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41.
We present molecular orbital/density functional theory (MO/DFT) calculations that predict a greater isotopic fractionation in redox reactions than in reactions involving ligand exchange. The predicted fractionation factors, reported as 1000·ln(56-54α), associated with equilibrium between Fe-organic and Fe-H2O species were <1.6‰ in vacuo and <1.2‰ in solution when the oxidation state of the system was held constant. These fractionation factors were significantly smaller than those predicted for equilibrium between different oxidation states of Fe, for which 1000·ln(56-54α) was >2.7‰ in vacuo and >2.2‰ in solution when the bound ligands were unchanged. The predicted 56Fe/54Fe ratio was greater in complexes containing Fe3+ and in complexes with shorter Fe-O bond lengths; both of these trends follow previous theoretical results. Our predictions also agree with previous experimental measurements that suggest that the largest biological fractionations will be associated with processes that change the oxidation state of Fe, and that identification of biologically controlled Fe isotope fractionation may be difficult when abiotic redox fractionations are present in the system. The models studied here also have important implications for future theoretical isotope calculations, because we have discovered the necessity of using vibrational frequencies instead of reduced masses when predicting reduced partition functions in aqueous-phase species. 相似文献
42.
James D. Prikryl 《Geochimica et cosmochimica acta》2008,72(18):4508-4520
The dissolution and growth of uranophane [Ca(UO2)2(SiO3OH)2·5H2O] have been examined in Ca- and Si-rich test solutions at low temperatures (20.5 ± 2.0 °C) and near-neutral pH (∼6.0). Uranium-bearing experimental solutions undersaturated and supersaturated with uranophane were prepared in matrices of ∼10−2 M CaCl2 and ∼10−3 M SiO2(aq). The experimental solutions were reacted with synthetic uranophane and analyzed periodically over 10 weeks. Interpretation of the aqueous solution data permitted extraction of a solubility constant for the uranophane dissolution reaction and standard state Gibbs free energy of formation for uranophane ( kJ mol−1). 相似文献
43.
If a magma is a hybrid of two (or more) isotopically distinctend-members, at least one of which is partially crystalline,separation of melt and crystals after hybridization will leadto the development of isotopic heterogeneities in the magmaas long as some of the pre-existing crystalline material (antecrysts)retains any of its original isotopic composition. This holdstrue whether the hybridization event is magma mixing as traditionallyconstrued, bulk assimilation, or melt assimilation. Once a magma-scaleisotopic heterogeneity is formed by crystal–melt separation,it is essentially permanent, persisting regardless of subsequentcrystallization, mixing, or equilibration events. The magnitudeof the isotopic variability resulting from crystal–meltseparation can be as large as that resulting from differentialcontamination, multiple isotopically distinct sources, or insitu isotopic evolution. In one model, a redistribution of one-thirdof the antecryst cargo yielded a crystal-enriched sample with87Sr/86Sr of 0·7058, whereas the complementary crystal-poorsample has 87Sr/86Sr of 0·7068. In other models, crystal-richsamples are enriched in radiogenic Sr. Isotopic heterogeneitiescan be either continuous (controlled by the modal distributionof crystals and melt) or discontinuous (when there is completeseparation of crystals and liquid). The first case may be exemplifiedby some isotopically zoned large-volume rhyolites, formed bythe eruptive inversion of a modally zoned magma chamber. Inthe latter case, the isotopic composition of any (for example)interstitial liquid will be distinct from the isotopic compositionof the bulk crystal fraction. The separation of such an interstitialliquid may explain the presence of isotopically distinct late-stageaplites in plutons. Crystal–melt separation provides anadditional option for the interpretation of isotopically zonedor heterogeneous magmas. This option is particularly attractivefor systems whose chemical variation is otherwise explicableby fractionation-dominated processes. Non-isotopic chemicalheterogeneities can also develop in this fashion. KEY WORDS: isotopic heterogeneity; zoning; hybrid magma; crystal separation; Sr isotopes; aplite; rhyolite 相似文献
44.
There are few inter-African country urban analyses because of the continent’s enormous size and socioeconomic diversity, language barriers, and wide variations in national and regional urban research capacity. Nevertheless, comparative urban studies are critical in understanding contemporary African urbanization. In this comparative spatial and temporal analysis of Ghana and Kenya’s urbanization, we find that both countries are urbanizing rapidly and are faced with many common urban problems. Moreover, Ghana is more urbanized than Kenya and has a larger indigenous urban imprint and a more widely dispersed urban pattern. Besides their physiographic and population conditions, we trace these countries’ convergent and divergent urban trends to their shared but unique experiences of colonialism, nationalism and globalization. 相似文献
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Summary In order to interpret the observed features of pressure records produced by waves from large explosions in the earth's atmosphere, the writers have obtained numerical solutions of the homogeneous equations governing acoustic-gravity wave propagation in a stratified compressible fluid. Theoretical dispersion curves and variations of perturbation kinetic energy with altitude are presented for 11 normal modes. It is shown that the step-like character of the phase velocity curves in the velocity-period plane can be interpreted as being the result of interference between two families of normal modes-«quasi-horizontal modes» representing energy propagation in the lower atmosphere (below the ozonosphere) and «quasi-vertical modes» representing energy propagation in the upper atmosphere (above the ozonosphere). The theoretical prediction that several normal modes contribute to the observed barogram traces is verified by Fourier analysis of a number of wave records.Lamont Geological Observatory Contribution No. 611. — This research was supported by National Science Foundation Grant NSF-G-11997, Office of Naval Research Contract Nonr 266 (70), and National Science Foundation Grant NSF-GP-550. — Part of this research was done at the NASA Institute for Space Studies, New York, N. Y. 相似文献
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48.
Lucas G. Adamson Donald W. Quigley H. Ross Ainsworth George V. Chilingar 《Engineering Geology》1966,1(6):451-459
Most previous studies and applications of electrochemical stabilization of soils through electroosmosis have been made on clayey soils. The object of this investigation was to find out if relatively small amounts of clay (1.5%–3.5%, by weight) present in a sandy soil would be enough for stabilization and strengthening to be possible. The results indicate increases of cohesion of the order of 100–200 lb./sq.ft. X-ray analyses of treated soils indicate that sheet structures of clays are reduced and silicates destroyed upon treatment by electroosmosis. Newly-formed minerals also cement the soil. These neoformations include gibbsite, limonite, calcite, hydrohematite, hydrogoethite (hydrolepidocrocite), hisingerite, allophane, allophanoid, gypsum, hematite, magnetite, nontronite, trona and natron (Na2 CO3, 10H2O). The process seems to be irreversible. 相似文献
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50.