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微尺度混沌混合作为多孔介质中化学反应的驱动力。

Microscale Chaotic Mixing as a Driver for Chemical Reactions in Porous Media.

机构信息

Géosciences Rennes, Université de Rennes, UMR CNRS 6118, 263 Avenue du Général Leclerc, F-35042 Rennes, France.

École Nationale Supérieure de Chimie, Université de Rennes, UMR CNRS 6226, 11 Allée de Beaulieu, F-35708 Cedex 7 Rennes, France.

出版信息

Environ Sci Technol. 2024 May 21;58(20):8899-8908. doi: 10.1021/acs.est.3c09749. Epub 2024 May 6.

Abstract

Mixing-induced reactions play a key role in a large range of biogeochemical and contaminant transport processes in the subsurface. Fluid flow through porous media was recently shown to exhibit chaotic mixing dynamics at the pore scale, enhancing microscale concentration gradients and controlling mixing rates. While this phenomenon is likely ubiquitous in environmental systems, it is not known how it affects chemical reactions. Here, we use refractive index matching and laser-induced fluorescence imaging of a bimolecular redox reaction to investigate the consequence of pore scale chaotic mixing on the reaction rates. The overestimation of measured reaction rates by the classical macrodispersion model highlights the persistence of incomplete mixing on the pore scale. We show that the reaction product formation is controlled by microscale chaotic mixing, which induces an exponential increase of the mixing interface and of the reaction rates. We derive a reactive transport model that captures experimental results and predicts that chaotic mixing has a first order control on reaction rates across a large range of time scales and Péclet and Damköhler numbers. These findings provide a new framework for understanding, assessing, and predicting mixing-induced reactions and their role on the fate and mobility of environmental compounds in natural porous media.

摘要

混合诱导反应在地下环境中广泛的生物地球化学和污染物输运过程中起着关键作用。最近的研究表明,多孔介质中的流体流动在孔隙尺度上表现出混沌混合动力学,增强了微观浓度梯度并控制了混合速率。虽然这种现象在环境系统中可能普遍存在,但尚不清楚它如何影响化学反应。在这里,我们使用折射率匹配和双分子氧化还原反应的激光诱导荧光成像来研究孔隙尺度混沌混合对反应速率的影响。经典的宏观弥散模型高估了测量的反应速率,这突出表明在孔隙尺度上不完全混合仍然存在。我们表明,反应产物的形成受到微尺度混沌混合的控制,这导致混合界面和反应速率呈指数增长。我们推导了一个反应输运模型,该模型可以捕捉实验结果并预测混沌混合对反应速率具有一级控制作用,跨越了很大的时间尺度和 Peclet 和 Damköhler 数范围。这些发现为理解、评估和预测混合诱导反应及其在天然多孔介质中环境化合物的命运和迁移中的作用提供了一个新的框架。

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