Understanding the interaction between multiphase flow and reactive transport in porous media is critical for many environmental and industrial applications. When a nonwetting immiscible phase is present within the pore space, it can remain immobile, which we call unsaturated flow, or move, resulting in multiphase flow. Previous studies under unsaturated flow conditions have shown that, for a given flow rate, the product of a mixing-driven reaction increases as wetting phase saturation decreases. Conversely, the opposite effect is observed for a given Péclet number (i.e., the flow rate is adapted depending on the wetting phase saturation). However, the impact of multiphase flow dynamics on mixing-driven reactions is poorly understood due to experimental and numerical challenges. To assess the impact of multiphase flow conditions on product formation, we use an optimized chemiluminescence reaction and an experimental setup that allows the separate injection of reactants along with a stationary two-phase flow. In our experiments, the mass of the reaction product under stationary two-phase flow conditions increases faster than Fickian beyond the diffusive time. The global kinetics initially increase before experiencing a monotonic decrease with significant fluctuations caused by the displacement of the nonwetting phase. For a given flow rate of the wetting phase, product formation depends on the flow rate of the nonwetting immiscible phase.

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http://dx.doi.org/10.1021/acs.est.4c09449DOI Listing

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