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Dynamics of Magnesite Formation at Low Temperature and High pCO_2 in Aqueous Solution

机译:低温高浓度pCO_2水溶液中菱镁矿形成动力学。

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摘要

Magnesite precipitation from aqueous solution, despite conditions of supersaturation, is kinetically hindered at low temperatures for reasons that remain poorly understood. The present study examines the products of Mg(OH)_2 reaction in solutions saturated with supercritical CO_2 at high pressures (90 and 110 atm) and low temperatures (35 and 50 ℃). Solids characterization combined with in situ solution analysis reveal that the first reaction products are the hydrated carbonates hydromagnesite and nesquehonite, appearing simultaneously with brucite dissolution. Magnesite is not observed until it comprises a minor product at 7 days reaction at 50 ℃. Complete transition to magnesite as the sole product at 35 ℃ (135 days) and at a faster rate at 50 ℃ (56 days) occurs as the hydrated carbonates slowly dissolve under the slightly acidic conditions generated at high pCO_2. Such a reaction progression at high pCO_2 suggests that over long term the hydrated Mg- carbonates functioned as intermediates in magnesite formation. These findings highlight the importance of developing a better understanding of the processes expected to occur during CO_2 storage. They also support the importance of integrating magnesite as an equilibrium phase in reactive transport calculations of the effects of CO_2 sequestration on geological formations at long time scale.
机译:尽管存在过饱和条件,但从水溶液中菱镁矿沉淀在动力学上仍然受阻,原因尚不清楚。本研究研究了在高压(90和110 atm)和低温(35和50℃)下超临界CO_2饱和溶液中Mg(OH)_2反应的产物。固体表征与原位溶液分析相结合显示,第一个反应产物是水合碳酸盐水菱镁矿和水镁石,与水镁石溶解同时出现。菱镁矿直到在50℃下反应7天才形成次要产物时才观察到菱镁矿。由于水合碳酸盐在高pCO_2产生的弱酸性条件下缓慢溶解,因此在35℃(135天)以50℃(56天)以更快的速度完全转变成菱镁矿。在高pCO_2下的这种反应进程表明,从长远来看,水合碳酸镁碳酸盐可作为菱镁矿形成的中间体。这些发现突出了对更好地理解CO_2储存过程中预期发生的过程的重要性。他们还支持将菱镁矿整合为平衡相的重要性,这是在很长的时间内对二氧化碳固存对地质构造的影响的反应输运计算中。

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  • 来源
    《Environmental Science & Technology》 |2015年第17期|10736-10744|共9页
  • 作者单位

    Pacific Northwest National Laboratory, P.O. Box 999, MS K8-96, Richland, Washington 99352, United States;

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

    Pacific Northwest National Laboratory, P.O. Box 999, MS K8-96, Richland, Washington 99352, United States;

    Pacific Northwest National Laboratory, P.O. Box 999, MS K8-96, Richland, Washington 99352, United States;

    The Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    The Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States;

    Pacific Northwest National Laboratory, P.O. Box 999, MS K8-96, Richland, Washington 99352, United States,Washington State University, Pullman, Washington 99164, 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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