Among the numerous materials being considered for solid CO 2 sorbents, metal-organic frameworks (MOFs) are some of the most promising . Through tuning the substituent metal nodes and organic linkers, these highly crystalline materials allow altering of their surface areas, pore sizes, and open metal sites to optimize their structural and adsorption properties. MOFs also show promise for, e.g., capture of other gases , energy storage , and drug delivery , and so the research community has intensively investigated this class of materials. In 2020, it was estimated that there are over 90,000 MOFs synthesized and 500,000 theorized , giving way to an enormous search space for finding the optimal structure for a particular application.