Unlocking the Secrets of Liquid–Liquid Interfaces and Phase Equilibria: Exploring the Interplay of Critical Composition, Interfacial Tension, and Mutual Solubility

This study reveals pivotal insight into liquid-liquid interfaces by demonstrating that the interface composition mirrors that at the critical point. This revelation leads to the formulation of a novel liquid-liquid distribution law and thermodynamic inequality, establishing a direct connection between mutual solubility values and critical compositions. While particularly accurate for regular solutions, the findings exhibit substantial reliability in nonregular systems, supported by experimental data on binary and ternary mixtures. Importantly, the study illustrates that, with known critical compositions, interfacial tension data alone are sufficient for calculating mutual solubilities, providing a practical alternative for assessing molecular solubility. The paper further showcases the versatility of the simple bottle-testing (cloud-testing) method, effectively serving as both a tensiometer and a mutual-solubility meter. This method utilizes established critical composition data to predict the compositions and interfacial tension of coexisting phases concurrently, offering a cost-effective alternative to complex analytical techniques. As a notable outcome, given critical compositions, basic laboratory equipment such as a beaker and a syringe can equivalently function as both a tensiometer and a mutual solubility detector (e.g., GC). The paper also discusses the application of this method in understanding the liquid-liquid phase behavior in biological systems, exemplified by biomolecular condensates or Lewy bodies.