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首页> 外文期刊>Environmental Science & Technology >Distinctive Reactivities at Biotite Edge and Basal Planes in the Presence of Organic Ligands: Implications for Organic-Rich Geologic CO_2 Sequestration
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Distinctive Reactivities at Biotite Edge and Basal Planes in the Presence of Organic Ligands: Implications for Organic-Rich Geologic CO_2 Sequestration

机译：有机配体存在下黑云母边缘和基底平面的独特反应性：对富含有机物的地质CO_2固存的意义

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摘要

To better understand how scCO_2-saturated brine-mineral interactions can affect safe and efficient geologic CO_2 sequestration (GCS), we studied the effects of organic ligands (acetate and oxalate) on biotite dissolution and surface morphological changes. The experimental conditions were chosen to be relevant to GCS sites (95 ℃ and 102 atm CO_2). Quantitative analyses of dissolution differences between biotite edge and basal planes were made. Acetate slightly inhibited biotite dissolution and promoted secondary precipitation. The effect of acetate was mainly pH-induced aqueous acetate speciation and the subsequent surface adsorption. Under the experimental conditions, most of acetate exists as acetic acid and adsorbs to biotite surface Si and Al sites, thereby reducing their release. However, oxalate strongly enhanced biotite dissolution and induced faster and more significant surface morphology changes by forming bidentate mononuclear surface complexes. For the first time, we show that oxalate selectively attacks edge surface sites and enhances biotite dissolution. Thus, oxalate increases the relative reactivity ratio of biotite edge surfaces to basal surfaces, while acetate does not impact this relative reactivity. This study provides new information on reactivity differences at biotite edge and basal planes in the presence of organic ligands, which has implications for safe CO_2 storage in organic-rich sites.
机译：为了更好地理解scCO_2饱和的盐水与矿物之间的相互作用如何影响安全有效的地质CO_2隔离（GCS），我们研究了有机配体（乙酸盐和草酸盐）对黑云母溶解和表面形态变化的影响。选择与GCS位置有关的实验条件（95℃和102 atm CO_2）。定量分析了黑云母边缘和基面之间的溶出度差异。醋酸盐略微抑制黑云母溶解并促进二次沉淀。乙酸盐的影响主要是pH引起的乙酸盐水溶液形态和随后的表面吸附。在实验条件下，大多数乙酸盐以乙酸形式存在，并吸附到黑云母表面的Si和Al位点，从而减少了它们的释放。然而，草酸盐通过形成双齿单核表面复合物，大大增强了黑云母的溶解，并引起更快，更重要的表面形态变化。首次，我们表明草酸盐选择性攻击边缘表面部位并增强黑云母溶解。因此，草酸盐增加了黑云母边缘表面与基底表面的相对反应性比率，而乙酸盐不影响该相对反应性。这项研究提供了有关在有机配体存在的情况下黑云母边缘和底面反应性差异的新信息，这对于在富含有机物的地点安全存储CO_2具有影响。

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  • 来源
    《Environmental Science & Technology》 |2015年第16期|10217-10225|共9页
  • 作者

    Lijie Zhang; Young-Shin Jun;

  • 作者单位

    Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Campus Box 1180, St. Louis, Missouri 63130, United States;

    Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, One Brookings Drive, Campus Box 1180, 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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