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1.
High-temperature X-ray diffraction experiments have been performed on melilite solid solutions, on single crystal and powder samples. In åkermanite–gehlenite series, the volumetric thermal expansion increases from gehlenite, 26.5(2) E-06 K-1, to åkermanite, 31.2(1) E-06 K-1. The variation is related to the cation content in the tetrahedral T1 site of the structure, and the linear expansion along the a axis has the greatest variation as a function of composition. The expansion perpendicular to the tetrahedral layers does not present any significant variation as a function of composition. In the åkermanite–Na melilite series, the presence of Na in the [8]-coordinated site strongly increases the linear expansion along the c axis, while the volumetric expansion decreases from åkermanite to Na melilite, whose value can be extrapolated to 27.4 E-06 K-1  相似文献   

2.
Growth rates of monomineralic, polycrystalline åkermanite (Ca2MgSi2O7) rims produced by solid-state reactions between monticellite (CaMgSiO4) and wollastonite (CaSiO3) single crystals were determined at 0.5 GPa dry argon pressure, 1,000–1,200°C and 5 min to 60 h, using an internally heated pressure vessel. Inert Pt-markers, initially placed at the monticellite–wollastonite interface, indicate symmetrical growth into both directions. This and mass balance considerations demonstrate that rim growth is controlled by transport of MgO. At 1,200°C and run durations between 5 min and 60 h, rim growth follows a parabolic rate law with rim widths ranging from 0.4 to 16.3 μm indicating diffusion-controlled rim growth. The effective bulk diffusion coefficient \( D_{\text{eff,MgO}}^{\text{Ak}} \) is calculated to 10?15.8±0.1 m2 s?1. Between 1,000°C and 1,200°C, the effective bulk diffusion coefficient follows an Arrhenius law with E a = 204 ± 18 kJ/mol and D 0 = 10?8.6±1.6 m2 s?1. Åkermanite grains display a palisade texture with elongation perpendicular to the reaction interface. At 1,200°C, average grain widths measured normal to elongation, increase with the square root of time and range from 0.4 to 5.4 μm leading to a successive decrease in the grain boundary area fraction, which, however, does not affect \( D_{\text{eff,MgO}}^{\text{Ak}} \) to a detectible extent. This implies that grain boundary diffusion only accounts for a minor fraction of the overall chemical mass transfer, and rim growth is essentially controlled by volume diffusion. This is corroborated by the agreement between our estimates of the effective MgO bulk diffusion coefficient and experimentally determined volume diffusion data for Mg and O in åkermanite from the literature. There is sharp contrast to the MgO–SiO2 binary system, where grain boundary diffusion controls rim growth.  相似文献   

3.
4He accumulated in fluids is a well established geochemical tracer used to study crustal fluid dynamics. Direct fluid samples are not always collectable; therefore, a method to extract rare gases from matrix fluids of whole rocks by diffusion has been adapted. Helium was measured on matrix fluids extracted from sandstones and mudstones recovered during the San Andreas Fault Observatory at Depth (SAFOD) drilling in California, USA. Samples were typically collected as subcores or from drillcore fragments. Helium concentration and isotope ratios were measured 4?C6 times on each sample, and indicate a bulk 4He diffusion coefficient of 3.5?±?1.3?×?10?C8 cm2?s?C1 at 21°C, compared to previously published diffusion coefficients of 1.2?×?10?C18 cm2?s?C1 (21°C) to 3.0?×?10?C15 cm2?s?C1 (150°C) in the sands and clays. Correcting the diffusion coefficient of 4Hewater for matrix porosity (??3%) and tortuosity (??6?C13) produces effective diffusion coefficients of 1?×?10?C8 cm2?s?C1 (21°C) and 1?×?10?C7 (120°C), effectively isolating pore fluid 4He from the 4He contained in the rock matrix. Model calculations indicate that <6% of helium initially dissolved in pore fluids was lost during the sampling process. Complete and quantitative extraction of the pore fluids provide minimum in situ porosity values for sandstones 2.8?±?0.4% (SD, n?=?4) and mudstones 3.1?±?0.8% (SD, n?=?4).  相似文献   

4.
Synthetic Fe3+-melilites containing NaCaFe3+-Si2O7-, Ca2Fe3+AlSiO7- or Sr2Fe3+AlSiO7-components have been studied by 57Fe Mössbauer spectroscopy. The spectrum of åkermanite containing an NaCaFe3+Si2O7-component consists of one doublet identified to belong to Fe3+ in T1 sites. The spectra of åkermanite and gehlenite containing Ca2Fe3+ AlSiO7- or Sr2Fe3+ AlSiO7-component consist of two doublets. The inner and outer doublets are identified to belong to Fe3+ in the less distorted T1 and that in the more distorted T2 sites, respectively. The area ratios of the spectra show that the site occupancy of Fe3+ (T1) in gehlenite is less than that in åkermanite in which the distribution of Fe3+ in T1 and T2 sites is apparently random. The different distributions can be explained in terms of competition between minimizing the deficiency in the electrostatic valence and the preference of Al for T1 sites which the isomer shift measurements show to be more ionic.  相似文献   

5.
Synthetic melilites on the join Ca2MgSi2O7 (åkermanite: Ak)-Ca2Fe3+AlSiO7 (ferrialuminium gehlenite: FAGeh) were studied using X-ray powder diffraction and 57Fe Mössbauer spectroscopic methods to determine the distribution of Fe3+ between two different tetrahedral sites (T1 and T2), and the relationship between ionic substitution and incommensurate (IC) structure. Melilites were synthesized from starting materials with compositions of Ak100, Ak80FAGeh20, Ak70FAGeh30 and Ak50FAGeh50 by sintering at 1,170–1,350 °C and 1 atm. The average chemical compositions and end-member components, Ak, FAGeh and Geh (Ca2Al2SiO7), of the synthetic melilites were Ca2.015Mg1.023Si1.981O7 (Ak100), Ca2.017Mg0.788Fe 0.187 3+ Al0.221Si1.791O7 (Ak78FAGeh19Geh3), Ca1.995Mg0.695Fe 0.258 3+ Al0.318Si1.723O7 (Ak69FAGeh25Geh6) and Ca1.982Mg0.495Fe 0.449 3+ Al0.519Si1.535O7 (Ak49FAGeh44Geh7), respectively. Rietveld refinements using X-ray powder diffraction data measured using CuK α -radiation at room temperature converged successfully with goodness-of-fits of 1.15–1.26. The refined Fe occupancies at the T1 and T2 sites and the Mg and Si contents determined by electron microprobe analysis gave the site populations of [0.788Mg + 0.082Fe3+ + 0.130Al]T1[0.104Fe3+ + 0.104Al + 1.792Si]T2 for Ak78FAGeh19Geh3, [0.695Mg + 0.127Fe3+ + 0.178Al]T1[0.132Fe3+ + 0.144Al + 1.724Si]T2 for Ak69FAGeh25Geh6 and [0.495Mg + 0.202Fe3+ + 0.303Al]T1[0.248Fe3+ + 0.216Al + 1.536Si]T2 for Ak49FAGeh44Geh7 (apfu: atoms per formula unit), respectively. The results indicate that Fe3+ is distributed at both the T1 and the T2 sites. The mean T1–O distance decreases with the substitution of Fe3+ + Al3+ for Mg2+ at the T1 site, whereas the mean T2–O distance increases with substitution of Fe3+ + Al3+ for Si4+ at the T2 site, causing decrease in the a dimension and increase in the c dimension. However, in spite of the successful Rietveld refinements for the X-ray powder diffraction data measured using CuK α-radiation at room temperature, each Bragg reflection measured using CuK α1-radiation at room temperature showed weak shoulders, which were not observed in those measured at 200 °C. The Mössbauer spectra of the melilites measured at room temperature consist of two doublets assigned to Fe3+ at the T1 site and two or three doublets to Fe3+ at the T2 site, implying the existence of multiple T1 and T2 sites with different site distortions. These facts can be interpreted in terms of the IC structure in all synthetic melilites at room temperature, respectively. The results of Mössbauer analysis indicate that the IC structure in melilite is caused by not only known multiple T1 site, but also multiple T2 site at room temperature.  相似文献   

6.
The weathering rates and mechanisms of three types of glassy rocks were investigated experimentally at 25 °C, pH 1.0 to 6.2, and reaction times as much as to 3 months. Changes in major element chemistry were monitored concurrently as a function of time in the aqueous solution and within the near surface region of the glass. Leach profiles, obtained by a HF leaching technique, displayed near-surface zones depleted in major cations. These zones increased in depth with increasing time and decreasing pH of reactions. Release rates into the aqueous solution were parabolic for Na and K and linear for Si and Al. A coupled weathering model, involving surface dissolution with concurrent diffusion of Na, K, and Al, produced a mass balance between the aqueous and glass phases. Steady state conditions are reached at pH 1.0 after approximately 3 weeks of reaction. Steady-state is not reached even after 3 months at pH 6.2.An interdiffusion model describes observed changes in Na diffusion profiles for perlite at pH 1.0. The calculated Na self-diffusion coefficient of 5 × 10?19 cm2·s?1 at 25°C approximates coefficients extrapolated from previously reported high temperature data for obsidian. The self-diffusion coefficient for H3O+, 1.2 × 10?20 cm2·s?1, is similar to measured rates of water diffusion during hydration of obsidian to form perlite.  相似文献   

7.
Tracer diffusion coefficients of 153Gd and 152Eu in olivine tholeiite have been determined at temperatures between 1150 and 1440°C. The results are identical for both tracers within experimental error. Between 1440 and 1320°C the diffusion coefficients are given by D(Eu, Gd) = 0.058 exp(?40,600/ RT). Between 1320 and 1210°C, the diffusion coefficients are constant at D = (1.4 ± 0.4) × 10?7 cm2s?1 and between 1210 and 1150°C, the D values drop irregularly to 4 × 10?9 cm2s?1. The liquidus temperature (1270°C) lies within the region of constant D. Such anomalous behavior has not been encountered in previous studies of Ca, Sr, Ba and Co diffusion in basalt. To explain the constant D value near the liquidus, we speculate that the structure of the melt changes as a function of temperature in such a way that the normal temperature dependence of the diffusivity is compensated. For example, the rare earth ions may be displaced from their (high temperature) octahedral coordination sites to other sites where they are more readily dissociated and therefore become progressively more mobile. The behavior below 1210°C may be the result of relatively stable complexes or molecules in the melt or of the formation of a REE bearing crystalline phase that has so far escaped detection. Preliminary results for Eu diffusion in obsidian are D (Eu, 800°C) = 5 × 10?13 cm2 s?1 and D (Eu, 950°C) = 1.5 × 10?11 cm2 s?1. These data are consistent with an activation energy of 59 Kcal mole?1. These low diffusivities indicate that the partitioning of REE in crystallizing intermediate and acidic melts may be controlled by diffusion in the melt rather than equilibrium between the crystal surface and the bulk melt.The diffusion data are applied to partial melting in the mantle, in an attempt to explain how LREE enriched tholeiites may be derived from a LREE depleted mantle source. In this model LREE diffuse from garnet bearing regions that have small melt fractions into garnet free regions that have relatively large melt fractions. REE diffusion is so slow that this process is quantitatively significant only in small partially molten bodies (diameter ～1 km or less) or in larger, but strongly flattened bodies. Internal convective motion during diapiric rise would also increase the efficiency of the process.  相似文献   

8.
Synthetic melilites on the join Ca2MgSi2O7 (åkermanite) — Ca2FeSi2O7 (iron åkermanite) with Fe/(Fe+Mg) from 0.0 to 0.7 exhibit, at room temperature, an incommensurate phase with a rectangular modulation of a wavelength of about 19 Å in the [110] direction. Upon increase of temperature, they transform to a commensurate melilite structure at about 80° C for Fe/(Fe+Mg)=0.0 and about 250° C for Fe/(Fe+Mg)=0.6. In addition to the T(2) positions of the melilite structure filled by Si, the incommensurate phase exhibits two distinguishable T(1) sites containing the Mg and Fe2+. These two sites merge into one site during the phase transition from the incommensurate to the commensurate phase. A structural model for the incommensurate phase is based on the misfit between the tetrahedral (Mg, Fe2+)Si2O 7 4? sheets and the Ca2+ ions.  相似文献   

9.
Subsolidus marginal zoning in calcium-poor clinopyroxenes and intermediate zoning in discontinuously zoned subcalcic- to calcium-rich clinopyroxenes from ironrich igneous rocks is used to calculate the interdiffusion coefficient, DCa?(Fe,Mg), parallel to the crystallographic caxis. Wagner's mathematical models describing the displacement of interfaces in solids as the result of isothermal diffusion are adopted. The steady-state heat flow equation is used to approximate the diffusion times. The calculated interdiffusion coefficients are of a reasonable order of magnitude, viz. 6.0×10?20?2.0×10?17cm2· sec?1 at about 900° C.  相似文献   

10.
The thermal expansion of gehlenite, Ca2Al[AlSiO7], (up to T=830 K), TbCaAl[Al2O7] (up to T=1100 K) and SmCaAl[Al2O7] (up to T=1024 K) has been determined. All compounds are of the melilite structure type with space group Thermal expansion data were obtained from in situ X-ray powder diffraction experiments in-house and at HASYLAB at the Deutsches Elektronen Synchrotron (DESY) in Hamburg (Germany). The thermal expansion coefficients for gehlenite were found to be: α1=7.2(4)×10−6×K−1+3.6(7)×10−9ΔT×K−2 and α3=15.0(1)×10−6×K−1. For TbCaAl[Al2O7] the respective values are: α1=7.0(2)×10−6×K−1+2.0(2)×10−9ΔT×K−2 and α3=8.5(2)×10−6×K−1+2.0(3)×10−9ΔT×K−2, and the thermal expansion coefficients for SmCaAl[Al2O7] are: α1=6.9(2)×10−6×K−1+1.7(2)×10−9ΔT×K−2 and α3=9.344(5)×10−6×K−1. The expansion mechanisms of the three compounds are explained in terms of structural trends obtained from Rietveld refinements of the crystal structures of the compounds against the powder diffraction patterns. No structural phase transitions have been observed. While gehlenite behaves like a ‘proper’ layer structure, the aluminates show increased framework structure behavior. This is most probably explained by stronger coulombic interactions between the tetrahedral conformation and the layer-bridging cations due to the coupled substitution (Ca2++Si4+)–(Ln 3++Al3+) in the melilite-type structure. This article has been mistakenly published twice. The first and original version of it is available at .  相似文献   

11.
Electron transport properties of single crystal and polycrystalline natural mineral galena (PbS) samples from the Trep?a mine, Yugoslavia, were determined using the photoacoustic frequency transmission technique. Their thermal diffusivity (D T≈0.16 × 10?5 m2 s?1), the coefficient of diffusion (D between 0.15×10?2 0.16×10?2 m2 s?1) and lifetime of the excess carrier (τ≈35 μs and the front and rear recombination velocity (s g≈65.5 m s?1 and s b≈66.4 m s?1, respectively), were calculated by comparing the experimental results and the theoretical photoacoustic amplitude and phase signals. The lattice parameter obtained by X-ray work was a?=5.936?Å. The free carrier concentration of these single-crystal samples was measured using the Hall method (N?=?3×1018 cm?3). Measurements of the optical reflectivity of the same samples, as a function of wavelength, in the infrared and far infrared ranges, were performed. In the far infrared range a free electron plasma frequency was observed and numerically analyzed, using the least-squares fitting procedure. The values of optical parameters were calculated and the value of the free carrier concentration obtained by the Hall method was confirmed.  相似文献   

12.
The dissolution of chrysotile is studied in regard to the surfaces analysis by photoelectron spectrometry. After leaching of chrysotile (Provenance: Thetford; about 200 mg of fibers of 1 cm length) in nonstirred 0.1 N oxalic conditions, the composition of the mineral surfaces is determined by XPS; kinetic curves of dissolution are given in the range 22–80°C. Two conditions for the rate-limiting step are involved for the explanation of the dissolution: diffusion of Mg2+ through the fibrous gel or dissociation of chrysotile. By the former, some values of the diffusion coefficient are proposed: D varies from 5·10?19 cm2s?1 to 5·10?16 cm2s?1, in the range 22–80°C. By the second model, the leaching rate is estimated from 3 Å (22°C) per h to 250 Å (80°C) per h. For the 2 models, the activation heat energy is in the range 15–20 Kcal.  相似文献   

13.
Previous studies have suggested that the extraction of copper by hydroxyoxime extractants involves mass transfer with chemical reaction. This paper reports the results of experiments where an aqueous copper solution (4.94 g dm?3 copper, 5.26 g dm?3 H2SO4) is contacted with a 5% v/v LIX 64N solution in Escaid 100, in a diffusion cell with a stagnant interface. The concentration-distance distribution of the diffusional band of copper complex which appeared in the organic phase was measured at various times, and the results can be modelled by equations based on diffusion about an interface with and without interfacial resistance.If the previously measured diffusion constants for copper in the aqueous and organic phases were used in the model, then an unrealistically high resistance (200,000–300,000 s cm?1) would have to be chosen to obtain a correlation. If a low resistance (1,000 s cm?1) is assumed and the previously measured diffusion constants for copper in the aqueous phase (5.2·10?6 cm2 s?1) and copper in the organic phase (5.0·10?6 cm2 s?1) are taken, then it is necessary to reduce the organic phase diffusion constant to 2·10?6 cm2 s?1 to obtain correlation of the model with the data. It is proposed that as the organic product film develops, the diffusivity of the copper complex is reduced.  相似文献   

14.
The kinetics of zoned garnet porphyroblast growth is exemplified in a sample of garnet-staurolite-biotite schist from the northern Ladoga region. The diffusion-controlled porphyroblast growth was accompanied by a decrease in the kinetic coefficient during phase reactions. Even at insignificant (1–2°C) thermal overstepping, the leading role of diffusion as a factor that controls kinetics of porphyroblast growth in medium-grade metapelites is consistent with the parameters of metamorphic crystallization: T = 500–650°C, t = 1 Ma; D A1 app = 10?14 cm2/s, L = 0.2–0.6 cm, r = 1–3 mm, ΔC Al = 1.5 × 10?4–1.5 × 10?3 mol/cm3.  相似文献   

15.
The thermal expansion of gehlenite, Ca2Al[AlSiO7], (up to T=830 K), TbCaAl[Al2O7] (up to T=1,100 K) and SmCaAl[Al2O7] (up to T=1,024 K) has been determined. All compounds are of the melilite structure type with space group Thermal expansion data was obtained from in situ X-ray powder diffraction experiments in-house and at HASYLAB at the Deutsches Elektronen Synchrotron (DESY) in Hamburg (Germany). The thermal expansion coefficients for gehlenite were found to be: α1=7.2(4)×10−6 K−1+3.6(7)×10−9ΔT K−2 and α3=15.0(1)×10−6 K−1. For TbCaAl[Al2O7] the respective values are: α1=7.0(2)×10−6 K−1+2.0(2)×10−9ΔT K−2 and α3=8.5(2)×10−6 K−1+2.0(3)×10−9ΔT K−2, and the thermal expansion coefficients for SmCaAl[Al2O7] are: α1=6.9(2)× 10−6 K−1+1.7(2)×10−9ΔT K−2 and α3=9.344(5)×10−6 K−1. The expansion-mechanisms of the three compounds are explained in terms of structural trends obtained from Rietveld refinements of the crystal structures of the compounds against the powder diffraction patterns. No structural phase transitions have been observed. While gehlenite behaves like a ’proper’ layer structure, the aluminates show increased framework structure behaviour. This is most probably explained by stronger coulombic interactions between the tetrahedral conformation and the layer-bridging cations due to the coupled substitution (Ca2++Si4+)-(Ln 3++Al3+) in the melilite-type structure. Electronic Supplementary Material Supplementary material is available for this article at  相似文献   

16.
Colin H. Donaldson 《Lithos》1975,8(2):163-174
Concentration gradients in glass adjacent to skeletal olivines in a DSDP basalt have been examined by electron probe. The glass is depleted in Mg, Fe, and Cr and enriched in Si, Al, Na, and Ca relative to that far from olivine. Ionic diffusion coefficients for the glass compositions are calculated from temperature, ionic radius and melt viscosity, using the Stokes-Einstein relation. At 1170°C, the diffusion coefficient of Mg2+ ions in the basalt is 4·5.10?9 cm2/s. Comparison with measured diffusion coefficients in a mugearite suggests this value may be 16 times too small. The concentration gradient data and the diffusion coefficients are used to calculate instantaneous olivine growth rates of 2–6.10?7 cm/s. This is too slow for olivine to have grown in situ during quenching. Growth necessarily preceded emplacement such that the composition of the crystals plus the enclosing glass need not be that of a melt. The computed olivine growth rates are compatible with the rate of crystallization deduced for the Skaegaard intrusion.  相似文献   

17.
Single crystals of (Ca1–xSrx)2MgSi2O7 slightly doped with 1000 ppm Mn2+ and with x ranging from 0.04 to 0.32 were grown from the melt in a mirror furnace applying the Czochalski technique. Transmission electron microscopy (TEM) revealed incommensurately modulated structures at room-temperature for all compositions in accordance with earlier studies by electron paramagnetic resonance (EPR). Electron diffraction patterns clearly show satellite reflections typical for two-dimensional modulation, and their successive destabilization with increasing Sr content. The modulation is of tartan-like appearance. Beyond a Sr/(Sr+Ca) ratio of about 0.32 the synthesis of stable solid solution åkermanite type crystals was proved not to be feasible, indicating the existence of a miscibility gap in the Sr åkermanite system. As presumed from the diffuse scattering around the satellite reflections, and suggested more conclusively by crystallographic processing of high resolution EM images the Sr ions incorporated into the incommensurate crystal phase are distributed in an ordered fashion and are partly adapted to the displacive modulation of the pure åkermanite. This means, occupational modulation even makes a contribution to the overall modulation characteristics in (Ca1–xSrx)2 MgSi2O7.  相似文献   

18.
The diffusivities of network-forming cations (Si4+, Al3+, Ge4+ and Ga3+) in melts of the jadeitic composition NaAl(Si, Ge)2O6 and Na(Al, Ga)Si2O6 have been measured at pressures between 6 and 20 kbar at 1400°C. The rates of interdiffusion of Si4+-Ge4+ and Al3+-Ge3+ increase with increasing pressure at constant temperature. The results are consistent with the ion-dynamics computer simulations of Jadeite melt by Angellet al. (1982, 1983). The coefficient measured for the Si4+-Ge4+ interdiffusion is between 8 × 10?10 and 2.5 × 10?8cm2sec at 6 kbar, depending on the composition of the melt, whereas at 20 kbar it is between 7 × 10?9 and 2 × 10?7cm2sec. The effect of pressure is greater for more Si-rich compositions (i.e., closer to NaAlSi2O6 composition). The coefficient measured for the Al3+-Ga3+ inter- diffusion is between 9 × 10?10 and 3 × 10?9 cm2/sec at 6 kbar and between 3 × 10?9 and 1 × 10?8cm2sec at 20 kbar. The rate of increase in diffusivity with pressure of Al3+-Ga3+ (a factor of 3–4) is smaller than that of Si4+-Ge4+ (a factor of 7–17).The Si4+-Ge4+ interdiffusion in melts of Na2O · 4(Si, Ge)O2 composition has also been measured at 8 and 15 kbar for comparison. The effect of pressure on the diffusivity in this melt is significantly smaller than that for the jadeitic melts. The increase in diffusivity of the network-forming cations in jadeitic melts with increasing pressure may be related to the decrease in viscosity of the same melt. The present results, as well as the ion-dynamics simulations, suggest that the homogenization of partial melts and mixing of magmas would be more efficient at greater depths.  相似文献   

19.
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20.
The gaseous state and chemical inert behavior of radon make it important tracer for the radon transport study through the building materials. The radon resistant property of building construction materials is important parameter to control the indoor radon levels in living and workplaces. The materials with higher radium content can be made less severe by the use of some building materials of low diffusion coefficient and diffusion length. This makes the study of radon diffusion through building material more important along with the study of exhalation and radioactivity content. Keeping this in mind the radon diffusion study was carried out through different building construction materials used for wall and floor by active and passive techniques. The diffusion coefficient from these building materials measured by passive methods varied from (0.9 ± 0.5) × 10?7 to (22.95 ± 13.19) × 10?6 m2s?1 and radon diffusion length varied from 0.21 to 3.31 m for cement, soil, sand, wall putty and plaster of Paris (POP) etc. The radon diffusion coefficient measured by active technique varied from 1.93 × 10?10 to 1.36 × 10?7 m2s?1 for samples with definite geometry like paper, polyethylene, marble, granite etc. The radon diffusion coefficient and diffusion length depend upon the porosity and density of materials for powder samples.  相似文献   

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