Diffusion of Small Molecules in Metal Organic Framework Materials
; Phys. Rev. Lett. 110, 026102 (2013).
BibTeX
@article{Canepa2013diffusion,
author = {Canepa, P. and Nijem, N. and Chabal, Y. J. and Thonhauser, T.},
title = {{Diffusion of Small Molecules in Metal Organic Framework Materials}},
journal = {Physical Review Letters},
volume = {110},
pages = {026102},
year = {2013},
doi = {10.1103/PhysRevLett.110.026102}
}Brief summary
How quickly gases move through a porous material decides how useful it is for storing or capturing them. Combining quantum-mechanical simulations with time-resolved infrared spectroscopy, we identify four ways in which H2, CO2 and water travel through the framework MOF-74-Mg, and settle whether the molecules also bind at secondary sites.
Full abstract
Ab initio simulations are combined with in situ infrared spectroscopy to unveil the molecular transport of H2, CO2, and H2O in the metal organic framework MOF-74-Mg. Our study uncovers—at the atomistic level—the major factors governing the transport mechanism of these small molecules. In particular, we identify four key diffusion mechanisms and calculate the corresponding diffusion barriers, which are nicely confirmed by time-resolved infrared experiments. We also answer a long-standing question about the existence of secondary adsorption sites for the guest molecules, and we show how those sites affect the macroscopic diffusion properties. Our findings are important to gain a fundamental understanding of the diffusion processes in these nanoporous materials, with direct implications for the usability of MOFs in gas sequestration and storage applications.