Mineralogical Heterogeneity Controls Dissolution-Front Instability and Reactive-Transport Scaling in Porous Media

IF 2.6 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ACS Earth and Space Chemistry Pub Date : 2026-10-15 Epub Date: 2026-09-23 DOI:10.1021/acsearthspacechem.6c00200
Kai Li, Ran Hu, Zhibing Yang, Yi-Feng Chen
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Abstract

Mineral dissolution in multicomponent porous media involves coupled mineral–water reactions, solute transport, and evolving pore topology. However, most continuum reactive-transport models still rely on constitutive relations developed for single-mineral media, and the influence of insoluble mineral phases remains poorly understood. Here, we use three-dimensional pore-scale reactive transport simulations to investigate how the insoluble mineral fraction affects dissolution patterns and the evolution of hydraulic and reactive properties. Mineralogical heterogeneity has regime-dependent effects on dissolution-front stability. At relatively low Péclet numbers, moderate insoluble mineral fractions enhance concentration heterogeneity and promote wormholing, whereas larger fractions disrupt connected reactive pathways and suppress flow focusing. At relatively high Péclet numbers, insoluble phases monotonically weaken preferential channel development and drive dissolution toward a more uniform pattern. Mineralogical heterogeneity also alters permeability evolution. As the insoluble mineral fraction increases, the permeability–porosity relationship becomes progressively more linear in log–log space and approaches a power-law form, while the maximum permeability–porosity exponent decreases and shows a converging trend. We further find that the reactive surface area and bulk dissolution rate can be described by empirical porosity-based relationships, which remain consistent across the tested Péclet numbers, Damköhler numbers, and random mineral distributions. These results improve our understanding of dissolution processes in mineralogically heterogeneous porous media and provide empirical relationships for continuum-scale reactive transport modeling.

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矿物非均质性控制着多孔介质中溶解锋不稳定性和反应输运结垢
矿物在多组分多孔介质中的溶解涉及到矿物-水耦合反应、溶质输运和孔隙拓扑结构的演化。然而,大多数连续介质反应输运模型仍然依赖于单矿物介质的本构关系,而不溶性矿物相的影响仍然知之甚少。在这里,我们使用三维孔隙尺度的反应输运模拟来研究不溶性矿物组分如何影响溶解模式以及水力和反应性质的演变。矿物学非均质性对溶蚀前缘稳定性具有制度依赖效应。在相对较低的psamclet数下,中等不溶性矿物组分增强了浓度的非均质性并促进了虫孔形成,而较大的组分则破坏了连接的反应途径并抑制了流动聚焦。在相对较高的passiclet数下,不溶相单调地削弱了优先通道的发展,并推动溶解向更均匀的模式发展。矿物非均质性也改变渗透率演化。随着不溶性矿物分数的增加,渗透率-孔隙度关系在对数-对数空间上逐渐线性化,接近幂律形式,而最大渗透率-孔隙度指数减小并呈收敛趋势。我们进一步发现,反应表面积和整体溶解速率可以用基于经验孔隙度的关系来描述,这些关系在测试的psamcletnumber, Damköhler number和随机矿物分布中保持一致。这些结果提高了我们对矿物学上非均质多孔介质溶解过程的理解,并为连续尺度反应输运模型提供了经验关系。
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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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