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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Formation of zinc carbonate phases on dissolving calcite, aragonite, and vaterite in acidic aqueous solutions

Calcium carbonate (CaCO 3 ) minerals serve as a major sink to retain metal ions through mineral-water interfacial reactions in which the capacity and long-term stability of contaminant uptake are influenced by coupled dissolution and precipitation reactions of both primary and secondary carbonate minerals (i.e., mineral replacement). Notably, recent studies of calcite reactivity in acidic solutions containing high levels of metal ions demonstrated complex behavior under conditions of sustained disequilibrium. Here, we explored the reactivity of three CaCO 3 polymorphs (calcite, aragonite, and vaterite) with acidic Zn 2+ -containing aqueous solutions using a suite of imaging techniques including optical and scanning electron microscopies, synchrotron-based micro X-ray fluorescence, and transmission X-ray microscopy. Zn uptake by calcite occurred through a two-step process: the formation of a thin layer of the zinc precipitate on the substrate surface followed by the growth of fibrous and radiating hydrozincite particles from the layer. In contrast, Zn uptake by aragonite occurred by mineral replacement where the secondary Zn carbonate phase preserved the external morphology of the original crystal (i.e., a pseudomorph). The replacement of vaterite by hydrozincite occurred within the confined space beneath the porous shell of vaterite, signifying that the primary mechanism driving Zn carbonate precipitation was chemical exchange through the pores. When multiple CaCO 3 polymorphs coexisted, the replacement of aragonite and vaterite occurred preferentially over that of calcite. These results demonstrate the distinct morphological and mineralogical controls over the reactivities of calcium carbonate minerals with Zn 2+ under acidic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Evaluating the role of re-adsorption of dissolved Hg 2+ during cinnabar dissolution using isotope tracer technique

Cinnabar dissolution is an important factor controlling mercury (Hg) cycling. Recent studies have suggested the co-occurrence of re-adsorption of the released Hg during the course of cinnabar dissolution. However, there is a lack of feasible techniques that can quantitatively assess the amount of Hg re-adsorbed on cinnabar when investigating cinnabar dissolution. In this study, a new method, based on isotope tracing and dilution techniques, was developed to study the role of Hg re-adsorption in cinnabar dissolution. The developed method includes two key components: (1) accurate measurement of both released and spiked Hg in aqueous phase and (2) estimation of re-adsorbed Hg on cinnabar surface via the reduction in spiked 202 Hg 2+ . By adopting the developed method, it was found that the released Hg for trials purged with oxygen could reach several hundred g L –1 , while no significant cinnabar dissolution was detected under anaerobic condition. Cinnabar dissolution rate when considering Hg re-adsorption was approximately 2 times the value calculated solely with the Hg detected in the aqueous phase. Lastly, these results suggest that ignoring the Hg re-adsorption process can significantly underestimate the importance of cinnabar dissolution, highlighting the necessity of applying the developed method in future cinnabar dissolution studies.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2015

Effects of increased upward flux of dissolved salts caused by CO2 storage or other factors

Injection of CO2 in deep saline aquifers is being considered to reduce greenhouse gases in the atmosphere, and this process is expected to increase the pressure in these deep aquifers. One potential consequence of pressurization is an increase in the upward flux of saline water. Saline groundwater occurs naturally at shallow depths in many sedimentary basins, so an upward flux of solutes could degrade the quality of freshwater aquifers and threaten aquatic ecosystems. One problem could occur where saline water flowed upward along preferential paths, like faults or improperly abandoned wells. Diffuse upward flow through the natural stratigraphy could also occur in response to basin pressurization. This process would be slower, but diffuse upward flow could affect larger areas than flow through preferential paths, and this motivated us to evaluate this process. We analyzed idealized 2D and 3D geometries representing the essential details of a shallow, freshwater aquifer underlain by saline ground water in a sedimentary basin. The analysis was conducted in two stages, one that simulated the development of a freshwater aquifer by flushing out saline water, and another that simulated the effect of a pulse-like increase in the upward flux from the basin. The results showed that increasing the upward flux from a basin increased the salt concentration and mass loading of salt to streams, and decrease the depth to the fresh/salt transition. The magnitude of these effects varied widely, however, from a small, slow process that would be challenging to detect, to a large, rapid response that could be an environmental catastrophe. The magnitude of the increased flux, and the initial depth to the fresh/salt transition in groundwater controlled the severity of the response. We identified risk categories for salt concentration, mass loading, and freshwater aquifer thickness, and we used these categories to characterize the severity of the response. This showed that risks would likely be minor if the upward flux was smaller than a few tenths of the magnitude of recharge, according to the 2D analyses. The 3D analyses also show that upward flux could occur without a significant increase in the risk categories. The major contribution of this work is that it shows how a large increase in diffuse upward flux from a basin could cause significant problems, but a small increase in upward flux may occur without significantly affecting risks to the shallow freshwater flow system. This heightens the importance of understanding interactions between shallow and deep hydrologic systems when characterizing CO2 storage projects.

54 ENVIRONMENTAL SCIENCES↗