Quantitatively modeling adsorbate diffusion through zeolitic imidazolate frameworks (ZIFs) must account for the inherent flexibility of these materials. Here, the lack of a transferable intramolecular ZIF force field (FF) for use in classical simulations has previously made an accurate simulation of adsorbate diffusion in many ZIFs impossible. We resolve this problem by introducing a density functional theory parameterized force field (FF) for ZIFs named the intraZIF-FF, which includes perturbations to the class I force fields previously used to model ZIFs. This FF outperforms ad hoc force fields at predicting ab initio relative energies and atomic forces taken from fully periodic ab initio molecular dynamics simulations of SALEM-2, ZIF-7, ZIF-8, and ZIF-90. We use the intraZIF-FF to predict the infinite dilution self-diffusion coefficients of 30 adsorbates with molecular diameters ranging from 2.66 to 7.0 Å in these 4 ZIFs. These results greatly increase the number of adsorbates for which accurate information about molecular diffusion in ZIFs is available.
Verploegh, Ross J., et al. "Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field." Journal of Physical Chemistry. C, vol. 123, no. 14, Mar. 2019. https://doi.org/10.1021/acs.jpcc.9b00733
Verploegh, Ross J., Kulkarni, Ambarish, Boulfelfel, Salah Eddine, Haydak, Jonathan C., Tang, Dai, & Sholl, David S. (2019). Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field. Journal of Physical Chemistry. C, 123(14). https://doi.org/10.1021/acs.jpcc.9b00733
Verploegh, Ross J., Kulkarni, Ambarish, Boulfelfel, Salah Eddine, et al., "Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field," Journal of Physical Chemistry. C 123, no. 14 (2019), https://doi.org/10.1021/acs.jpcc.9b00733
@article{osti_1712845,
author = {Verploegh, Ross J. and Kulkarni, Ambarish and Boulfelfel, Salah Eddine and Haydak, Jonathan C. and Tang, Dai and Sholl, David S.},
title = {Screening Diffusion of Small Molecules in Flexible Zeolitic Imidazolate Frameworks Using a DFT-Parameterized Force Field},
annote = {Quantitatively modeling adsorbate diffusion through zeolitic imidazolate frameworks (ZIFs) must account for the inherent flexibility of these materials. Here, the lack of a transferable intramolecular ZIF force field (FF) for use in classical simulations has previously made an accurate simulation of adsorbate diffusion in many ZIFs impossible. We resolve this problem by introducing a density functional theory parameterized force field (FF) for ZIFs named the intraZIF-FF, which includes perturbations to the class I force fields previously used to model ZIFs. This FF outperforms ad hoc force fields at predicting ab initio relative energies and atomic forces taken from fully periodic ab initio molecular dynamics simulations of SALEM-2, ZIF-7, ZIF-8, and ZIF-90. We use the intraZIF-FF to predict the infinite dilution self-diffusion coefficients of 30 adsorbates with molecular diameters ranging from 2.66 to 7.0 Å in these 4 ZIFs. These results greatly increase the number of adsorbates for which accurate information about molecular diffusion in ZIFs is available.},
doi = {10.1021/acs.jpcc.9b00733},
url = {https://www.osti.gov/biblio/1712845},
journal = {Journal of Physical Chemistry. C},
issn = {ISSN 1932-7447},
number = {14},
volume = {123},
place = {United States},
publisher = {American Chemical Society},
year = {2019},
month = {03}}
Journal Article
·
Mon Mar 04 23:00:00 EST 2019
· Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
·OSTI ID:1576982