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The dependence of albite feldspar dissolution kinetics on fluid saturation state at acid and basic pH: Progress towards a universal relation

机译:钠长石长石溶解动力学对在酸性和碱性pH下流体饱和状态的依赖性:通用关系的进展

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摘要

Here we report on two separate ongoing, multi-year investigations on the dependence of the dissolution rate (R) of albite feldspar on fluid saturation state, as defined by the Gibbs free energy of reaction (△G_r) for dissolution. The investigations are based on dissolution at pH 9.2,150 ℃ and pH 3.3,100 ℃. Both studies reveal that the R-△G_r relation is highly nonlinear and sigmoidal. The kinetic data from the first study, being the most complete, can be fitted with a sigmoidal rate curve that is composed of two separate, parallel rate laws that represent distinct mechanisms of dissolution. The switch between one dominant mechanism and the other may be controlled by a critical free energy. The fact that in both studies the same type of sigmoidal R-△G_r relation exists for dissolution at different pH and temperature condition suggests that this behavior may be universal for albite and other feldspars. Moreover, the experimental data contradict the commonly used R-△G_r relation that is loosely based on transition state theory (TST). This has important implications with respect to the accuracy of geochemical codes that model water-rock interactions at near-equilibrium conditions.
机译:在这里,我们报告了关于钠长石长石溶解速率(R)对流体饱和状态的依赖性的两个单独的,正在进行的,为期多年的研究,这取决于溶解的吉布斯反应自由能(△G_r)。研究基于pH 9.2,150℃和pH 3.3,100℃下的溶出度。两项研究都表明,R-△G_r关系是高度非线性和S形的。来自最先研究的动力学数据是最完整的,可以拟合为S形曲线,该曲线由两个独立的平行速率定律组成,代表了不同的溶出机理。一个主要机制与另一个主要机制之间的切换可以通过临界自由能控制。在两项研究中,在不同的pH和温度条件下均存在相同类型的S型R-△G_r关系以溶解的事实表明,这种行为对于钠长石和其他长石可能是普遍的。此外,实验数据与通常基于过渡状态理论(TST)松散使用的R-△G_r关系矛盾。这对于在接近平衡条件下模拟水-岩相互作用的地球化学法规的准确性具有重要意义。

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  • 来源
    《Comptes rendus》 |2010年第8期|P.676-684|共9页
  • 作者单位

    Environmental Geochemistry, LGIT, CNRS UMR C5559, University of Grenoble 1, OSUG, BP 53X, 38041 Grenoble cedex 9, France;

    rnCNRS UMR 8538, laboratoire de geologie, Ecole normale superieure de Paris, 24, rue Lhomond, 75231 Paris cedex 05, FrancernInstitut de physique du globe de Paris, centre de recherches sur le stockage geologique du CO_2, 4, place Jussieu, 75005 Paris, France;

    Environmental Geochemistry, LGIT, CNRS UMR C5559, University of Grenoble 1, OSUG, BP 53X, 38041 Grenoble cedex 9, France;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    feldspar; albite; dissolution; kinetic rate laws; gibbs free energy; water-rock interaction; CO_2 sequestration;

    机译:长石钠长石解散动率定律;吉布斯自由能水岩相互作用;固存CO_2;

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