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Title: High-Throughput Computational Screening of Multivariate Metal–Organic Frameworks (MTV-MOFs) for CO 2 Capture

Abstract

Multivariate metal–organic frameworks (MTV-MOFs) contain multiple linker types within a single structure. Arrangements of linkers containing different functional groups confer structural diversity and surface heterogeneity and result in a combinatorial explosion in the number of possible structures. In this work, we carried out high-throughput computational screening of a large number of computer-generated MTV-MOFs to assess their CO 2 capture properties using grand canonical Monte Carlo simulations. The results demonstrate that functionalization enhances CO 2 capture performance of MTV-MOFs when compared to their parent (unfunctionalized) counterparts, and the pore size plays a dominant role in determining the CO 2 adsorption capabilities of MTV-MOFs irrespective of the combinations of the three functional groups (-F, -NH2, and -OCH3) that we investigated. We also found that the functionalization of parent MOFs with small pores led to larger enhancements in CO 2 uptake and CO 2/N 2 selectivity than functionalization in larger-pore MOFs. Free energy contour maps are presented to visually compare the influence of linker functionalization between frameworks with large and small pores.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4]
  1. State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
  2. School of Chemical and Biomolecular Engineering, Pusan National University, Busan 46241, Korea (South)
  3. School of Chemical, Biological, and Environmental Engineering, Oregon State University, Corvallis, Oregon 97331, United States
  4. Department of Chemical and Biological Engineering, Northwestern University, Evanston, Illinois 60208, United States
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1484018
Grant/Contract Number:  
FG02-12ER16362; SC0008688
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 8; Journal Issue: 24; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English

Citation Formats

Li, Song, Chung, Yongchul G., Simon, Cory M., and Snurr, Randall Q. High-Throughput Computational Screening of Multivariate Metal–Organic Frameworks (MTV-MOFs) for CO2 Capture. United States: N. p., 2017. Web. doi:10.1021/acs.jpclett.7b02700.
Li, Song, Chung, Yongchul G., Simon, Cory M., & Snurr, Randall Q. High-Throughput Computational Screening of Multivariate Metal–Organic Frameworks (MTV-MOFs) for CO2 Capture. United States. doi:10.1021/acs.jpclett.7b02700.
Li, Song, Chung, Yongchul G., Simon, Cory M., and Snurr, Randall Q. Thu . "High-Throughput Computational Screening of Multivariate Metal–Organic Frameworks (MTV-MOFs) for CO2 Capture". United States. doi:10.1021/acs.jpclett.7b02700. https://www.osti.gov/servlets/purl/1484018.
@article{osti_1484018,
title = {High-Throughput Computational Screening of Multivariate Metal–Organic Frameworks (MTV-MOFs) for CO2 Capture},
author = {Li, Song and Chung, Yongchul G. and Simon, Cory M. and Snurr, Randall Q.},
abstractNote = {Multivariate metal–organic frameworks (MTV-MOFs) contain multiple linker types within a single structure. Arrangements of linkers containing different functional groups confer structural diversity and surface heterogeneity and result in a combinatorial explosion in the number of possible structures. In this work, we carried out high-throughput computational screening of a large number of computer-generated MTV-MOFs to assess their CO2 capture properties using grand canonical Monte Carlo simulations. The results demonstrate that functionalization enhances CO2 capture performance of MTV-MOFs when compared to their parent (unfunctionalized) counterparts, and the pore size plays a dominant role in determining the CO2 adsorption capabilities of MTV-MOFs irrespective of the combinations of the three functional groups (-F, -NH2, and -OCH3) that we investigated. We also found that the functionalization of parent MOFs with small pores led to larger enhancements in CO2 uptake and CO2/N2 selectivity than functionalization in larger-pore MOFs. Free energy contour maps are presented to visually compare the influence of linker functionalization between frameworks with large and small pores.},
doi = {10.1021/acs.jpclett.7b02700},
journal = {Journal of Physical Chemistry Letters},
number = 24,
volume = 8,
place = {United States},
year = {2017},
month = {12}
}

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Cited by: 6 works
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