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61.
In this study, the speciation of Zn2+, Pb2+, and Cu2+ ions sorbed at the calcite surface was monitored during a 2.5-year reaction period, using extended X-ray absorption spectroscopy to characterize metal speciation on the molecular scale. Experiments were performed using pre-equilibrated calcite-water suspensions of pH 8.3, at metal concentrations below the solubility of metal hydroxide and carbonate precipitates, and at constant metal surface loadings. The EXAFS results indicate that all three metals remained coordinated at the calcite surface as inner-sphere adsorption complexes during the 2.5-year ageing period, with no evidence to suggest slow formation of dilute metal-calcite solid solutions under the reaction conditions employed. All three divalent metals were found to form non-octahedral complexes upon coordination to the calcite surface, with Zn2+ adsorbing as a tetrahedral complex, Cu2+ as a Jahn-Teller distorted octahedral complex, and Pb2+ coordinating as a trigonal- or square-pyramidal surface complex. The non-octahedral configurations of these surface complexes may have hindered metal transfer from the calcite surface into the bulk, where Ca2+ is in octahedral coordination with respect to first-shell O. The use of pre-equilibrated calcite suspensions, with no net calcite dissolution or precipitation, likely prevented metal incorporation into the lattice as a result of surface recrystallization. The results from this study imply that ageing alone does not increase the stability of Zn2+, Pb2+, and Cu2+ partitioning to calcite if equilibrium with the solution is maintained during reaction; under these conditions, these metals are likely to remain available for exchange even after extended sorption times.  相似文献   
62.
The last British-Irish Ice Sheet (BIIS) created a landscape with many sedimentary basins that preserve archives of paleoenvironmental and paleoclimatic change during the Last Glacial-Interglacial Transition (LGIT; ~ 18-8 ka BP). The typical lithostratigraphic succession of these archives is composed of minerogenic/allogenic sediments formed during cold climatic conditions and organic-rich/authigenic sediments during warmer climates. This paper presents a multi-core lithostratigraphy compiled from the extant lake and surrounding basin at Llangorse Lake, south Wales, a basin lying within the southernmost limits of the last BIIS. This lake contains one of the longest continuous terrestrial sediment successions in the UK. Uncertainty previously existed concerning the presence and distribution of sediments at the site related to the Windermere Interstadial (~ 14.7 to ~ 12.9 ka BP) and Loch Lomond Stadial (~ 12.9 to 11.7 ka BP). A new borehole survey demonstrates that LGIT-age sediments are present at the site with nekron mud (gyttja), corresponding to the Lateglacial Interstadial, deposited in the deeper part of the lake waters and that these deposits are equivalent in age to marl deposits found at shallower depths at the margins of the basin. These deposits are associated with warmer conditions experienced during the Windermere Interstadial and Holocene, whilst minerogenic-rich sediments were deposited during the colder climatic conditions of the Dimlington Stadial and the Loch Lomond Stadial with rangefinder radiocarbon dates confirming this attribution. A model of lake level changes shows that drainage of the Dimlington Stadial glacial lake caused the largest fall, but there was also a further, smaller lake level fall at the end of the Windermere Interstadial and/or the start of the Loch Lomond Stadial, before the level rose in the early Holocene. The lithostratigraphic results presented here form the framework for further paleoenvironmental and paleoclimatic research at Llangorse Lake.  相似文献   
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64.
Forsmark in Sweden has been proposed as the site of a geological repository for spent high-level nuclear fuel, to be located at a depth of approximately 470 m in fractured crystalline rock. The safety assessment for the repository has required a multi-disciplinary approach to evaluate the impact of hydrogeological and hydrogeochemical conditions close to the repository and in a wider regional context. Assessing the consequences of potential radionuclide releases requires quantitative site-specific information concerning the details of groundwater flow on the scale of individual waste canister locations (1–10 m) as well as details of groundwater flow and composition on the scale of groundwater pathways between the facility and the surface (500 m to 5 km). The purpose of this article is to provide an illustration of multi-scale modeling techniques and the results obtained when combining aspects of local-scale flows in fractures around a potential contaminant source with regional-scale groundwater flow and transport subject to natural evolution of the system. The approach set out is novel, as it incorporates both different scales of model and different levels of detail, combining discrete fracture network and equivalent continuous porous medium representations of fractured bedrock.  相似文献   
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