to a few hundred Å. The packets of saponite layers are much smaller or less well defined than those of chlorite, corrensite and talc, indicating poorer crystal-linity of saponite. by contrast, chlorite and talc from the lower transition zone and the sheeted dike zone occur in packets up to thousands of Å thick. The Si/(Si+Al) ratio of these trioctahedral phyllosilicates increases and Fe/(Fe+Mg) decreases in the order chlorite, corrensite, saponite, and talc. These relations reflect optimal solid solution consistent with minimum misfit of articulated octahedral and tetrahedral sheets. Variations in composition of hydrothermal fluids and precursor minerals, especially in Si/(Si+Al) and Fe/(Fe+Mg) ratios, are thus important factors in controlling the parageneses of phyllosilicates. The phyllosilicates are generally well crystallized discrete phases, rather than mixed-layered phases, where they have been affected by relatively high fluid/rock ratios as in high-permeability basalts, in veins, or areas adjacent to veins. Intense alteration in basalts with high permeability (indicating high fluid/rock ratios) is characterized by pervasive albitization and zeolitization. Minimal alteration in the basalts without significant albitization and zeolitization is characterized by the occurrence of saponite±mixed-layer chlorite/smectite in the low-temperature alteration zone, and mixed-layer chlorite/corrensite or mixed-layer talc/chlorite in the high-temperature alteration zone. Textural non-equilibrium for phyllosilicates is represented by mixed layering and poorly defined packets of partially incoherent layers. The approach to textural equilibrium was controlled largely by the availability of fluid or permeability.Contribution No. 488 from the Mineralogical Laboratory, Department of Geological Sciences, The University of Michigan  相似文献   

7.
Upper Jurassic phosphate stromatolites of the Almola Sierra (Southern Spain) encrust macrofossils and hardgrounds, and form oncoids included within pelagic, condensed fossiliferous limestones. Their accretion was determined by bacterially mediated precipitation of phosphate, by the trapping and binding of fine siliciclastics and pelagic biomicrite and by the encrustation of benthonic foraminifera. Phosphorous, trace elements and rare-earth elements were concentrated from degraded organic matter and seawater by stromatolite-building communities, which mediated the formation of phosphate-rich and Fe-Al-Si-rich organic gels under oxic conditions, favouring the precipitation of amorphous mineral precursors (ACP and Fe-Al-Si oxyhydroxides). The observed Ce-enrichment for some stromatolites is explained by oxidative scavenging of Ce4+ from seawater by Fe—Mn oxyhydroxides. The bacterially mediated gels were able to migrate and fill the voids of the stromatolite structure, and later changed to carbonate-fluorapatite, haematite and poorly crystalline Fe-rich clays under postoxic conditions. Phosphatization of trapped carbonate particles also occurred. The phosphate stromatolites formed on a sediment-starved pelagic swell, during periods of no carbonate sedimentation and hardground development. Stromatolite lamination provides evidence for rhythmic alternation between bacterially mediated phosphogenesis, sedimentation and erosion, suggesting episodic changes in the sedimentary environment. Although some of the parameters that controlled phosphate precipitation associated with the stromatolites (local high organic productivity, sediment starvation, moderate depth of deposition and physicochemical conditions) were similar to those found in modern and ancient phosphogenic settings, the palaeogeographical framework and the intensity of sedimentary processes were different to those of the World's major phosphorite deposits.  相似文献   

8.
Systematic changes in mineralogy, enrichment and depletion of selected elements, and mineralogical speciation of selected elements in fly ash and bottom ash samples from the Lingan Power Plant were compared to run-of-mine and pulverized feed coal from the Sydney coalfield, Nova Scotia, eastern Canada. The analytical techniques used were an electron microprobe equipped with energy and wavelength X-ray dispersive spectrometers, X-ray diffraction, neutron activation, scanning electron microscopy with energy dispersive X-ray and incident light petrography. Three types of glasses (Fe/O-rich, Fe/Al/Si/O-rich and or Al/Si/O-rich) were identified in the combustion residues; they were formed as a result of the interaction of melted pyrite and clay minerals. Compared to the feed coal, most elements were enriched 10 to20 times in the fly ash. The concentration of the elements in both the fly ash and bottom ash are comparable to coal ash that is generated by the low temperature asher in the laboratory. Some chalcophile elements such as arsenic and lead occurred as a solid solution in pyrite in the feed coal and were concentrated in the float fraction (density: <2.81 g/cm3) of the fly ash with non-crystalline Fe-oxides. X-ray mapping of arsenic in the fly ash and bottom ash indicates that arsenic was evenly distributed as oxide within the Fe/O- and Fe/Al/Si/O-rich glass and crystalline phases in the fly ash, possibly in solid solution. Arsenic is associated with Fe/O and Fe/S crystalline phases in the bottom ash.  相似文献   

9.
Suspended matter (SM) from the Nyong basin (Cameroon, Africa), a tropical watershed, was collected by tangential flow ultrafiltration to separate particulate (>0.45 μm) and colloidal (<0.45 μm; >20 kDa) fractions. In this basin, two distinctive systems in a selected small catchment (Nsimi–Zoétélé) of the Nyong river basin have been considered: (i) colourless water (groundwater and spring) with a low suspended load (<3 mg/l) and a low total organic carbon content (TOC<1 mg/l) and (ii) coloured water (Mengong brook and Nyong river), which is organic rich (TOC>10 mg/l) and contains higher amounts of SM (10–20 mg/l) than the colourless water. Freeze-dried samples of SM have been analysed by X-ray diffraction (XRD), transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FTIR), electron paramagnetic resonance spectroscopy (EPR), and visible diffuse reflectance spectroscopy (DRS).

Colourless water mainly contains mineral phases, such as poorly ordered kaolinite, plus quartz and goethite in the particulate fraction, and euhedral kaolinite plus amorphous iron oxyhydroxides in the colloidal fraction. In contrast, the SM in coloured water is mainly organic in nature. The mineral phases in the particulate fraction are similar to those from clear water, but with additional phytoliths and diatom frustules composed of biogenic opal. In the colloidal fraction, complexation of Fe3+ and Mn2+ with organic matter is evidenced by EPR, together with significant occurrence of Fe oxyhydroxides associated with organic matter.

The sites of Al, Si, Fe, Mn in colloidal fractions derived from spectroscopic analyses are discussed with reference to chemical analyses performed by inductively coupled plasma mass spectrometry. Most of the observed solid phases or species correspond to those expected from published thermodynamic calculations for the same hydrosystem, except the colloidal iron oxyhydroxides in the coloured water. The presence of such iron phases is emphasised since they are expected to have large sorption capacities for numerous trace elements.

The crystal chemistry of SM is used to discuss the origin of the mineral particles transported from the soil to the main rivers in terms of mechanical and chemical erosion processes.  相似文献   


10.
Cretaceous phosphorites from the onshore of Tamil Nadu have been investigated for their origin and compared with those in the offshore. Cretaceous phosphorites occur as light brown to yellowish brown or white nodules in Karai Shale of the Uttatur Group in the onshore Cauvery basin. Nodules exhibit phosphatic nucleus encrusted by a chalky shell of carbonate. The nucleus of the nodules consists of light and dark coloured laminae, phosphate peloids/coated grains and detrital particles interspersed between the laminae. Scanning electron microscope (SEM) studies reveal trapping and binding activity of microbial filaments. A mat structure with linearly arranged microbial filaments and hollow, cell-based coccoid cyanobacterial mat are present. Nodules contain abundant carbonate fluorapatite, followed by minor calcite, quartz and feldspar. The P2O5 content of the phosphorites ranges from 18 to 26%. The CaO/P2O5, Sr and F contents are higher than that of pure carbonate fluorapatite. Concentrations of Si, Al, K, Fe, and Ti are low. We suggest that the nuclei of the nodules represent phosphate clasts related to phosphate stromatolites formed at intertidal conditions. At high energy levels the microbial mats were disintegrated into phosphate clasts, coated with carbonate and then reworked into Karai Shale. On the other hand, Quaternary phosphorites occur as irregular to rounded, grey coloured phosphate clasts at water depths between 180 and 320m on the continental shelf of Tamil Nadu. They exhibit grain-supported texture. Despite Quaternary in age, they also resemble phosphate stromatolites of intertidal origin and reworked as phosphate clasts onto the shelf margin depressions. Benthic microbial mats probably supplied high phosphorus to the sediments. Availability of excess phosphorus seems to be a pre-requisite for the formation of phosphate stromatolites.  相似文献   

11.
Batch and flow-through experiments were performed on quartz–feldspar granular aggregates at hydrothermal conditions (up to ≈150 °C, up to 5 MPa effective pressure, and near-neutral pH) for up to 141 days. The effect of dissolution–precipitation reactions on the surface morphology of the mineral grains was investigated. The starting materials as well as the solids and fluids resulting from the experiments were characterized using BET, energy dispersive X-ray spectroscopy, electron microprobe analysis, inductively coupled plasma-optical emission spectroscopy, scanning electron microscopy, transmission electron microscopy, X-ray powder diffraction, and X-ray fluorescence spectroscopy. The electrical conductivity of fluid samples was used as a proxy for the evolution of the fluid composition in the experiments. The chemical analyses of the fluids in combination with hydrogeochemical simulations with PHREEQC suggested the precipitation of Al–Si-bearing solid phases. Electron microscopy confirmed the formation of secondary amorphous Al–Si-bearing solid phases. The microscopic observations are consistent with a process of stoichiometric dissolution of the mineral grains, transport of dissolved ions in the fluid phase, and spatially coupled precipitation of sub-μm sized amorphous particles on mineral surfaces. These findings shed light onto early stages of diagenesis of quartz–feldspar sands and indicate that amorphous phases may be precursors for the formation of crystalline phases, for example, clay minerals.  相似文献   

12.
Hyperalkaline and saline radioactive waste fluids with elevated temperatures from S-SX high-level waste tank farm at Hanford, WA, USA accidentally leaked into sediments beneath the tanks, initiating a series of geochemical processes and reactions whose significance and extent was unknown. Among the most important processes was the dissolution of soil minerals and precipitation of stable secondary phases. The objective of this investigation was to study the release of Fe into the aqueous phase upon dissolution of Fe-bearing soil minerals, and the subsequent formation of Fe-rich precipitates. Batch reactors were used to conduct experiments at 50 °C using solutions similar in composition to the waste fluids. Results clearly showed that, similarly to Si and Al, Fe was released from the dissolution of soil minerals (most likely phyllosilicates such as biotite, smectite and chlorite). The extent of Fe release increased with base concentration and decreased with Al concentration in the contacting solution. The maximum apparent rate of Fe release (0.566 × 10−13 mol m−2 s−1) was measured in the treatment with no Al and a concentration of 4.32 mol L−1 NaOH in the contact solution. Results from electron microscopy indicated that while Si and Al precipitated together to form feldspathoids in the groups of cancrinite and/or sodalite, Fe precipitation followed a different pathway leading to the formation of hematite and goethite. The newly formed Fe oxy-hydroxides may increase the sorption capacity of the sediments, promote surface mediated reactions such as precipitation and heterogeneous redox reactions, and affect the phase distribution of contaminants and radionuclides.  相似文献   

13.
Fe-nodules occur within saprolites formed from weathering of granodioritic gneisses in the rain-shadow region of the Mysore Plateau adjacent to the Sahyadri Mountains in Southern India. These nodules and their host saprolites were studied for their geochemistry, including chemical speciation, to understand nodule formation and chemical redistribution processes during rock weathering. From their mode of occurrence, and mineralogical and geochemical data, we infer that the nodules originated by a two-stage process in which the initial extensive weathering of gneisses likely facilitated subsequent ferrolysis weathering and nodule formation. Nodules originated by precipitation of goethite, hematite and gibbsite along with several amorphous phases within the matrix of weathered gneisses. This is possible only under hydromorphic conditions, suggesting that parts of the plateau must have gone through a humid phase prior to the present aridity. In the saprolites, Al, Fe, and Ti become enriched because of the removal of Si, Ca, Na, and K. However within the nodule, Fe, Ti, Cr, and Ni are deposited after their chemical transport from the saprolite. Titanium, known for its immobile nature, was also mobilized and concentrated under the conditions of nodule formation. The most important elements in the nodule constitution are Fe, Al, Ti, and Mn, each having both crystalline and amorphous phases. Fe-Ti and Mn oxyhydroxides grain coatings in the saprolites and discrete amorphous Mn and Ti phases in the nodules seem to have scavenged trace elements from the weathering profile. REE were mobilized during weathering and nodule genesis in which Ce and Ti show a strong geochemical coherence. The enrichment of only HREE in saprolite, and both HREE and LREE with significant Ce in the nodule, indicate the control of evolving secondary minerals in the REE redistribution during rock weathering. Strong enrichment of Ce in the weathering profile and in nodules has important implications to the REE chemistry of river waters.  相似文献   

14.
The source material, precursor and formation processes of chlorite rims, and impact of pore-lining chlorite on reservoir quality of the Shiqianfeng sandstones, Dongpu Depression, Bohai Bay Basin, China, are studied using an integrated approach, including core observation, point-count analysis of thin-sections, scanning electron microscopy, electron microprobe analysis and cathode luminescence. The petrographic analysis shows that chlorite rims consist of grain-coating chlorite, poorly crystalline pore-lining chlorite and euhedral-crystallised pore-lining chlorite. The chemical composition shows that pore-lining chlorite is mainly Fe-rich with an average of 0.785 for Fe/(Fe+Mg) ratio. Petrographic analysis shows a large amount of volcanic dust (3.0～16.0 vol%, average of 7.93 vol%) in Shiqianfeng sandstones, which determines the formation of poorly crystalline pore-lining chlorite. Transformation of volcanic dust to smectite rims started with shallow burial depth at an early diagenetic stage, followed by in situ alteration of the smectite rims to poorly crystalline chlorite rims. Euhedral-crystallised chlorite mainly develops in sandstones with high porosity, high permeability and open flow systems. Pore-lining chlorite can inhibit quartz overgrowth but cannot effectively prevent pore-filling of authigenic quartz, carbonate and kaolinite cements, and therefore cannot prevent porosity destruction. However, the occurrence of pore-lining chlorite is a barometer of good reservoir quality and intense hydrodynamic conditions.  相似文献   

15.
Iron-rich smectite is commonly described in the diagenetic fraction of deep-sea sediment, as millimeter to centimeter aggregates dispersed in the sediment, or as a coating on sedimentary particles or nodules. This study examines several factors to elucidate formation mechanisms of a particular iron-rich smectite and its potential transformation to glauconite. The study combines a detailed mineralogical investigation on natural samples and a chemical modeling approach to assess mineralogical reactions and pathways.Transmission electron microscopy (TEM) observations and analytical electron microscopy (TEM-AEM) analyses were conducted on microtomed samples of millimeter- to centimeter-long green grains. These grains are widespread in pelagic calcareous sediment from the Costa Rica margin. They are composed of pyrites that are partially dissolved and are surrounded by amorphous or very poorly crystallized iron-rich particles. Iron-rich montmorillonite grows from an amorphous precursor and its formation requires the input of Si, O, Mg, K, Na and Ca; our results suggest that these inputs are supported by the dissolution of sedimentary phases such as volcanic glasses, siliceous fossils and silicates.Thermodynamic modeling of fluid-sediment interactions was conducted with the geochemical computer code PhreeqC, using mineralogical and pore fluid compositions from sediment samples and calculated estimates for thermodynamic constants of smectites that are not maintained by the computer code. Simulations confirm the possibility that the green grains are the product of pyrite alteration by seawater under oxidizing conditions. The extent of smectite production is controlled by the kinetics of pyrite dissolution and fluid migration. The absence of aluminum in the Costa Rica margin system explains the formation of an iron-rich montmorillonite instead of glauconite, whereas the presence of calcite that buffers the system explains the formation of an iron-rich montmorillonite instead of iron oxides.  相似文献   

16.
Laterite occurs extensively over the crystalline and sedimentary rocks in the midland and lowland areas of south Kerala, India. Two lateritization cycles are identified in this area. Large, good-quality kaolin deposits, composed mostly of kaolinite, are characteristic of the sedimentary sequence in south Kerala. These deposits were formed on deposition of the weathering materials of the khondalites towards the first cycle of lateritization. After deposition and uplift of the sedimentary rocks, another lateritization cycle affected these, as well as the khondalites during pre-Quaternary times with the formation of a planation surface at 25–125 m above sea level having thick laterite profiles. The laterite profiles over the kaolin deposits show higher concentration of Fe-oxides (mostly in the form of hematite) and titania, compared to their concentration in the kaolins. Higher contents of Cr and Ni are also characteristic of the laterite over kaolin deposits. Recrystallization of the kaolinite, appearance of Al, Fe and Si amorphous phases in the kaolin clays and partial removal of Fe and Ti from them are attributed to the second lateritization cycle.  相似文献   

17.
In order to evaluate the extent of a natural enrichment of Fe and Mn over the whole of the Hunchun Basin, the stability of Fe-Mn mineral phases, their status, the weathering rate of source materials, and soil characteristics were determined. A variety of samples were collected from sediments, soil profiles, and surface soils. In the solutions after a sequentially selective dissolution using sodium pyrophosphate (p), acid oxalate (o), and dithionite-citrate-bicarbonate (d), Si, Al and Fe were dominant in the d and p fractions, and Mn in the o and p fractions. The results showed that the existing phases and status of Fe and Mn were distinctly different, and that the abundance of amorphous Mn phases made thermodynamic calculation difficult. An application of these ferruginous weathering products was therefore made to understand basin development. The first terrace of the Hunchun River is more active than the second terrace, which can be inferred from it having a higher value in Fed/Fet. Amorphous Fe phases such as Fe(OH)3 and Fe3(OH)8 were controlling factors of Fe in the thermodynamic calculations. The transformation of the amorphous Fe phases to more stable phases was hindered by high contents of smectite and gibbsite, amorphous opaline produced from rice roots, and organic phosphate pesticides or fertilizers in soils. Source-rock deduction using water samples suggested granitic weathering. Precipitation around the Hunchun Basin is gradually becoming more acidic. Therefore, in the future it is inevitable that ecological and environmental problems related to the Fe phases mentioned above will occur in the drinking water supply for this area, especially in that of the first terrace.  相似文献   

18.
《Geochimica et cosmochimica acta》1999,63(19-20):3395-3406
Transmission electron microscopy (TEM), with energy dispersive X-ray (EDX) analysis and energy filtered transmission electron microscopy/electron energy loss spectroscopy (EFTEM/EELS), as well as powder X-ray diffraction (XRD) and scanning electron microscopy (SEM), have been used to study bed sediments from two acid mine drainage (AMD) sites in western Montana, USA. TEM and associated techniques, including sample preparation via epoxy impregnation and ultramicrotome sectioning, afford the opportunity to better interpret and understand complex water-rock interactions in these types of samples. For the sample taken from the first site (Mike Horse mine), ferrihydrite is the dominant phase, Si and Zn are the most abundant elements sorbed to ferrihydrite surfaces, and Pb is notably absent from ferrihydrite association. Three additional important metal-containing phases (gahnite, hydrohetaerolite, and plumbojarosite), that were not apparent in the powder XRD pattern because of their relatively low concentration, were identified in the TEM. The presence of these phases is important, because, for example, gahnite and plumbojarosite act as sinks for Zn and Pb, respectively. Therefore, the mobility of Pb from this part of the drainage system depends on the stability of plumbojarosite and the ability of ferrihydrite to sorb the released Pb. From thermodynamic data in the literature, we predict that Pb will be released by the dissolution of plumbojarosite above a pH of 4 to 5, but it will then be recaptured by ferrihydrite if the pH continues to rise to 5.5 and higher, irrespective of competition effects from other metals. Therefore, only a relatively narrow pH window exists in which Pb can escape this portion of the system as an aqueous species. For the sample taken from the other site included in this study (the Carbonate mine), jarosite and quartz are the dominant phases. Interestingly, however, the jarosites are both Pb-poor and Pb-enriched. In addition, TEM reveals the presence of microcrystalline hematite with Si, S, and P sorbed to its surfaces, a nearly pure amorphous Si, Al oxyhydroxide, and an amorphous silica phase containing minor amounts of Al, Ca, and Fe. Pb will probably be released from these mixed K-Pb jarosites above pH 4 to 5, but the Pb may be retarded by the strongly adsorbing microcrystalline hematite in this pH range. The sink for Al in this system is the amorphous Si, Al oxyhydroxide, not Al(OH)3 which is typically used in AMD modeling schemes.  相似文献   

19.
《Applied Geochemistry》1998,13(6):715-734
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20.
The impact particulate-phosphorus (particulate-P) has on eutrophication of aquatic systems that greatly depends on its composition. As a result, analysis methods for evaluating particulate-P speciation must be capable of identifying and/or quantifying the wide range of forms particulate-P can take. In the present study, we compare the particulate P speciation of the fine and colloidal fractions of riverbed sediment and suspended matter from two rivers in the Lake Geneva basin (French Alps) as determined with chemical extractions to results of a combined Transmission Electron Microscopy and Energy Dispersive Detection (TEM–EDS) analysis of the same samples. TEM–EDS provides semi-quantitative information about the distribution of P throughout the solid fraction of a sample and on the diversity of carrier phases, which are identified by their morphology and stochiometry. EDS-detectable quantities of phosphorus were found in 15–35% of the particles in the samples analyzed. As expected, particulate-P existed in a wide variety of forms, mostly associated with Al, Fe, Ca and Si. Some types of particles, often well-crystallized phosphate minerals, had high P contents (10–30%), but the dominant carrier phases of P were diffuse matrices of particles with low P contents (<5%). These matrices had a wide range of chemical compositions and included clay minerals, crystallized and amorphous phases of Fe, as well as intermediary components. Classical chemical extractions showed major differences in P content and speciation between the upstream and downstream sediment samples. The downstream samples showed higher frequencies of particles containing P, a larger diversity of carrier phases, a higher contribution of clays as carrier phases of P, and the presence of a new fraction with Al and Fe amorphous minerals. The processes that create and select carrier phases of particulate-P are part of the general dynamics of P within a watershed.  相似文献   

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