@article{88aed2bc26954f29a2a66e7d76182576,
title = "Large-Scale Refinement of Metal-Organic Framework Structures Using Density Functional Theory",
abstract = "Efforts to computationally characterize large numbers of nanoporous materials often rely on databases of experimentally resolved crystal structures. The accuracy of experimental crystal structures used in such calculations has a significant impact on the reliability of the results. In this work, we report structures optimized using periodic density functional theory (DFT) for more than 800 experimentally synthesized metal-organic frameworks (MOFs). Many MOFs changed significantly upon structural optimization, particularly materials that were crystallographically resolved in their solvated form. For each MOF, we simulated the adsorption of CH4 and CO2 using grand canonical Monte Carlo both before and after DFT optimization. The DFT optimization has a large impact on simulated gas adsorption in some cases. For example, CO2 loading at 1 bar changed by more than 25% in over 25% of the MOFs we considered.",
author = "Dalar Nazarian and Camp, {Jeffrey S.} and Chung, {Yongchul G.} and Snurr, {Randall Q.} and Sholl, {David S.}",
note = "Funding Information: This work has been supported by the Department of Energy Nanoporous Materials Genome Center, supported by the U.S. Department of Energy Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences and Biosciences under Award DEFG02-12ER16362 and used resources of the Argonne Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC02-06CH11357. This research was supported in part through the computational resources and staff contributions provided for the Quest high-performance computing facility (Project Allocation: p20663) at Northwestern University which is jointly supported by the Office of the Provost, the Office for Research, and Northwestern University Information Technology. Y.G.C was supported by the Pusan National University Research Grant 2016. We gratefully acknowledge Christopher Knight for assistance with running calculations on MIRA and Cory Simon for helpful discussions. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",
year = "2017",
month = mar,
day = "28",
doi = "10.1021/acs.chemmater.6b04226",
language = "English (US)",
volume = "29",
pages = "2521--2528",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "6",
}