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Tunable Manipulation of Mineral Carbonation Kinetics in Nanoscale Water Films via Citrate Additives

机译:通过柠檬酸盐添加剂对纳米级水膜中矿物碳酸化动力学的调控

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摘要

We explored the influence of a model organic ligand on mineral carbonation in nanoscale interfacial water films by conducting five time-resolved in situ X-ray diffraction (XRD) experiments at 50 °C. Forsterite was exposed to water-saturated supercritical carbon dioxide (90 bar) that had been equilibrated with 0–0.5 m citrate (C_(6)H_(5)O_(7)~(–3)) solutions. The experimental results demonstrated that greater concentrations of citrate in the nanoscale interfacial water film promoted the precipitation of magnesite (MgCO_(3)) relative to nesquehonite (MgCO_(3)·3H_(2)O). At the highest concentrations tested, magnesite nucleation and growth were inhibited, lowering the carbonation rate constant from 9.1 × 10~(–6) to 3.6 × 10~(–6) s~(–1). These impacts of citrate were due to partial dehydration of Mg~(2+)(aq) and the adsorption of citrate onto nuclei and magnesite surfaces. This type of information may be used to predict and tailor subsurface mineralization rates and pathways.
机译:我们通过在50°C下进行五个时间分辨的原位X射线衍射(XRD)实验,探索了模型有机配体对纳米级界面水膜中矿物碳酸化的影响。镁橄榄石暴露于水饱和的超临界二氧化碳(90 bar)中,该溶液已用0–0.5 m柠檬酸盐(C_(6)H_(5)O_(7)〜(–3))溶液平衡。实验结果表明,相对于Neshonhonite(MgCO_(3)·3H_(2)O),纳米级界面水膜中柠檬酸盐的较高浓度促进了菱镁矿(MgCO_(3))的沉淀。在最高测试浓度下,菱镁矿的成核和生长受到抑制,碳化速率常数从9.1×10〜(–6)降低到3.6×10〜(–6)s〜(–1)。柠檬酸盐的这些影响归因于Mg〜(2 +)(aq)的部分脱水以及柠檬酸盐在核和菱镁矿表面的吸附。此类信息可用于预测和调整地下矿化速率和途径。

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  • 来源
    《Environmental Science & Technology》 |2018年第12期|7138-7148|共11页
  • 作者单位

    Department of Geology and Geophysics, University of Wyoming, 1000 E. University Avenue, Laramie, Wyoming 82071, United States;

    Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, P.O. Box 999, MS K8-98, Richland, Washington 99352, United States;

    Department of Geology and Geophysics, University of Wyoming, 1000 E. University Avenue, Laramie, Wyoming 82071, United States,School of Energy Resources, University of Wyoming, 1000 E. University Avenue, Laramie, Wyoming 82071, United States;

    Shanghai Advanced Research Institute, Chinese Academy of Sciences, Pudong Xinqu, Shanghai, China 201203;

    Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, P.O. Box 999, MS K8-98, Richland, Washington 99352, United States;

    Energy and Environment Directorate, Pacific Northwest National Laboratory, P.O. Box 999, MS K8-98, Richland, Washington 99352, 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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  • 正文语种 eng
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