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281.
Damien Daval Roland Hellmann Delphine Tisserand François Guyot 《Geochimica et cosmochimica acta》2010,74(9):2615-5525
Measurements of the dissolution rate of diopside (r) were carried out as a function of the Gibbs free energy of the dissolution reaction (ΔGr) in a continuously stirred flow-through reactor at 90 °C and pH90 °C = 5.05. The overall relation between r and ΔGr was determined over a free energy range of −130.9 < ΔGr < −47.0 kJ mo1−1. The data define a highly non-linear, sigmoidal relation between r and ΔGr. At far-from-equilibrium conditions (ΔGr ? −76.2 kJ mo1−1), a rate plateau is observed. In this free energy range, the rates of dissolution are constant, independent of [Ca], [Mg] and [Si] concentrations, and independent of ΔGr. A sharp decrease of the dissolution rate (∼1 order of magnitude) occurs in the transition ΔGr region defined by −76.2 < ΔGr ? −61.5 kJ mo1−1. Dissolution closer to equilibrium (ΔGr > −61.5 kJ mo1−1) is characterised by a much weaker inverse dependence of the rates on ΔGr. Modeling the experimental r-ΔGr data with a simple classical transition state theory (TST) law as implemented in most available geochemical codes is found inappropriate. An evaluation of the consequences of the use of geochemical codes where the r-ΔGr relation is based on basic TST was carried out and applied to carbonation reactions of diopside, which, among other reactions with Ca- and Mg-bearing minerals, are considered as a promising process for the solid state sequestration of CO2 over long time spans. In order to take into account the actual experimental r-ΔGr relation in the geochemical code that we used, a new module has been developed. It reveals a dramatic overestimation of the carbonation rate when using a TST-based geochemical code. This points out that simulations of water-rock-CO2 interactions performed with classical geochemical codes should be evaluated with great caution. 相似文献
282.
Internal architecture of a till sheet,Tiskilwa Formation,north‐central Illinois,USA: Application of architectural element analysis
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Jessica M. Slomka Carolyn H. Eyles Riley P. M. Mulligan Edward Donald Mckay III Richard C. Berg 《Sedimentology》2015,62(5):1328-1359
Thick till sheets deposited during the Quaternary form significant aquitards in many areas of North America. However, the detailed sedimentary heterogeneity and architecture and depositional history of till units are not well understood. This study utilizes architectural element analysis to delineate the internal sedimentary architecture of the Tiskilwa Formation exposed at two outcrop sections in north‐central Illinois, USA. Architectural element analysis facilitates systematic delineation of sedimentary architecture based on the nature of facies contacts and change in facies associations, delineation of unit geometries and understanding of depositional processes at different scales of resolution; making architectural element analysis suitable for the sedimentological analysis and palaeoenvironmental reconstruction of subglacial deposits. Eleven facies types are identified in this study, including sand, gravel and diamict facies that record a suite of subglacial depositional processes. Detailed analysis of facies contacts (bounding surface hierarchy) and change in facies associations allows the delineation of five architectural elements, including coarse‐grained lens, coarse‐grained sheet, mixed zone, diamict lens and diamict sheet elements. The spatial arrangement and genetic interpretation of elements, and their spatial relationship with fifth‐order bounding surfaces, allows the delineation of five larger scale architectural units (‘element associations’), which can be mapped in the local study area and record at least three stacked successions of meltwater accumulation and till deposition. The results of this study can be utilized for architectural analysis of till sheets and provide insight to groundwater flow pathways through till in the study area and elsewhere. 相似文献