Browsing by Subject "geochemistry"
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Item An Investigation of Linked Physical And Biogeochemical Processes In Heterogeneous Soils In The Vadose Zone(2012-10-19) Hansen, David JosephChemical dynamics in the vadose zone are poorly understood due to the transient nature of chemical and hydrologic conditions, but are nonetheless critical to understanding contaminant fate and transport. This work explored the effects of soil structure (i.e. layers, lenses) on linked geochemical, hydrological, and microbiological processes under changing hydrologic conditions (e.g. rainfall, introduction of groundwater, and fluctuating water table heights). A homogenized medium-grained sand, homogenized organic-rich loam and a sand-over-loam layered column were constructed for the first series of experiments. The second series of experiments employed two soil columns with lenses that were packed identically with sterilized and untreated sediments. Each consisted of two lenses of organic-rich loam in a medium-grained sand matrix. Lenses were located at different vertical depths and were horizontally offset. In-situ collocated probes collected soil hydrologic and chemical data. In the layered column, enhanced biogeochemical cycling was observed over the texturally homogeneous soil columns. Enumerations of Fe(III) and SO42- reducing microorganisms also show 1-2 orders of magnitude greater community numbers in the layered column. The greatest concentrations of aqueous FeS clusters (FeSaq) were observed in close proximity to the soil interface. To our knowledge, this was the first documentation of FeSaq in partially saturated sediments. Mineral and soil aggregate composite layers were also most abundant near the soil layer interface; the presence of which, likely contributed to an order of magnitude decrease of hydraulic conductivity. In the live lens column, Fe-oxide bands formed at the fringes of the lenses that retarded water flow rates by an order of magnitude compared to the sterilized column. Microbial activity also produced insoluble gases and that led to the creation of a separate gas phase that reduced hydraulic conductivity. This limited the interaction between groundwater with soil-pore waters that led to the formation of geochemically distinct water masses in relatively close proximity to one another. No such changes were observed in the sterilized column. When compared to homogenous columns, the presence of soil heterogeneities altered biogeochemical and hydrologic processes considerably which highlights the need to consider soil heterogeneity in contaminant fate and transport models. These findings suggest that quantifying coupled hydrologic-biogeochemical processes occurring at small scale soil interfaces is critical to accurately describing and predicting chemical changes at the larger system scale.Item Lead Isotopic Variations of the Pacific and Implications for Paleogene Water Mass Composition(2013-11-13) Subt, CristinaTo understand the effects changes in the meridional overturning circulation (MOC) played on past climate we need to determine where convection occurred. The late Cretaceous and early Paleogene interval (~75 to 35 Ma) was characterized by low meridional temperature gradients. Nd isotopes indicate high-latitude convection in the Pacific Ocean during this interval, with deep waters mixing in the tropical Pacific. Here we investigate the evolution of the Pb isotopic composition of water masses in the Pacific to constrain variability in weathering inputs into the inferred convection regions from ~75 to 35 Ma. We generated ^(206),^(207),^(208)Pb/^(204)Pb isotope records for North Pacific DSDP and ODP Sites 192, 464, and 883, and South Pacific DSDP Sites 323, 463, and 596. South Pacific deep waters increasing in contributions. Pb composition in the subtropical South Pacific also suggests a stronger influence of dust dissolution whereas the Nd composition was dominated by water mass composition. North Pacific Pb values may also have reflected shifting sources during the EECO. The Pb and Nd composition at Site 883 shows a short radiogenic excursion in Pb values ~40 Ma, possibly cased by a short period of strengthened North Pacific Deep Water (NPDW) influence on the isotopic composition during the Mid-Eocene Climatic Optimum (MECO). ^(206)Pb/2^(04)Pb trends differ from ^(207),^(208)Pb/^(204)Pb values, which typically show similar trends to each other?resulting from the mixing of multiple Pb sources. North Pacific sites typically exhibit relatively lower Pb compositions than South Pacific, and evidence from detrital analyses suggests sources of Pb to North Pacific sites received strong contributions of continental dust. Pb and Nd are coupled in North Pacific sites between ~62 and 50 Ma, as well as in the Southern Ocean throughout the study period, indicating the Pb composition in this region was influenced by the composition of advected deep water masses. North Pacific sites also show decoupling of Pb and Nd ~50 Ma, during the Early Eocene Climatic Optimum (EECO), which may be indicative of more distal