The Hele-Shaw–Cahn–Hilliard model, coupled with phase separation, is numerically simulated to demonstrate the formation of anomalous fingering patterns in a radial displacement of a partially miscible binary-fluid system. The composition of injected fluid is set to be less viscous than the displaced fluid and within the spinodal or metastable phase-separated region, in which the second derivative of the free energy is negative or positive, respectively. Because of phase separation, concentration evolves non-monotonically between the injected and displaced fluids. The simulations reveal four areas of the concentration distribution between the fluids: the inner core; the low-concentration grooves/high-concentration ridges; the isolated fluid fragments or droplets; the mixing zone. The grooves/ridges and the fragments/droplets, which are the unique features of phase separation, form in the spinodal and metastable regions. Four typical types of patterns are categorized: core separation (CS); fingering separation (FS); separation fingering (SF); lollipop fingering, in the order of the dominance of phase separation, respectively. For the patterns of CS and FS, isolated fluid fragments or droplets around the inner core are the main features. Fingering formation is better maintained with droplets in the SF pattern if the phase separation is relatively weaker than viscous fingering (VF). Even continuous fingers are well preserved in the case of dominant VF; phase separation results in lollipop-shaped fingers. The evolving trend of the patterns is in line with the experiments. These patterns are summarized in a pattern diagram, mainly by the magnitude of the second derivative of the free energy profile.

Viscous fingering or Saffman–Taylor instability shows fingering interfacial patterns when a more mobile fluid displaces a less mobile one in porous media. The effective interfacial tension (EIT) is like capillary force, acting at the miscible interface on time scales shorter than interface relaxation. It has been numerically reported so far that the fingers are wider with EIT compared with those without EIT. A recent experiment observed finger widening with increasing flow rate in a miscible system with EIT, which is not observed in classical immiscible and miscible systems. In this study, we have numerically investigated the effect of $Pe$ (which corresponds to the injection flow rates in the experiment) on miscible viscous fingering with/without EIT. We have shown that the fingers are monotonically thinner with an increase in $Pe$ in the system without EIT, while finger widening with increasing $Pe$ is observed in the system with EIT. Furthermore, we have also examined a one-dimensional underlying concentration profile and EIT profile by using a one-dimensional diffusion–convection model because EIT is proportional to the squared concentration gradient. We have then shown that the concentration gradient is steeper and, thus, the EIT is larger as $Pe$ is larger. Therefore, this is the first numerical study that can theoretically verify finger widening with increasing flow rate, which occurs only in a miscible system with EIT to the extent of our targeting EIT values, and explain the mechanism by one-dimensional analysis.

We develop coupled evolution equations for viscous fingering (VF) and phase separation in partially miscible systems by combining a simple double-well thermodynamic free energy and Korteweg force with a classical miscible VF model for a binary system. The VF pattern transition into a droplet formation pattern by the spinodal decomposition effect is demonstrated, and the simultaneous increases in the depth of the energy minimum, in the difference in the equilibrium concentrations, and in the Korteweg force, enhance the droplet growth. The pattern's interfacial length increases with the spinodal decomposition effects. These results match the corresponding experimental results.

Classical viscous fingering (VF) instability, the formation of finger-like interfacial patterns, occurs when a less viscous fluid displaces a more viscous one in porous media in immiscible and fully miscible systems. However, the dynamics in partially miscible fluid pairs, exhibiting a phase separation due to its finite solubility into each other, has not been largely understood so far. This study has succeeded in experimentally changing the solution system from immiscible to fully miscible or partially miscible by varying the compositions of the components in an aqueous two-phase system (ATPS) while leaving the viscosities relatively unchanged at room temperature and atmospheric pressure. Here, we have experimentally discovered a new topological transition of VF instability by performing a Hele-Shaw cell experiment using the partially miscible system. The finger formation in the investigated partially miscible system changes to the generation of spontaneously moving multiple droplets. Through additional experimental investigations, we determine that such anomalous VF dynamics is driven by thermodynamic instability such as phase separation due to spinodal decomposition and Korteweg convection induced by compositional gradient during such phase separation. We perform the numerical simulation by coupling hydrodynamics with such chemical thermodynamics and the spontaneously moving droplet dynamics is obtained, which is in good agreement with the experimental investigations of the ATPS. This numerical result strongly supports our claim that the origin of such anomalous VF dynamics is thermodynamic instability.