Augmenting the Carbon Dioxide Uptake and Selectivity of Metal–Organic Frameworks by Metal Substitution: Molecular Simulations of LMOF-202

[Image: see text] Metal organic frameworks (MOFs) are promising porous materials for the adsorption of CO(2.) Here, we report the study of a luminescent MOF (LMOF), called LMOF-202. We have employed Grand Canonical Monte Carlo (GCMC) simulations to understand and explain the adsorption phenomena inside LMOF-202, and based on the phenomena happening at the molecular level, we have varied the metal ions in LMOF-202 to increase the CO(2) affinity and selectivity of the material. We show that the CO(2) adsorption capacity and selectivity can be increased by approximately 1.5 times at 1 bar and 298 K by changing the metal ion from Zn to Ba. We also report the feasibility of using this material to capture CO(2) from flue gas under realistic conditions (1 bar and 298 K). This work shows that LMOF-202 merits further consideration as a carbon capture adsorbent.