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Title: High-Throughput Screening of Metal–Organic Frameworks for CO 2 Capture in the Presence of Water

Competitive co-adsorption of water is a major problem in the deployment of adsorption-based CO 2 capture. Water molecules may compete for adsorption sites, reducing the capacity of the material, and dehumidification prior to separating CO 2 from N 2 increases process complexity and cost. The development of adsorbent materials that can selectively adsorb CO 2 in the presence of water would be a major step forward in the deployment of CO2 capture materials in practice. In this study, large-scale computational screening was carried out to search for metal-organic frameworks (MOFs) with high selectivity toward CO 2 over H 2O. Calculating framework charges for thousands of MOFs is a significant challenge, so initial screening used a fast, but approximate, charge calculation method. Based on the initial screening, 15 MOFs were selected, and Monte Carlo simulations were carried out to compute the adsorption isotherms for these MOFs using more accurate framework charges calculated by density functional theory. Here, a detailed investigation was performed on the effect of using different methods for calculating partial charges, and it was found that electrostatic interactions contribute the majority of the adsorption energy of H 2O in the selected MOFs.
Authors:
 [1] ;  [2] ;  [3]
  1. Huazhong Univ. of Science and Technology, Wuhan (China). State Key Lab. of Coal Combustion, School of Energy and Power Engineering,
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering; Pusan National Univ., Busan (Korea, Republic of). School of Chemical and Biomolecular Engineering
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemical and Biological Engineering
Publication Date:
Grant/Contract Number:
FG02-12ER16362; SC0008688
Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 32; Journal Issue: 40; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Research Org:
Univ. of Minnesota, Minneapolis, MN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Orgs:
National Energy Research Scientific Computing Center (NERSC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Adsorption; post-combustion CO2 capture; humidity; molecular simulation; Monte Carlo
OSTI Identifier:
1476387

Li, Song, Chung, Yongchul G., and Snurr, Randall Q.. High-Throughput Screening of Metal–Organic Frameworks for CO2 Capture in the Presence of Water. United States: N. p., Web. doi:10.1021/acs.langmuir.6b02803.
Li, Song, Chung, Yongchul G., & Snurr, Randall Q.. High-Throughput Screening of Metal–Organic Frameworks for CO2 Capture in the Presence of Water. United States. doi:10.1021/acs.langmuir.6b02803.
Li, Song, Chung, Yongchul G., and Snurr, Randall Q.. 2016. "High-Throughput Screening of Metal–Organic Frameworks for CO2 Capture in the Presence of Water". United States. doi:10.1021/acs.langmuir.6b02803. https://www.osti.gov/servlets/purl/1476387.
@article{osti_1476387,
title = {High-Throughput Screening of Metal–Organic Frameworks for CO2 Capture in the Presence of Water},
author = {Li, Song and Chung, Yongchul G. and Snurr, Randall Q.},
abstractNote = {Competitive co-adsorption of water is a major problem in the deployment of adsorption-based CO2 capture. Water molecules may compete for adsorption sites, reducing the capacity of the material, and dehumidification prior to separating CO2 from N2 increases process complexity and cost. The development of adsorbent materials that can selectively adsorb CO2 in the presence of water would be a major step forward in the deployment of CO2 capture materials in practice. In this study, large-scale computational screening was carried out to search for metal-organic frameworks (MOFs) with high selectivity toward CO2 over H2O. Calculating framework charges for thousands of MOFs is a significant challenge, so initial screening used a fast, but approximate, charge calculation method. Based on the initial screening, 15 MOFs were selected, and Monte Carlo simulations were carried out to compute the adsorption isotherms for these MOFs using more accurate framework charges calculated by density functional theory. Here, a detailed investigation was performed on the effect of using different methods for calculating partial charges, and it was found that electrostatic interactions contribute the majority of the adsorption energy of H2O in the selected MOFs.},
doi = {10.1021/acs.langmuir.6b02803},
journal = {Langmuir},
number = 40,
volume = 32,
place = {United States},
year = {2016},
month = {9}
}