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首页> 外文期刊>Environmental Science & Technology >Impacts of Diffusive Transport on Carbonate Mineral Formation from Magnesium Silicate-CO_2-Water Reactions
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Impacts of Diffusive Transport on Carbonate Mineral Formation from Magnesium Silicate-CO_2-Water Reactions

机译：扩散运输对硅酸镁-CO_2-水反应碳酸盐矿物形成的影响

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摘要

Reactions of CO_2 with magnesium silicate minerals to precipitate magnesium carbonates can result in stable carbon sequestration. This process can be employed in ex situ reactors or during geologic carbon sequestration in magnesium-rich formations. The reaction of aqueous CO_2 with the magnesium silicate mineral forsterite was studied in systems with transport controlled by diffusion. The approach integrated bench-scale experiments, an in situ spectroscopic technique, and reactive transport modeling. Experiments were performed using a tube packed with forsterite and open at one end to a CO_2-rich solution. The location and amounts of carbonate minerals that formed were determined by postexperiment characterization of the solids. Complementing this ex situ characterization, ~(13)C NMR spectroscopy tracked the inorganic carbon transport and speciation in situ. The data were compared with the output of reactive transport simulations that accounted for diffusive transport processes, aqueous speciation, and the forsterite dissolution rate. All three approaches found that the onset of magnesium carbonate precipitation was spatially localized about 1 cm from the opening of the forsterite bed. Magnesite was the dominant reaction product. Geochemical gradients that developed in the diffusion-limited zones led to locally supersaturated conditions at specific locations even while the volume-averaged properties of the system remained undersaturated.
机译：CO_2与硅酸镁矿物的反应生成碳酸镁沉淀可导致稳定的碳固存。此过程可用于异地反应堆或富镁地层的地质固碳过程中。在扩散受扩散控制的体系中研究了CO_2水溶液与镁镁硅酸盐镁橄榄石的反应。该方法整合了实验室规模的实验，原位光谱技术和反应性传输模型。使用装有镁橄榄石的试管进行实验，该试管的一端向富含CO_2的溶液敞开。形成的碳酸盐矿物的位置和数量由固体的实验后表征确定。作为这种非原位表征的补充，〜（13）C NMR光谱跟踪了无机碳的原位迁移和形成。将该数据与反应性运输模拟的输出进行比较，后者解释了扩散性运输过程，水溶液形态和镁橄榄石的溶解速率。所有这三种方法都发现，碳酸镁沉淀的开始在空间上距镁橄榄石床的开口约1 cm。菱镁矿是主要的反应产物。即使在系统的体积平均性质仍然不饱和的情况下，在扩散受限区域中形成的地球化学梯度也会在特定位置导致局部过饱和状态。

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  • 来源
    《Environmental Science & Technology》 |2014年第24期|14344-14351|共8页
  • 作者

    Daniel E. Giammar; Fei Wang; Bin Guo; J. Andrew Surface; Catherine A. Peters; Mark S. Conradi; Sophia E. Hayes;

  • 作者单位

    Department of Energy, Environmental and Chemical Engineering, Washington University, St. Louis, Missouri 63130, United States;

    Department of Energy, Environmental and Chemical Engineering, Washington University, St. Louis, Missouri 63130, United States;

    Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, United States;

    Department of Chemistry, Washington University, St. Louis, Missouri 63130, United States,PPG, Pittsburgh, Pennsylvania;

    Department of Civil and Environmental Engineering, Princeton University, Princeton, New Jersey 08544, United States;

    Department of Chemistry, Washington University, St. Louis, Missouri 63130, United States;

    Department of Chemistry, Washington University, St. Louis, Missouri 63130, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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