This grant provides funding for a synergistic program of combinatorial experiments, molecular simulations, and theoretical modeling aimed at making advances in the design of pervaporation membrane materials. Pervaporation is an energy-friendly process for separation of liquid mixtures that works by preferentially transporting one of the liquid components across a selective membrane into the vapor phase on the other side. Molecular insights regarding structure-function relationships in membrane materials will be obtained by studying water-alcohol separation as the model application. The work will focus on crosslinked polyacrylate copolymer membranes that offer a high degree of tunability in chemical composition compared to traditional silicone-based membranes. High-throughput experimental screening methods consisting of matrix-based sample preparation and testing of membrane properties will be combined with molecular simulations of water and alcohol diffusion rates to quantify membrane performance. Through data-driven validation, a novel theoretical framework for membrane performance will be developed, providing predictive capabilities for rapid design of pervaporation membranes for separation applications.