Disclosing gate-opening/closing events inside a flexible metal-organic framework loaded with CO2 by reactive and essential dynamics

We have combined reactive molecular dynamics simulations with principal component analysis to provide a clearer view of the interactions and motion of the CO2 molecules inside a metal-organic framework and the movements of the MOF components that regulate storage, adsorption, and diffusion of the guest species. The tens-of-nanometer size of the simulated model, the capability of the reactive force field tuned to reproduce the inorganic-organic material confidently, and the unconventional use of essential dynamics have effectively disclosed the gate-opening/closing phenomenon, possible coordinations of CO2 at the metal centers, all the diffusion steps inside the MOF channels, the primary motions of the linkers, and the effects of their concerted rearrangements on local CO2 relocations.

Automated summary

We employed reactive molecular dynamics simulations and principal component analysis to obtain a clearer understanding of the interactions and motions of CO2 molecules and metal-organic framework components. Our simulations revealed the gate-opening/closing phenomenon, possible CO2 coordinations at the metal centers, diffusion steps inside the MOF channels, motions of the linkers, and the effects of their concerted rearrangements on CO2 relocations.