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首页> 外文期刊>Water resources research >Influence of porosity structures on mixing-induced reactivity at chemical equilibrium in mobile/immobile Multi-Rate Mass Transfer (MRMT) and Multiple INteracting Continua (MINC) models
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Influence of porosity structures on mixing-induced reactivity at chemical equilibrium in mobile/immobile Multi-Rate Mass Transfer (MRMT) and Multiple INteracting Continua (MINC) models

机译：流动/不动多速率传质（MRMT）和多重相互作用连续体（MINC）模型中孔隙结构对化学平衡下混合诱导的反应性的影响

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摘要

Trapping mechanisms and slow diffusion in poorly connected porosities are well modeled by several anomalous transport models including the Multi-Rate Mass Transfer framework (MRMT). In MRMT, solutes in fast mobile advective zones are slowed down by first-order exchanges with immobile zones. While MRMT models have been used essentially for conservative transport, we investigate their relevance to reactive transport. To this end, we analyze the influence of the structure of the diffusive porosity zone on the distribution of concentrations within the immobile zone and on the reactivity of simple precipitation/dissolution bimolecular reactions at equilibrium. We build Multi-Rate Mass Transfer (MRMT) and Multiple INteracting Continua (MINC) models with equivalent transport characteristics. Both models have the same mobile zone concentrations at any time. They, however, differ by the connectivity structure of their immobile zones. MRMT has a star-shaped connectivity structure with the mobile zone linked to all immobile zones and acting as the sole exchanger. MINC has a chained-type connectivity where immobile zones are mutually connected on a line. We show that both connectivity structures give the same concentration variance whatever the model parameters, dimensionality, and initial conditions. Reaction rates of bimolecular reaction at chemical equilibrium are also highly similar but not equal as long as concentration gradients within the diffusive zone remain low like in the uniform injection case, or at large times when high initial concentration gradients have been reduced. For high initial immobile concentration gradients in the diffusive zone, however, reaction rates are much lower in the star-shaped connectivity structure (MRMT), and consequently depend on the organization of the immobile porosity structure. Negative concentrations also occur in some of the immobile zones of the equivalent MRMT as a result of the direct connection of the mobile and immobile zones. While acceptable for conservative components, negative concentrations limit the relevance of MRMT to model reactivity at high immobile concentration gradients. The concept of immobile zone concentration should thus be taken with great care and systematically be assessed.
机译：包括多速率传质框架（MRMT）在内的几种异常输运模型很好地模拟了圈闭不良孔隙中的圈闭机制和缓慢扩散。在MRMT中，快速流动对流区中的溶质因与静止区的一阶交换而减慢了速度。虽然MRMT模型已基本上用于保守运输，但我们研究了它们与反应性运输的相关性。为此，我们分析了扩散孔隙区的结构对固定区内浓度分布以及平衡时简单沉淀/溶解双分子反应的反应性的影响。我们建立具有相同传输特性的多速率传质（MRMT）和多个交互连续体（MINC）模型。两种型号随时都有相同的移动区域浓度。但是，它们的固定区域的连接结构不同。 MRMT具有星形连接结构，其移动区域链接到所有固定区域并充当唯一交换器。 MINC具有链式连接，其中固定区域在一条线上相互连接。我们表明，无论模型参数，尺寸和初始条件如何，这两种连通性结构均具有相同的浓度方差。在化学平衡时，双分子反应的反应速率也非常相似，但不相等，只要在扩散区内的浓度梯度保持不变（如均匀注入情况下），或者在较大的时候已经降低了较高的初始浓度梯度。但是，对于扩散区中较高的初始固定浓度梯度，星形连接结构（MRMT）中的反应速率要低得多，因此取决于固定孔隙结构的组织。由于可移动区域和不可移动区域的直接连接，在等效MRMT的某些不可移动区域中也会出现负浓度。尽管可以接受保守成分，但负浓度限制了MRMT在高固定浓度梯度下模拟反应性的相关性。因此，应格外注意固定区域集中的概念，并对其进行系统地评估。

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  • 来源
    《Water resources research》 |2013年第12期|8511-8530|共20页
  • 作者

    J.-R. de Dreuzy; A. Rapaport; T. Babey; J. Harmand;

  • 作者单位

    Geosciences Rennes, UMR CNRS 6118, Campus de Beaulieu, Universite de Rennes 1, FR-35042 Rennes CEDEX, France,Institute of Environmental Analysis and Water Studies, CSIC, Barcelona, Spain;

    UMR 729 INRA SupAgro MISTEA, Montpellier, France,EPI INRA INRIA MODEMIC, Sophia-Antipolis, France;

    Geosciences Rennes, UMR CNRS 6118, Campus de Beaulieu, Rennes,France;

    EPI INRA INRIA MODEMIC, Sophia-Antipolis, France,INRA-LBE, UR 0050, Avenue des etangs, Narbonne, France;

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