https://scholars.lib.ntu.edu.tw/handle/123456789/611464
標題: | Efficient and Accurate Charge Assignments via a Multilayer Connectivity-Based Atom Contribution (m-CBAC) Approach | 作者: | Zou C. Penley D.R. Cho E.H. Lin L.-C. LI-CHIANG LIN |
關鍵字: | Database systems;Metal-Organic Frameworks;Multilayers;Organometallics;Quantum theory;Computationally efficient;Connectivity pattern;Energy applications;Henry coefficients;Metalorganic frameworks (MOFs);Molecular simulations;Orders of magnitude;Pearson coefficient;Atoms | 公開日期: | 2020 | 卷: | 124 | 期: | 21 | 起(迄)頁: | 11428-11437 | 來源出版物: | Journal of Physical Chemistry C | 摘要: | Metal-organic frameworks (MOFs) have drawn considerable attention for their potential in a variety of energy applications such as gas separations and storage. With thousands of MOFs reported and more being discovered, molecular simulations can play a critical role in facilitating the material discovery. In those calculations, accurate charge assignments to the framework atoms are essential. In this study, we expand on the connectivity-based atom contribution (CBAC) method to develop an efficient, robust, and accurate approach for charge assignments. Distinct from the original CBAC method, which uses 1st layer connectivity of a target atom, our approach, denoted as multilayer CBAC (m-CBAC), incorporates multilayer connectivity up to 2nd layers. An extensive set of ?2700 MOFs with the density-derived electrostatic and chemical (DDEC) charges is used to train the databases. The approach assigns charges in a systematic manner, where the highest-level connectivity database (i.e., 2nd-layer connectivity) is first searched, followed by lower-level connectivity patterns until the connectivity pattern is recognized. This approach makes the charge predictions feasible to almost all MOFs. Our results show that the charges assigned using m-CBAC resemble the DDEC charges very well (Pearson coefficient of 0.988). At the same time, the m-CBAC approach is computationally efficient, which is orders of magnitude faster than quantum mechanical approaches. Also, this study demonstrates that the accurate charge assignments from m-CBAC lead to reliable predictions on the Henry coefficient of CO2 in MOFs. Overall, the m-CBAC approach can enable fast charge assignments for MOFs with good accuracy, and a software for m-CBAC charge assignments together with charges assigned for ?12 000 MOFs in a recently released MOF database is made available along with this work. ? 2020 American Chemical Society. |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85086725739&doi=10.1021%2facs.jpcc.0c01524&partnerID=40&md5=bbb3cfeb870b6f7847832a15aec9bb34 https://scholars.lib.ntu.edu.tw/handle/123456789/611464 |
DOI: | 10.1021/acs.jpcc.0c01524 |
顯示於: | 化學工程學系 |
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