Impact of pore-scale chaotic mixing on Darcy-scale reaction rates

Abstract: Prediction of reactive transport in porous media remains challenging when pore scale incomplete mixing is at play. Previous experimental studies investigated chemical reactions in porous media by visualizing reaction product or reactants mostly in uniform flow. However, the local reaction rate, which is necessary to infer mechanisms of reaction in pore space, could not be obtained without considering transport of reaction products and reactants. Thus, the interpretation remained elusive. We visualized the reaction rate field using chemiluminescnece within index-matched 3D porous media under zero acceleration and constant acceleration flow fields to investigate how pore scale chaotic mixing and Darcy scale fluid acceleration rectify reactive transport. We found that the reaction rate kept increasing from upstream to downstream in constant acceleration field, whereas it increased only at the upstream zone in zero acceleration field. The ratio of dispersion rate and size of the mixing interface determined such an effect of acceleration. Moreover, the experimental results showed stronger dependency of reaction rate on velocity compared to the numerical simulations that assume complete mixing in pore space. To explain this, we suggested the mechanistic model that includes the pore scale folding of lamellae due to chaotic mixing and the pore scale concentration gradients against compression. Such a pore scale mechanism was consistent with the experimentally observed change in reaction rate over the space. These results give new insights on underlying mechanisms of reactive transport in porous media.