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11.
12.
Mossbauer spectroscopy has been used to determine the redox equilibria of iron and structure of quenched melts on the composition join Na2Si2O5-Fe2O3 to 40 kbar pressure at 1400° C. The Fe3+/ΣFe decreases with increasing pressure. The ferric iron appears to undergo a gradual coordination transformation from a network-former at 1 bar to a network-modifier at higher (≧10 kbar) pressure. Ferrous iron is a network-modifier in all quenched melts. Reduction of Fe3+ to Fe2+ and coordination transformation of remaining Fe3+ result in depolymerization of the silicate melts (the ratio of nonbridging oxygens per tetrahedral cations, NBO/T, increases). It is suggested that this pressure-induced depolymerization of iron-bearing silicate liquids results in increasing NBO/T of the liquidus minerals. Furthermore, this depolymerization results in a more rapid pressure-induced decrease in viscosity and activation energy of viscous flow of iron-bearing silicate melts than would be expected for iron-free silicate melts with similar NBO/T. 相似文献
13.
A general model for the structural state of iron in a variety of silicate and aluminosilicate glass compositions in the systems Na2O-Al2O3-SiO2-Fe-O, CaO-Al2O3-SiO2-Fe-O, and MgO-Al2O3-SiO2-Fe-O is proposed. Quenched melts with variable Al/Si and NBO/T (average number of nonbridging oxygens per tetrahedrally coordinated cation), synthesized over a range of temperatures and values of oxygen fugacity, are analyzed with57Fe Mössbauer spectroscopy. For oxidized glasses with Fe3+/∑Fe>0.50, the isomer shift for Fe3+ is in the range ~0.22–0.33 mm/s and ~0.36 mm/s at 298 K and 77 K, respectively. These values are indicative of tetrahedrally coordinated Fe3?. This assignment is in agreement with the interpretation of Raman, luminescence, and X-ray,K-edge absorption spectra. The values of the quadrupole splitting are ~0.90 mm/s (298 K and 77 K) in the Na-aluminosilicate glasses and compare with the values of 1.3 mm/s and 1.5 mm/s for the analogous Ca- and Mg-aluminosilicate compositions. The variations in quadrupole splittings for Fe3+ are due to differences in the degree of distortion of the tetrahedrally coordinated site in each of the systems. The values of the isomer shifts for Fe2+ ions in glasses irrespective of Fe3+/∑Fe are in the range 0.90–1.06 mm/s at 298 K and 1.0–1.15 mm/s at 77 K. The corresponding range of values of the quadrupole splitting is 1.75–2.10 mm/s at 298 K and 2.00–2.35 mm/s at 77 K. The temperature dependence of the hyperfine parameters for Fe2+ is indicative of noninteracting ions, but the values of the isomer shift are intermediate between those values normally attributable to tetrahedrally and octahedrally coordinated Fe2+. The assignment of the isomer-shift values of Fe2+ to octahedral coordination is in agreement with the results of other spectral studies. For reduced glasses (Fe3+/∑Fe≈<0.50), the value of the isomer shift for Fe3+ at both 298 K and 77 K increases and is linearly correlated with decreasing Fe3+/∑Fe in the range of \(f_{O_2 } \) between 10?3 and 10?6 atm when a single quadrupole-split doublet is assumed to represent the absorption due to ferric iron. The increase in value of the isomer shift with decreasing \(f_{O_2 } \) is consistent with an increase in the proportion of Fe3+ ions that are octahedrally coordinated. The concentration of octahedral Fe3+ is dependent on the \(T - f_{O_2 } \) conditions, and in the range of log \(f_{O_2 } \) between 10?2.0 and 10?5 a significant proportion of the iron may occur as iron-rich structural units with stoichiometry similar to that of inverse spinels such as Fe3O4, in addition to isolated Fe2+ and Fe3+ ions. 相似文献
14.
Bjørn Mysen 《Earth》1984,20(3):251-252
15.
The anionic structure of magmatic liquids has been estimated at 1 atm and at pressures corresponding to those of the upper mantle. These estimates are based predominantly on spectroscopic data on binary metal oxide-silica and ternary metal oxide-silica-alumina melts. Structural information on melt compositions in aluminate-silica joins has been used to provide detailed information on the role of Al3+ in natural magma at atmospheric and high pressure.Regardless of pressure, andesitic melts may be described as combinations of chain, sheet, and three-dimensional network units. Nearly all Al3+ in the magmatic liquid resides in the three-dimensional network units. This Al3+ is locally charge-balanced with Na+, K+, Ca2+, and Mg2+. In the latter two cases, Al3+ and Si4+ are ordered, whereas for Na+ and K+, Si4+ and Al3+ are randomly mixed. Solution of water in natural magma results in the formation of new nonbridging oxygens in addition to OH groups attached to Si4+ and metal cations.On the basis of determined solution mechanisms of CO2 and H2O in silicate melts, thermodynamic properties of HO+CO2, fluids and hydrous silicate melts and melting phase relations in peridotite-H2O-CO2, systems, it is found that natural andesitic magma in equilibrium with spinel Iherzolite in the upper mantle (10–20 kbar) must contain at least 5–7 wt.% H2O. Andesitic magma with 5–7 wt.% H2O in solution may be described as a mixture of Al-free three-dimensional units, sheets, and chains with a small proportion (less than 10%) of monomers. 相似文献
16.
The distribution of Mn was examined in the bottom sediments and water column (suspended paniculate matter) of the Laurentian Trough. Gulf of St. Lawrence. A characteristic profile of Mn with depth in the sediment consisted of a Mn-enriched surface oxidized zone, less than 20 mm thick, and a Mn-depleted subsurface reducing zone. A subsurface Mn maximum occurred within the oxidized zone. Below this maximum the concentration dropped sharply to nearly constant residual levels in the reducing zone. The accumulating estuarine sediments are deficient in Mn compared to the river input of suspended matter and are definitely not the ultimate sink for manganese. Manganese escapes from the sediment by diffusion and resuspension, forming Mn-enriched, fine-grained particles which are flushed out in the estuarine circulation. 5.0 × 109gyr?1 of Mn, or 50% more than the river input of dissolved Mn. are exported to the open ocean. In spite of the efficient mobilization and export of Mn, the quantity exported is a small fraction (0.2%) of the total flux to the deep-sea sediments. This is related to the low levels of paniculate matter transported by the St. Lawrence River. The export phénomenon, however, is probably true of many coastal regions of muddy sediments and thus has interesting implications for the oceanic budget of Mn. 相似文献
17.
Bjørn Mysen 《Contributions to Mineralogy and Petrology》1975,52(2):69-76
The iron-magnesium distribution coefficient, $$K'_D = (X_{\Sigma {\text{FeO}}} /X_{{\text{MgO}}} )^{{\text{olivine}}} (X_{{\text{MgO}}} /X_{\Sigma {\text{FeO}}} )^{{\text{liquid}}} ,$$ has frequently been used as a means of testing whether experimental and natural silicate liquids could have been in equilibrium with olivine of mantle composition. It is shown here that this K′ D decreases with increasing oxygen fugacity (xxx) for a hydrous partial melt in equilibrium with a natural spinel peridotite assemblage under pressure and temperature conditions corresponding to those of the upper mantle (from 0.52 at the xxx of the iron-wüstite buffer to 0.04 at the xxx of the magnetite-hematite buffer). K′ D also increases with increasing pressure, with decreasing temperature, and probably with increasing Mg/(Mg+∑ Fe) of the parental peridotite, suggesting that $$K_D = (X_{{\text{FeO}}} /X_{{\text{MgO}}} )^{{\text{olivine}}} (X_{{\text{MgO}}} /X_{{\text{FeO}}} )^{{\text{liquid}}}$$ also increases with increasing pressure and decreasing temperature. Thus, unless these four variables (P, T, xxx, silicate composition) are known for a natural magma, K′ D and probably K D are variables, and the Mg/(Mg+∑ Fe) of such a magma cannot be correlated to that of the parent. The K D determined at 1 atm pressure by Roeder and Emslie has frequently been used to test whether the Mg/(Mg+∑ Fe) ratios of experimentally formed liquids at high pressure in equilibrium with olivine of known Fo content represent the equilibrium Mg/(Mg+Fe2+) of this liquid, assuming that ∑Fe=Fe2+ and that K′ D does not vary with P, T, and composition of the system. Published data demonstrate that the oxygen fugacities of the experimental designs employed by different laboratories vary between those of the magnetite-hematite and magnetite-wüstite buffers (6 orders of magnitude), resulting in K′ D between 0.04 and 0.31 at 1050° C and 15 kbar, for example. Thus, published arguments as to whether the quenched liquids represent equilibrium compositions based on iron-magnesium partitioning are inadequate. The effects of P, T, xxx, and the composition of the starting material must also be considered. 相似文献
18.
Nickel partitioning between forsterite and aluminosilicate melt of fixed bulk composition has been determined at 1300°C to 20 kbar pressure. The value of the forsterite-liquid nickel partition coefficient is lowered from >20 at pressures equal to or less than 15 kbar to <10 at pressures above 15 kbar.Published data indicate that melts on the join Na2O-Al2O3-SiO2 become depolymerized in the pressure range 10–20 kbar as a result of Al shifting from four-coordination at low pressure to higher coordination as the pressure is increased. This coordination shift results in a decreasing number of bridging oxygens in the melt. It is suggested that the activity coefficient of nickel decreases with this decrease in the number of bridging oxygens. As a result, the nickel partition coefficient for olivine and liquid is lowered.Magma genesis in the upper mantle occurs in the pressure range where the suggested change in aluminum coordination occurs in silicate melts. It is suggested, therefore, that data on nickel partitioning obtained at low pressure are not applicable to calculation of the nickel distribution between crystals and melts during partial melting in the upper mantle. Application of high-pressure experimental data determined here for Al-rich melts to the partial melting process indicates that the melts would contain about twice as much nickel as indicated by the data for the low-pressure experiments. If, as suggested here, the polymerization with pressure is related to the Al content of the melt, the difference in the crystal-liquid partition coefficient for nickel at low and high pressure is reduced with decreasing Al content of the melt. Consequently, the change ofDNiol-andesite melt is greater than that ofDNiol-basalt melt, for example. 相似文献
19.
20.
The structure of silicate melts in the system Na2O·4SiO2 saturated with reduced C-O-H volatile components and of coexisting silicate-saturated C-O-H solutions has been determined in a hydrothermal diamond anvil cell (HDAC) by using confocal microRaman and FTIR spectroscopy as structural probes. The experiments were conducted in-situ with the melt and fluid at high temperature (up to 800 °C) and pressure (up to 1435 MPa). Redox conditions in the HDAC were controlled with the reaction, Mo + H2O = MoO2 + H2, which is slightly more reducing than the Fe + H2O = FeO + H2 buffer at 800 °C and less.The dominant species in the fluid are CH4 + H2O together with minor amounts of molecular H2 and an undersaturated hydrocarbon species. In coexisting melt, CH3 - groups linked to the silicate melt structure via Si-O-CH3 bonding may dominate and possibly coexists with molecular CH4. The abundance ratio of CH3 - groups in melts relative to CH4 in fluids increases from 0.01 to 0.07 between 500 and 800 °C. Carbon-bearing species in melts were not detected at temperatures and pressures below 400 °C and 730 MPa, respectively. A schematic solution mechanism is, Si-O-Si + CH4?Si-O-CH3+H-O-Si. This mechanism causes depolymerization of silicate melts. Solution of reduced (C-O-H) components will, therefore, affect melt properties in a manner resembling dissolved H2O. 相似文献