(690e) Synergistic Computational and Experimental Investigation of MOF-Enhanced Mixed-Matrix Membranes for Advanced Gas Separation

In the pursuit of sustainable gas separation technologies, membrane-based systems stand out for their potential to offer energy-efficient alternatives to conventional methods. Specifically, mixed-matrix membranes (MMMs), which mix inorganic fillers with polymer matrices, have been identified as a key strategy for overcoming the inherent selectivity-permeability trade-off found in conventional polymeric membranes. In this context, metal-organic frameworks (MOFs), with their tunable pore architecture and site-specific interaction capabilities, emerge as an ideal candidate to enhance MMM performance. Given the theoretical complexities associated with studying the interactions at the MOF-polymer interface in MMMs, this research is dedicated to the computational exploration of gas transport where MOFs and polymers meet within MMMs. Specifically, our focus is on the detailed examination of how propane and propylene gases pass through this interface, with the goal of enhancing our comprehension of these critical processes to better-understand the propane-propylene selectivity exhibited in zeolitic imidazolate framework-8 (ZIF-8) incorporating membranes.

This study utilizes density functional theory (DFT) and climbing image nudged elastic band (CI-NEB) calculations to examine the interactions between ZIF-8 and the 6FDA-DAM polymer models at their interfaces. Through this analysis, we delve into how the electronic and structural details at these interfaces influence the transport of gas molecules across the polymer/MOF interface in MMMs. By comparing our computational results with experimental transport data, we highlight the critical role of MOF/polymer interface interactions in gas separations, particularly focusing on the separation of propane and propylene. Ultimately, our research provides valuable insights into the molecular interactions within MMMs, offering a significant contribution to the development of advanced materials aimed at more sustainable and effective gas separation technologies.