| Abstract Scope |
Two-dimensional (2D) conductive metal-organic frameworks (MOFs) are a unique class of porous materials which offer electrical conductivity along with large surface area and penetrability for targeted analytes. In spite of these merits, engineering of targeted structure-property relationships in 2D MOFs remains a challenge due to limited fundamental understanding of intrinsic MOF structure and its electronic properties, as well as effects of humidity and confined water dynamics on their stability and electrical conductivity. To tame the flexible and ever-changing layered structures of 2D MOFs, we develop ab initio parametrized force fields that allow large-scale/long-time simulations of the dynamics of both dry and hydrated MOFs. Our molecular dynamics simulations reveal the structural reasons behind hydrolysis of Co3(HHTP)2 vs. intact Cu3(HHTP)2, HHTP=2,3,6,7,10,11-hexahydroxytriphenylene, elucidate the effects of temperature and humidity-induced structural deformations and heterogeneity on catalytic activity of Co3(HTTP)2, HTTP=hexathiotriphenylene, and answer the long-posed question of the nature of electrical conductivity in Ni3(HITP)2, HITP=2,3,6,7,10,11-hexaiminotriphenylene. |