Metal-organic frameworks (MOFs) have shown promise for gas storage and sequestration applications storage on account of their large surface to volume ratio and modularity in structural and chemical composition. In-silico prediction of adsorption equilibria is a cost-effective means of obtaining quantitative predictions and insight on metal-adsorbate binding in a MOF. Given a large number of candidate structures, quantum chemical calculations can suggest promising storage materials as synthetic targets. To ensure accurate description of the critical local chemistry, we employ the ωB97M-V functional, which is an accurate range-separated hybrid metaGGA that includes non-local VV10 dispersion, designed by the combinatorial ``survival of the most transferable'' protocol. Using energy decomposition analysis, we unravel the nature of the binding to reveal the chemical influences at play in metal-ligand interactions across framework families. Our findings suggest multiple hydrogen binding can be a tractable route towards enhancing volumetric storage in a MOF. To add to pore size and framework topology as key variables in rational framework design, we identify charge transfer as a significant driver in chemical handle-based gas separations.

Quantum chemical insight on gas adsorption in metal-organic frameworks

ACS Spring Meeting 2021

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.