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1.
Goethite(α-FeOOH), an abundant and highly reactive iron oxyhydroxide mineral, has been the subject of numerous studies of environmental interface reactivity. However, such studies have been hampered by the lack of experimental constraints on aqueous interface structure, and especially of the surface water molecular arrangements. Structural information of this type is crucial because reactivity is dictated by the nature of the surface functional groups and the structure or distribution of water and electrolyte at the solid-solution interface. In this study we have investigated the goethite (1 0 0) surface using surface diffraction techniques, and have determined the relaxed surface structure, the surface functional groups, and the three dimensional nature of two distinct sorbed water layers. The crystal truncation rod (CTR) results show that the interface structure consists of a double hydroxyl, double water terminated interface with significant atom relaxations. Further, the double hydroxyl terminated surface dominates with an 89% contribution having a chiral subdomain structure on the (1 0 0) cleavage faces. The proposed interface stoichiometry is ((H2O)(H2O)OH2OHFeOOFeR) with two types of terminal hydroxyls; a bidentate (B-type) hydroxo group and a monodentate (A-type) aquo group. Using the bond-valence approach the protonation states of the terminal hydroxyls are predicted to be OH type (bidentate hydroxyl with oxygen coupled to two Fe3+ ions) and OH2 type (monodentate hydroxyl with oxygen tied to only one Fe3+). A double layer three dimensional ordered water structure at the interface was determined from refinement of fits to the experimental data. Application of bond-valence constraints to the terminal hydroxyls with appropriate rotation of the water dipole moments allowed a plausible dipole orientation model as predicted. The structural results are discussed in terms of protonation and H-bonding at the interface, and the results provide an ideal basis for testing theoretical predictions of characteristic surface properties such as pKa , sorption equilibria, and surface water permittivity.  相似文献   

2.
Steady-state element release rates from crystalline basalt dissolution at far-from-equilibrium were measured at pH from 2 to 11 and temperatures from 5 to 75 °C in mixed-flow reactors. Steady-state Si and Ca release rates exhibit a U-shaped variation with pH where rates decrease with increasing pH at acid condition but increase with increasing pH at alkaline conditions. Silicon release rates from crystalline basalt are comparable to Si release rates from basaltic glass of the same chemical composition at low pH and temperatures ?25 °C but slower at alkaline pH and temperatures ?50 °C. In contrast, Mg and Fe release rates decrease continuously with increasing pH at all temperatures. This behaviour is interpreted to stem from the contrasting dissolution behaviours of the three major minerals comprising the basalt: plagioclase, pyroxene, and olivine. Calcium is primarily present in plagioclase, which exhibits a U-shaped dissolution rate dependence on pH. In contrast, Mg and Fe are contained in pyroxene and olivine, minerals whose dissolution rates decrease monotonically with pH. As a result, crystalline basalt preferentially releases Mg and Fe relative to Ca at acidic conditions. The injection of acidic CO2-charged fluids into crystalline basaltic terrain may, therefore, favour the formation of Mg and Fe carbonates rather than calcite. Element release rates estimated from the sum of the volume fraction normalized dissolution rates of plagioclase, pyroxene, and olivine are within one order of magnitude of those measured in this study.  相似文献   

3.
The sediments in the Salford Quays, a heavily-modified urban water body, contain high levels of organic matter, Fe, Zn and nutrients as a result of past contaminant inputs. Vivianite [Fe3(PO4)2 · 8H2O] has been observed to have precipitated within these sediments during early diagenesis as a result of the release of Fe and P to porewaters. These mineral grains are small (<100 μm) and micron-scale analysis techniques (SEM, electron microprobe, μ-EXAFS, μ-XANES and Raman) have been applied in this study to obtain information upon the structure of this vivianite and the nature of Zn uptake in the mineral. Petrographic observations, and elemental, X-ray diffraction and Raman spectroscopic analysis confirms the presence of vivianite. EXAFS model fitting of the FeK-edge spectra for individual vivianite grains produces Fe–O and Fe–P co-ordination numbers and bond lengths consistent with previous structural studies of vivianite (4O atoms at 1.99–2.05 Å; 2P atoms at 3.17–3.25 Å). One analysed grain displays evidence of a significant Fe3+ component, which is interpreted to have resulted from oxidation during sample handling and/or analysis. EXAFS modelling of the Zn K-edge data, together with linear combination XANES fitting of model compounds, indicates that Zn may be incorporated into the crystal structure of vivianite (4O atoms at 1.97 Å; 2P atoms at 3.17 Å). Low levels of Zn sulphate or Zn-sorbed goethite are also indicated from linear combination XANES fitting and to a limited extent, the EXAFS fitting, the origin of which may either be an oxidation artifact or the inclusion of Zn sulphate into the vivianite grains during precipitation. This study confirms that early diagenetic vivianite may act as a sink for Zn, and potentially other contaminants (e.g. As) during its formation and, therefore, forms an important component of metal cycling in contaminated sediments and waters. Furthermore, for the case of Zn, the EXAFS fits for Zn phosphate suggest this uptake is structural and not via surface adsorption.  相似文献   

4.
We dissolved Boulder Creek Granodiorite in a plug flow reactor for 5794 h at pH = 1 and T = 25 °C. The primary purpose of the experiment was to identify controls on dissolved δ44/40Ca, δ44/42Ca, and δ26/24Mg values during granite weathering. Herein, we also examine the origin of Ca and Mg isotopic variability among minerals composing the Boulder Creek Granodiorite, and we constrain fundamental characteristics of granite weathering important for quantifying the elemental and isotopic geochemistry of the reactor output. Nine Ca-bearing minerals display an 8.80‰ range of δ44/40Ca values and a 0.51‰ range of δ44/42Ca values. Three Mg-bearing minerals display a 1.53‰ range of δ26/24Mg values. These ranges expressed at the mineralogical scale are higher than the ranges thus far reported for bulk igneous rocks. Most of the δ44/40Ca variability reflects 40Ca enrichment in K-feldspar, and to a lesser extent, biotite, due to the radioactive decay of 40K over the 1.7 Ga age of the rock, whereas the entire range of δ44/42Ca values reflects mass-dependent isotope fractionation during igneous differentiation and crystallization. The range of δ26/24Mg values may represent either fractionation during the chloritization of biotite or interaction of the Boulder Creek Granodiorite with Mg-rich metamorphic fluids having low δ26/24Mg values.The elemental and isotopic composition of the reactor output varied substantially during the experiment. We synthesize the mineralogical and fluid data using coupled mass-conservation equations solved at non-steady-state. Model calculations reveal an intricate balance between increasing specific surface area and decreasing mineral concentrations. While surface area normalized dissolution rate constants were time-invariant, specific surface area increased as a power-law function of time through positive feedbacks between mechanical disaggregation, chemical dissolution, and mineral depletion. Variations in dissolved δ44/40Ca, δ44/42Ca, and δ26/24Mg values reflect conservative mixing rather than fractionation. Apatite and calcite initially control δ44/40Ca and δ44/42Ca values, followed by biotite, titanite, epidote, hornblende, and plagioclase. The release of radiogenic 40Ca clearly defines the period where biotite dissolution dominates. The brucite layer of chlorite initially controls δ26/24Mg values, followed by biotite, the TOT layer of chlorite, and hornblende. Through direct isotopic tracking, these results demonstrate that trace minerals, such as apatite and calcite in the case of Ca and brucite in the case of Mg, dominate elemental release during the incipient stages of granite weathering. The results further show that biotite dissolution dominates the middle stages of granite weathering and that plagioclase dissolution only becomes important during relatively late stages. The Ca and Mg isotope variations associated with these stages are distinct and potentially resolvable in soil mineral weathering studies.  相似文献   

5.
Seismic hazard is associated with recent and present fault activity in mountain ranges. In the Betic-Rif alpine mountain chain, tectonic activity started in the Cretaceous, and topographic uplift continues since Tortonian times as a consequence of the NW-SE oblique convergence between Africa and Eurasia. The deformation is active and produces seismicity that sometimes has catastrophic consequences. The Al Hoceima earthquake (February 24, 2004), considered one of the largest earthquakes ever recorded instrumentally in the westernmost Mediterranean (M = 6.3), caused great damage in the region. Seismological studies agree that the main shock was situated on land, at the limit between the External and Internal Zones of the Rif, at a depth of 10-14 km. The focal mechanism points to a strike-slip solution with a NW-SE oriented P axis, quite similar to those of the significant 1994 earthquake swarm located to the north. The epicenter aftershocks distribution would signal the presence of a N-S oriented sinistral fault, activated by the NW-SE regional compression associated to plate boundary convergence. In this setting, the seismogenic fault ruptures related to these seismic events are expected to have reached the Earth's surface. However, detailed field work carried out 1 month after the earthquake does not evidence any N-S strike-slip coseismic fault in the epicentral area. The main observed effects were landslides, damages to constructions, and locally open cracks indicating an unexpected NW-SE extension. Scarce N-S faults are normal, the main ones being located several kilometers away from the epicentral area. To explain this apparent contradiction between geological and seismological observations, we propose a decoupled tectonic model with crustal detachments that separate a deep brittle crust from an upper crust undergoing uplift, and the development of large folds and normal faults. This geological setting, common to internal zones of cordilleras, may need to be taken into account in future paleoseismicity studies and in the assessment of seismic hazard.  相似文献   

6.
In order to identify the parent bodies of cosmic spherules (melted micrometeorites) with porphyritic olivine (PO) and cryptocrystalline (CC) textures, we measured the oxygen isotopic composition of 15 giant (>800 μm) cosmic spherules recovered in the Transantarctic Mountains, Antarctica, with IR-laser fluorination/mass spectrometry, and we conducted a characterization of their petrographic and magnetic properties. Samples include 6, 8 and 1 spherules of PO, CC and barred olivine (BO) textural types, respectively. Eleven spherules (∼70% of the total: 4/6 PO and 6/8 CC, and the BO spherule) are related to ordinary chondrites based on oxygen isotopic compositions. Olivines in ordinary chondrite-related spherules have compositions Fa8.5-11.8, they are Ni-poor to Ni-rich (0.04-1.12 wt.%), and tend to be richer in CaO than other spherules (0.10-0.17 wt.%). Ordinary-chondrite related spherules also have high magnetite contents (∼2-12 wt.%). One PO and one CC spherules are related to previously identified 17O-enriched cosmic spherules for which the parent body is unknown. One CC spherule has an oxygen isotopic signature relating it to CM/CR carbonaceous chondrites. The majority of PO/CC cosmic spherules derive from ordinary chondrites; this result exemplifies how the texture of cosmic spherules is not only controlled by atmospheric entry heating conditions but also depends on the parent body, whether be it through orbital parameters (entry angle and velocity), or chemistry, mineralogy, or grain size of the precursor.  相似文献   

7.
The pressure-volume-temperature-composition (PVTX) properties of H2O-CH4 were determined from the bubble point curve to 500 °C and 3 kbar for compositions ?4 mol.% CH4 using the synthetic fluid inclusion technique. H2O-CH4 inclusions were produced by loading known amounts of Al3C4 and H2O into platinum capsules along with pre-fractured and inclusion-free quartz cores. During heating the Al3C4 and H2O react to produce CH4, and the H2O-CH4 homogeneous mixture was trapped as inclusions during fracture healing at elevated temperature and pressure. The composition of the fluid in the inclusion was confirmed using the weight loss technique after the experiment and by Raman spectroscopic analysis of the inclusions.Homogenization temperatures of the inclusions were determined and the results were used to construct iso-Th lines, defined as a line connecting the formation temperature and pressure with the homogenization temperature and pressure. The pressure in the inclusion at the homogenization temperature was calculated from the Duan equation of state (EOS). The slope (ΔP/ΔT) of each iso-Th line was calculated and the results fitted to a polynomial equation using step-wise multiple regression analysis to estimate the slope of the iso-Th line as a function of the homogenization temperature and composition according to:
(ΔP/ΔT)=a+b·m+c·m4+d·(Th)2+e·m·Th+f·m·(Th)4,  相似文献   

8.
Sandstone dissolution is a common water–rock reaction in the Earth’s crust, but a thorough understanding of this phenomenon is constrained by poorly determined kinetic data. To this end, kinetic data were determined for the dissolution of arkosic sandstone powders in deionised water (pH was about 7.0–7.3 and electrical conductivity was between 0.95 and 1.00 μS/cm). Release rates of dissolved elements were determined over the range 50–350 °C at 20, 15, and 10 MPa using a column flow-through pressure vessel reactor. The conductivity of the outlet solution, measured at room temperature, is dependent on the charge of major cations such as Na+, K+, Ca2+ and Mg2+ at these conditions. The conductivity of the outlet solution was used to determine the steady state of the dissolution of sandstone powders. The pH values of the outlet solutions at the steady state, measured ex situ at room temperature, were about 7.7, 8.3, 8.4, 8.4 and 7.6 at 75, 100, 150, 200 and 250 °C, respectively, at 10 MPa. Silicon, Na, K, Ca, Al and Mg are the major ions found in the solution at low temperatures, but Si is the only major ion retained at higher temperatures (>150 °C). Compared with static experiments, the flowing dissolution experiments occurred at conditions far from equilibrium. The relationship between temperature and dissolution rates of arkosic sandstone powders was described as log R = 0.005469t − 10.50 where R is the dissolution rates of sandstone powders in kg/(m2 s), t is temperature in °C which ranged from 100 to 350 °C at 20 and 15 MPa, and the dissolution rates of sandstone powders were measured only for the major dissolved elements without oxygen in the outlet solutions.  相似文献   

9.
A new mineral eurekadumpite found at the Centennial Eureka Mine in the Tintic district of Juab County in Utah in the United States occurs in the oxidation zone along with quartz, macalpineite, malachite, Zn-bearing olivenite, goethite, and Mn oxides. Eurekadumpite forms spherulites or rosettes up to 1 mm in size and their clusters and crusts up to 1.5 cm2 in cavities. Its individuals are divergent and extremely thin (up to 0.5 mm across and less than 1 μm thick) hexagonal or roundish leaflets. The mineral is deep blue-green or turquoise-colored. Its streaks are light turquoise-colored. Its luster is satiny in aggregates and pearly on individual flakes. Its cleavage is (010) perfect and micalike. Its flakes are flexible but inelastic. Its Mohs hardness is 2.5–3.0, and D(meas) = 3.76(2) and D(calc) = 3.826 g/cm3. The mineral is optically biaxial negative, and α = 1.69(1), β ∼ γ = 1.775(5), and 2V meas = 10(5)°. Its pleochroism is strong: Y = Z = deep blue-green, and X = light turquoise-colored. Its orientation is X = b. The wavenumbers of the bands in the IR spectrum (cm−1; the strong lines are underlined, and w denotes the weak bands) are 3400, 2990, 1980w, 1628, 1373w, 1077, 1010, 860, 825, 803, 721w, 668, 622, 528, 461. The IR spectrum shows the occurrence of the tellurite (Te4+,O3)2− and arsenate (As5+,O4)3− anionic groups and H2O molecules; Cu and Zn cations are combined with OH− groups. The chemical composition of eurekadumpite is as follows (wt %, average of 14 electron-microprobe analyses; H2O determined using the Alimarin method): 0.04 FeO, 36.07 CuO, 20.92 ZnO, 14.02 TeO2, 14.97 As2O5, 1.45 Cl, 13.1 H2O, O = Cl2 −0.33, total 100.24. The empirical formula based on 2 Te atoms is (Cu10.32Zn5.85Fe0.01)Σ16.18(TeO3)2(AsO4)2.97[Cl0.93(OH)0.07]Σ1(OH)18.45 · 7.29H2O. The idealized formula is (Cu,Zn)16(TeO3)2(AsO4)3Cl(OH)18 · 7H2O. Eurekadumpite is monoclinic (pseudohexagonal), and the most probable space groups are P2/m, P2, or Pm. The unit-cell parameters refined from the powder X-ray data are as follows: a = 8.28(3), b = 18.97(2), c = 7.38(2) ?, β = 121.3(6)°, V = 990(6) ?3, and Z = 1. The strongest reflections of the X-ray powder pattern (d, ? (I) [hkl]) are as follows: 18.92(100) [010], 9.45(19) [020], 4.111(13) [[`2]\bar 2 01], 3.777(24) [050, [`2]\bar 2 21, 041], 2.692(15) [[`3]\bar 3 11, 151, [`3]\bar 3 02], 2.524(41)[170, [`2]\bar 2 52, [`1]\bar 1 71], 1.558(22) [[`4]\bar 4 82, [`3]\bar 3 .10.1, 024]. The name of the mineral means, firstly, that it was found in specimens from dumps of the Centennial Eureka Mine. In addition, it could mean found in a dump (the Greek word eureka means I have found it). There is an allusion to the great role that dumps of abandoned mines have played in the discovery of new minerals. Type specimens are deposited at the Fersman Mineralogical Museum of the Russian Academy of Sciences in Moscow, at the Smithsonian National Museum of Natural History in Washington, and at the American Museum of Natural History in New York.  相似文献   

10.
Enthalpies of formation of ferrihydrite and schwertmannite were measured by acid solution calorimetry in 5 N HCl at 298 K. The published thermodynamic data for these two phases and ε-Fe2O3 were evaluated, and the best thermodynamic data for the studied compounds were selected.Ferrihydrite is metastable in enthalpy with respect to α-Fe2O3 and liquid water by 11.5 to 14.7 kJ•mol−1 at 298.15 K. The less positive enthalpy corresponds to 6-line ferrihydrite, and the higher one, indicating lesser stability, to 2-line ferrihydrite. In other words, ferrihydrite samples become more stable with increasing crystallinity. The best thermodynamic data set for ferrihydrite of composition Fe(OH)3 was selected by using the measured enthalpies and (1) requiring ferrihydrite to be metastable with respect to fine-grained lepidocrocite; (2) requiring ferrihydrite to have entropy higher than the entropy of hypothetical, well-crystalline Fe(OH)3; and (3) considering published estimates of solubility products of ferrihydrite. The ΔG°f for 2-line ferrihydrite is best described by a range of −708.5±2.0 to −705.2±2.0 kJ•mol−1, and ΔG°f for 6-line ferrihydrite by −711.0±2.0 to −708.5±2.0 kJ•mol−1.A published enthalpy measurement by acid calorimetry of ε-Fe2O3 was re-evaluated, arriving at ΔH°f (ε-Fe2O3) = −798.0±6.6 kJ•mol−1. The standard entropy (S°) of ε-Fe2O3 was considered to be equal to S° (γ-Fe2O3) (93.0±0.2 J•K−1•mol−1), giving ΔG°f (ε-Fe2O3) = −717.8±6.6 kJ•mol−1. ε-Fe2O3 thus appears to have no stability field, and it is metastable with respect to most phases in the Fe2O3-H2O system which is probably the reason why this phase is rare in nature.Enthalpies of formation of two schwertmannite samples are: ΔH°f (FeO(OH)0.686(SO4)0.157•0.972H2O) = −884.0±1.3 kJ•mol−1, ΔH°f (FeO(OH)0.664(SO4)0.168•1.226H2O) = −960.7±1.2 kJ•mol−1. When combined with an entropy estimate, these data give Gibbs free energies of formation of −761.3 ± 1.3 and −823.3 ± 1.2 kJ•mol−1 for the two samples, respectively. These ΔGf° values imply that schwertmannite is thermodynamically favored over ferrihydrite over a wide range of pH (2-8) when the system contains even small concentration of sulfate. The stability relations of the two investigated samples can be replicated by schwertmannite of the “ideal” composition FeO(OH)3/4(SO4)1/8 with ΔG°f = −518.0±2.0 kJ•mol−1.  相似文献   

11.
根据X射线衍射(XRD)分析发现: A Fe3(SO4)2(OH)6(A=K+、H3O+)系列铁钒的XRD数据十分相近,难以用XRD区别,需通过能谱(EDS)辅助分析,才能区分此类铁矾。另外,此类铁矾的003和107面网间距d随K+含量增大而增大,且呈一元三次方程的关系;而033和220面网间距d随K+含量增大而减小,呈一元二次方程的关系。对该现象从铁矾晶体结构方面进行解释:K+、H3O+离子位于较大空隙中,且沿着Z轴方向排列,当K+、H3O+离子之间相互替换时,会导致该铁矾晶体结构在Z轴方向有较明显的变化。  相似文献   

12.
Chemical (meta)sedimentary rocks in the amphibolite facies ≥3700 Ma Isua supracrustal belt (W. Greenland) are mostly strongly deformed, so there is only a small chance of the survival of features such as stromatolites or microfossils that would be direct proof of a ≥3700 Ma biosphere. Therefore the search for evidence of ≥3700 Ma life in Isua rocks has focused on chemical signatures, particularly C-isotopes. The new approach presented here is based on whole rock chemistry rather than isotopic signatures. Isua chemical sedimentary rocks have Ca–Mg–Fe bulk compositions that coincide with ferroan dolomite – siderite/Fe-oxide mixtures. Most have low Al2O3, TiO2 contents (<0.5 and <0.05 wt% respectively) showing minimal contamination from terriginous materials. Identical seawater-like REE + Y shale-normalised trace element signatures with La, Ce, Eu and Y positive anomalies are found in magnetite-rich banded iron formation (BIF – such as the geochemical standard IF-G), dolomite-rich rocks and quartz–carbonate–calc-silicate rocks. Additionally from a rare, small area of low deformation in Isua, there are ∼3700 Ma pillow lava interstices consisting of quartz + tremolite + calcite derived from pre-metamorphic dolomite + silica. Thus the dolomite in the chemical sediments and the pillow interstice was part of the pre-metamorphic assemblage, and was deposited from seawater and/or low-temperature groundwater (as shown by the REE + Y chemistry). Therefore, at least some Isua carbonate rocks are sedimentary or diagenetic in origin rather than being formed by metasomatism at 600–500 °C as proposed by Rose et al. (1996. American Journal of Science 296, 1004–1044).  相似文献   

13.
异构比φiC4 /φnC4 和φiC5 /φnC5 的石油地质意义   总被引：6，自引：1，他引：6  
同分子量的正构烷烃和异构烷烃存在着物理化学性质差异,在运移过程中受围岩的物理化学性质及其它外部因素的影响必然产生分异效应,从而使二者在空间分布上具有一定的特征和规律,异构比指标可以在一定程度上反映出这种特征和规律性。用异构比φiC4 /φnC4 和φiC5 /φnC5 指标可以判断有机质的成熟度,研究轻烃运移的途径、方向、生成环境及轻烃的生物降解。  相似文献   

14.
Biachellaite, a new mineral species of the cancrinite group, has been found in a volcanic ejecta in the Biachella Valley, Sacrofano Caldera, Latium region, Italy, as colorless isometric hexagonal bipyramidal-pinacoidal crystals up to 1 cm in size overgrowing the walls of cavities in a rock sample composed of sanidine, diopside, andradite, leucite and hauyne. The mineral is brittle, with perfect cleavage parallel to {10$ \bar 1 $ \bar 1 0} and imperfect cleavage or parting (?) parallel to {0001}. The Mohs hardness is 5. Dmeas = 2.51(1) g/cm3 (by equilibration with heavy liquids). The densities calculated from single-crystal X-ray data and from X-ray powder data are 2.515 g/cm3 and 2.520 g/cm3, respectively. The IR spectrum demonstrates the presence of SO42−, H2O, and absence of CO32−. Biachellaite is uniaxial, positive, ω = 1.512(1), ɛ = 1.514(1). The weight loss on ignition (vacuum, 800°C, 1 h) is 1.6(1)%. The chemical composition determined by electron microprobe is as follows, wt %: 10.06 Na2O, 5.85 K2O, 12.13 CaO, 26.17 Al2O3, 31.46 SiO2, 12.71 SO3, 0.45 Cl, 1.6 H2O (by TG data), −0.10 −O=Cl2, total is 100.33. The empirical formula (Z = 15) is (Na3.76Ca2.50K1.44)Σ7.70(Si6.06Al5.94O24)(SO4)1.84Cl0.15(OH)0.43 · 0.81H2O. The simplified formula is as follows: (Na,Ca,K)8(Si6Al6O24)(SO4)2(OH)0.5 · H2O. Biachellaite is trigonal, space group P3, a =12.913(1), c = 79.605(5) ?; V = 11495(1) ?3. The crystal structure of biachellaite is characterized by the 30-layer stacking sequence (ABCABCACACBACBACBCACBACBACBABC)∞. The tetrahedral framework contains three types of channels composed of cages of four varieties: cancrinite, sodalite, bystrite (losod) and liottite. The strongest lines of the X-ray powder diffraction pattern [d, ? (I, %) (hkl)] are as follows: 11.07 (19) (100, 101), 6.45 (18) (110, 111), 3.720 (100) (2.1.10, 300, 301, 2.0.16, 302), 3.576 (18) (1.0.21, 2.0.17, 306), 3.300 (47) (1.0.23, 2.1.15), 3.220 (16) (2.1.16, 222). The type material of biachellaite has been deposited at the Fersman Mineralogical Museum of the Russian Academy of Sciences, Moscow, Russia, registration number 3642/1.  相似文献   

15.
This paper reports in situ observations on barite (0 0 1) surface dissolution behavior in 0.1–0.001 M NaCl solutions at 30 °C using atomic force microscopy (AFM). The step retreating on barite (0 0 1) surfaces changed with increasing NaCl solution concentrations. In solutions with a higher NaCl concentration (⩾0.01 M), many steps showed curved or irregular fronts during the later experimental stage, while almost all steps in solutions with a lower NaCl concentration exhibited straight or angular fronts, even during the late stage. The splitting phenomenon of the initial 〈h k 0〉 one-layer steps (7.2 Å) into two half-layer steps (3.6 Å) occurred in all NaCl solutions, while that of the initial [0 1 0] one-layer steps observed only in the 0.1 M NaCl solution. The step retreat rates increased with an increasing NaCl solution concentration. We observed triangular etch pit and deep etch pit formation in all NaCl solutions, which tended to form late in solutions with lower NaCl concentrations. The deep etch pit morphology changed with increasing NaCl solution concentrations. A hexagonal form elongated in the [0 1 0] direction was bounded by the {1 0 0}, {3 1 0}, and (0 0 1) faces in a 0.001 M NaCl solution, and a rhombic form was bounded by the {5 1 0} and (0 0 1) faces in 0.01 M and 0.1 M NaCl solutions. An intermediate form was observed in a 0.005 M NaCl solution, which was defined by {1 0 0}, a curved face tangent to the [0 1 0] direction, {3 1 0}, and (0 0 1) faces: the intermediate form appeared between the hexagonal and rhombic forms in solutions with lower and higher NaCl concentrations, respectively. The triangular etch pit and deep etch pit growth rates also increased with the NaCl solution concentration. Combining the step and face retreat rates in NaCl solutions estimated in this AFM study as well as the data on the effect of water temperature on the retreat rates reported in our earlier study, we produced two new findings. One finding is that the retreat rates increase by approximately two-fold when the NaCl solution concentration increases by one order of magnitude, and the other finding is that the retreat rate increase due to a one order of magnitude increase in the NaCl concentration corresponds to an increase of approximately 8 °C in water temperature. This correlation may help to understand and evaluate increasing dissolution kinetics induced by the different mechanisms where barite dissolution is promoted by the catalytic effect of Na+ and Cl− ions (through an increase in the NaCl solution concentration) or by an increase in the hydration of Ba2+ and SO42− (through an increase in water temperature).  相似文献   

16.
Iron and Sr bearing phases were thoroughly investigated by means of spectrometric and microscopic techniques in Callovian–Oxfordian (COX) samples originating from the ANDRA Underground Research Laboratory (URL) in Bure (France). Strontium was found to be essentially associated with celestite, whereas Fe was found to be distributed over a wide range of mineral phases. Iron was mainly present as Fe(II) in the studied samples (∼93% from Mössbauer results). Most of the Fe(II) was found to be in pyrite, sideroplesite/ankerite and clay minerals. Iron(III), if present, was associated with clay minerals (probably illite, illite-smectite mixed layer minerals and chlorite). No Fe(III) oxy(hydro)xide could be detected in the samples. Strontianite was not observed either. Based on these observations, it is likely that the COX porewater is in equilibrium with the following carbonate minerals, calcite, dolomite and ankerite/sideroplesite, but not with strontianite. It is shown that this equilibrium information can be combined with clay cation exchange composition information in order to give direct estimates or constraints on the solubility products of the carbonate minerals dolomite, siderite and strontianite. As a consequence, an experimental method was developed to retrieve the cation exchanged Fe(II) in very well preserved COX samples.  相似文献   

17.
A 30,000 yr dinocyst and pollen record from the eastern equatorial Atlantic (off Cameroon) has been investigated in order to identify land–ocean linkages during the last deglacial transition. A strong correlation between the abundance of Brigantedinium spp. and the Ca/Fe ratio during the last glacial period suggests enhanced marine productivity in association with cool seawater temperatures and nutrient input linked to coastal upwelling and/or a proximal river mouth. Dry conditions are recorded on the adjacent continent with a significant representation of open vegetation indicators and the Afromontane taxon Podocarpus. After 17 cal ka BP these indicators register a sharp decline as a result of a climatic transition from the dry/cooler conditions of the last glacial period to the wetter/warmer conditions of the deglaciation. Simultaneously, dinocysts show a significant shift from dominant heterotrophs to an increasing abundance of autotrophs, reflecting warmer conditions. Significant changes are observed during the Younger Dryas, with a return to drier conditions and higher salinities. The start of the Holocene is marked by very low-salinity conditions, reflecting optimal monsoonal conditions over west equatorial Africa. The end of the African Humid Period is observed between 6 and 5 cal ka BP, followed by significant fluctuations in both terrestrial and oceanic proxies.  相似文献   

18.
Any progress in our understanding of low-temperature mineral assemblages and of quantitative physico-chemical modeling of stability conditions of mineral phases, especially those containing toxic elements like selenium, strongly depends on the knowledge of structural and thermodynamic properties of coexisting mineral phases. Interrelation of crystal chemistry/structure and thermodynamic properties of selenium-containing minerals is not systematically studied so far and thus any essential generalization might be difficult, inaccurate or even impossible and erroneous. Disagreement even exists regarding the crystal chemistry of some natural and synthetic selenium-containing phases. Hence, a systematic study was performed by synthesizing ferric selenite hydrates and subsequent thermal analysis to examine the thermal stability of synthetic analogues of the natural hydrous ferric selenite mandarinoite and its dehydration and dissociation to unravel controversial issues regarding the crystal chemistry. Dehydration of synthesized analogues of mandarinoite starts at 56–87?°C and ends at 226–237?°C. The dehydration happens in two stages and two possible schemes of dehydration exist: (a) mandarinoite loses three molecules of water in the first stage of the dehydration (up to 180?°C) and the remaining two molecules of water will be lost in the second stage (>180?°C) or (b) four molecules of water will be lost in the first stage up to 180?°C and the last molecule of water will be lost at a temperature above 180?°C. Based on XRD measurements and thermal analyses we were able to deduce Fe2(SeO3)3·(6-x)H2O (x?=?0.0–1.0) as formula of the hydrous ferric selenite mandarinoite. The total amount of water apparently affects the crystallinity, and possibly the stability of crystals: the less the x value, the higher crystallinity could be expected.  相似文献   

19.
Relatively few radiometrically dated records are available for the central Mediterranean spanning the marine oxygen isotope stage 6–5 (MIS 6–5) transition and the first part of the Last Interglacial. Two flowstone cores from Tana che Urla Cave (TCU, central Italy), constrained by 19 U/Th ages, preserve an interval of continuous speleothem deposition between ca. 159 and 121 ka. A multiproxy record (δ18O, δ13C, growth rate and petrographic changes) obtained from this flowstone preserves significant regional-scale hydrological changes through the glacial/interglacial transition and multi-centennial variability (interpreted as alternations between wetter and drier periods) within both glacial and interglacial stages. The glacial stage shows a wetter period between ca. 154 and 152 ka, while the early to middle Last Interglacial period shows several drying events at ca. 129, 126 and 122 ka, which can be placed in the wider context of climatic instability emerging from North Atlantic marine and NW European terrestrial records. The TCU record also provides important insights into the evolution of local environmental conditions (i.e. soil development) in response to regional and global-scale climate events.  相似文献   

20.
韩建平 《物探与化探》1994,18(6):476-477,472
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