TY - JOUR
T1 - Towards rapid computational screening of metal-organic frameworks for carbon dioxide capture
T2 - Calculation of framework charges via charge equilibration
AU - Wilmer, Christopher E.
AU - Snurr, Randall Q.
N1 - Funding Information:
The authors would like to thank Dr. A. Özgur Yazaydin for helpful discussions. This work was supported by the Defense Threat Reduction Agency and in part by the National Science Foundation through TeraGrid resources provided by Information Technology at Purdue – the Rosen Center for Advanced Computing , under grant number TG-CTS080016N .
PY - 2011/7/15
Y1 - 2011/7/15
N2 - Metal-organic frameworks are promising materials for the capture of carbon dioxide. Finding the best metal-organic frameworks from the vast number of possibilities could be greatly accelerated by efficient computational screening techniques. We have previously reported an effective screening protocol for predicting carbon dioxide adsorption performance in metal-organic frameworks that uses grand canonical Monte Carlo simulations of gas adsorption. In the model, molecules interact via van der Waals and electrostatic interactions with each other and the framework. However, the method requires single-point quantum mechanics calculations for the estimation of atomic partial charges. In this study we investigate the feasibility of a modified protocol that bypasses the computationally expensive quantum mechanics calculations by applying instead the charge equilibration method. We compare the results of both protocols directly on fourteen metal-organic frameworks and conclude that the new protocol is sufficiently accurate for screening purposes and is significantly faster.
AB - Metal-organic frameworks are promising materials for the capture of carbon dioxide. Finding the best metal-organic frameworks from the vast number of possibilities could be greatly accelerated by efficient computational screening techniques. We have previously reported an effective screening protocol for predicting carbon dioxide adsorption performance in metal-organic frameworks that uses grand canonical Monte Carlo simulations of gas adsorption. In the model, molecules interact via van der Waals and electrostatic interactions with each other and the framework. However, the method requires single-point quantum mechanics calculations for the estimation of atomic partial charges. In this study we investigate the feasibility of a modified protocol that bypasses the computationally expensive quantum mechanics calculations by applying instead the charge equilibration method. We compare the results of both protocols directly on fourteen metal-organic frameworks and conclude that the new protocol is sufficiently accurate for screening purposes and is significantly faster.
KW - CO capture
KW - Charge equilibration
KW - Gas adsorption
KW - Metal-organic frameworks
KW - Molecular simulations
KW - Monte Carlo
KW - Partial atomic charge
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U2 - 10.1016/j.cej.2010.10.035
DO - 10.1016/j.cej.2010.10.035
M3 - Article
AN - SCOPUS:79960011510
SN - 1385-8947
VL - 171
SP - 775
EP - 781
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
IS - 3
ER -