Computationally Exploring Structure-Property Relationships of Thermal Transport in Metal-Organic Frameworks

Metal-Organic Frameworks (MOFs) are crystalline, highly porous materials that have been heralded as revolutionary materials for gas storage and separations applications. However, the practical utility of MOFs depends on how rapidly they can disperse the significant amount of thermal energy produced during the exothermic adsorption process. Despite its significance, there is a limited understanding of the structure-thermal transport relationships in MOFs. To tackle this problem, we conducted the first high-throughput computational screening of thermal conductivity in MOFs by performing classical molecular dynamics (MD) simulations on a diverse set of 10,194 hypothetical MOFs. We observed that high thermal conductivity in MOFs is favored by small pores, high densities, and four-connected metal nodes. Furthermore, we discovered six hypothetical MOF structures that displayed very high average thermal conductivity. Interestingly, these six MOFs share square planar metal nodes that are each connected to four perpendicular organic linkers, implying that topology may be particularly important for thermal transport in MOFs.