Department of Chemical and Biological Engineering2024-11-0920130888-588510.1021/ie403159c2-s2.0-84890323102http://dx.doi.org/10.1021/ie403159chttps://hdl.handle.net/20.500.14288/9887Porous coordination networks (PCNs) offer considerable potential for gas separation applications due to their tunable pore sizes, large surface areas, high pore volumes, and good thermal and mechanical stabilities. Although a large number of PCNs have been synthesized to date, the potential performance of PCNs for adsorption-based and/or membrane-based gas separation applications is not known. In this work, we used atomically detailed simulations to predict the performance of PCN materials both in adsorption-based and in membrane-based separations of CH4/H-2, CO2/CH4, CO2/H-2, and CO2/N-2 mixtures. After validating the accuracy of our atomic simulations by comparing simulated adsorption isotherms of CO2, CH4, H-2, and N-2 with the available experimental data, we predicted adsorption-based selectivity, working capacity, regenerability, sorbent selection parameter, diffusion-based selectivity, membrane-based selectivity, and gas permeability of various PCNs. Several PCNs were predicted to outperform traditional zeolites and widely studied metal organic frameworks in CO2 separation processes. PCN-26 was identified as a potential membrane material that can exceed the upper bound established for CO2/CH4 and CO2/N-2 separations due to its high CO2 permeability and selectivity.EngineeringChemical engineeringJournal Article328438800032Q26582