Membranes Incorporating 2D Single-Crystalline COFs for Superior Separation Performance: 3D Image-Informed Reactive Force Field Modeling and Scalable Mixed-Matrix Systems
Jasasmita Das, Yun Kyung Shin, Beatrice Bartolomei, Caleb Johannesmeyer, Gabriel T. dos Santos, Michael L. Barsoum, Roberto dos Reis, Vinayak P. Dravid, Adri C. T. van Duin, William R. Dichtel, Katie D. Li-OakeyAbstract
Bridging atomically precise materials design with scalable membrane manufacturing remains a central challenge in separation science. Two-dimensional covalent organic frameworks (2D COFs) offer tunable porosity and chemistry, but poor crystallinity and processability have limited their performance in membranes. Here we demonstrate that incorporating single-crystalline 2D COFs into anodic aluminum oxide supports and scalable mixed-matrix membrane enables exceptional separation performance, achieving ultrahigh permeance (MMM-SC-0.6: 8764 and 4531 L m–2 h–1 bar–1 for hexane and methanol, respectively) and near-quantitative rejection of nanoscale solutes. Reactive force field simulations through a multilayer COF model reveal the origins of rapid solvent transport and size selectivity through steric gating. These results establish highly crystalline COFs as practical, high-performance membrane materials and point to new routes for energy-efficient separations across chemical, environmental, and industrial technologies.