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首页> 外文期刊>Environmental Science & Technology >In Situ Natural Abundance ~(17)O and ~(25)Mg NMR Investigation of Aqueous Mg(OH)_2 Dissolution in the Presence of Supercritical CO_2
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In Situ Natural Abundance ~(17)O and ~(25)Mg NMR Investigation of Aqueous Mg(OH)_2 Dissolution in the Presence of Supercritical CO_2

机译：超临界CO_2存在下Mg（OH）_2水溶液的原位自然丰度〜（17）O和〜（25）Mg NMR研究

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摘要

We report an in situ high-pressure NMR capability that permits natural abundance ~(17)O and ~(25)Mg NMR characterization of dissolved species in aqueous solution and in the presence of supercritical CO_2 fluid (scCO_2). The dissolution of Mg(OH)_2 (brucite) in a multiphase water/scCO_2 fluid at 90 atm pressure and 50 ℃ was studied in situ, with relevance to geological carbon sequestration. ~(17)O NMR spectra allowed identification and distinction of various fluid species including dissolved CO_2 in the H_2O-rich phase, scCO_2 aqueous H_2O, and HCO_3~-. The widely separated spectral peaks for various species can all be observed both dynamically and quantitatively at concentrations as low as 20 raM. Measurement of the concentrations of these individual species also allows an in situ estimate of the hydrogen ion concentration, or pC_H~+ values, of the reacting solutions. The concentration of Mg~(2+) can be observed by natural abundance ~(25)Mg NMR at a concentration as low as 10 mM. Quantum chemistry calculations of the NMR chemical shifts on cluster models aided in the interpretation of the experimental results. Evidence for the formation of polymeric Mg~(2+) clusters at high concentrations in the H_2O-rich phase, a possible critical step needed for magnesium carbonate formation, was found.
机译：我们报告了原位高压NMR能力，允许在水溶液中和存在超临界CO_2流体（scCO_2）的情况下，溶解物的自然丰度〜（17）O和〜（25）Mg NMR表征。研究了Mg（OH）_2（微晶石）在90atm压力和50℃下在多相水/ scCO_2流体中的溶解情况，这与地质碳固存有关。 〜（17）O NMR光谱可以识别和区分各种流体，包括富H_2O相中溶解的CO_2，scCO_2 H_2O水溶液和HCO_3-。在低至20 raM的浓度下，可以动态和定量地观察到各种物种的广泛分离的光谱峰。通过测量这些单个物质的浓度，还可以就地估算出反应溶液中的氢离子浓度或pC_H〜+值。 Mg〜（2+）的浓度可以通过低至10 mM的自然丰度〜（25）Mg NMR来观察。簇模型上NMR化学位移的量子化学计算有助于解释实验结果。发现在富H_2O相中高浓度下形成聚合Mg〜（2+）团簇的证据，这是碳酸镁形成所需的可能关键步骤。

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  • 来源
    《Environmental Science & Technology》 |2016年第22期|12373-12384|共12页
  • 作者

    Mary Y. Hu; Xuchu Deng; K. Sahan Thanthiriwatte; Virgil E. Jackson; Chuan Wan; Odeta Qafoku; David A. Dixon; Andrew R. Felmy; Kevin M. Rosso; Jian Zhi Hu;

  • 作者单位

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Department of Chemistry, The University of Alabama, Shelby Hall, Tuscaloosa, Alabama 35487, United States;

    Department of Chemistry, The University of Alabama, Shelby Hall, Tuscaloosa, Alabama 35487, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Department of Chemistry, The University of Alabama, Shelby Hall, Tuscaloosa, Alabama 35487, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Pacific Northwest National Laboratory, Richland, Washington 99354, 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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