Storage and diffusion of CO(2) in covalent organic frameworks—A neural network-based molecular dynamics simulation approach

As a consequence of the accelerated climate change, solutions to capture, store and potentially activate carbon dioxide received increased interest in recent years. Herein, it is demonstrated, that the neural network potential ANI-2x is able to describe nanoporous organic materials at approx. density functional theory accuracy and force field cost, using the example of the recently published two- and three-dimensional covalent organic frameworks HEX-COF1 and 3D-HNU5 and their interaction with CO(2) guest molecules. Along with the investigation of the diffusion behaviour, a wide range of properties of interest is analyzed, such as the structure, pore size distribution and host-guest distribution functions. The workflow developed herein facilitates the estimation of the maximum CO(2) adsorption capacity and is easily generalizable to other systems. Additionally, this work illustrates, that minimum distance distribution functions can be a highly useful tool in understanding the nature of interactions in host-gas systems at the atomic level.