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Title: Force Field Development from Periodic Density Functional Theory Calculations for Gas Separation Applications Using Metal–Organic Frameworks

Abstract

We present accurate force fields developed from density functional theory (DFT) calculations with periodic boundary conditions for use in molecular simulations involving M2(dobdc) (M-MOF-74; dobdc4– = 2,5-dioxidobenzenedicarboxylate; M = Mg, Mn, Fe, Co, Ni, Zn) and frameworks of similar topology. In these systems, conventional force fields fail to accurately model gas adsorption due to the strongly binding open-metal sites. The DFT-derived force fields predict the adsorption of CO2, H2O, and CH4 inside these frameworks much more accurately than other common force fields. We show that these force fields can also be used for M2(dobpdc) (dobpdc4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate), an extended version of MOF-74, and thus are a promising alternative to common force fields for studying materials similar to MOF-74 for carbon capture applications. Furthermore, it is anticipated that the approach can be applied to other metal–organic framework topologies to obtain force fields for different systems. We have used this force field to study the effect of contaminants such as H2O and N2 upon these materials’ performance for the separation of CO2 from the emissions of natural gas reservoirs and coal-fired power plants. Specifically, mixture adsorption isotherms calculated with these DFT-derived force fields showed a significant reduction in the uptake of manymore » gas components in the presence of even trace amounts of H2O vapor. The extent to which the various gases are affected by the concentration of H2O in the reservoir is quantitatively different for the different frameworks and is related to their heats of adsorption. Additionally, significant increases in CO2 selectivities over CH4 and N2 are observed as the temperature of the systems is lowered.« less

Authors:
; ; ;  [1];  [2]; ; ; ; ;  [3];  [2]
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  1. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Synopsys, Inc., Mountain View, California 94043, United States
  2. Institut des Sciences et Ingénierie Chimiques, Valais, École Polytechnique Fédérale de Lausanne (EPFL), Rue de l’Industrie 17, CH-1951 Sion, Switzerland
  3. Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1257491
Alternate Identifier(s):
OSTI ID: 1393053
Grant/Contract Number:  
AC02-05CH11231; SC0001015
Resource Type:
Published Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Name: Journal of Physical Chemistry. C Journal Volume: 120 Journal Issue: 23; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mercado, Rocio, Vlaisavljevich, Bess, Lin, Li-Chiang, Lee, Kyuho, Lee, Yongjin, Mason, Jarad A., Xiao, Dianne J., Gonzalez, Miguel I., Kapelewski, Matthew T., Neaton, Jeffrey B., and Smit, Berend. Force Field Development from Periodic Density Functional Theory Calculations for Gas Separation Applications Using Metal–Organic Frameworks. United States: N. p., 2016. Web. doi:10.1021/acs.jpcc.6b03393.
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Mercado, Rocio, Vlaisavljevich, Bess, Lin, Li-Chiang, Lee, Kyuho, Lee, Yongjin, Mason, Jarad A., Xiao, Dianne J., Gonzalez, Miguel I., Kapelewski, Matthew T., Neaton, Jeffrey B., & Smit, Berend. Force Field Development from Periodic Density Functional Theory Calculations for Gas Separation Applications Using Metal–Organic Frameworks. United States. https://doi.org/10.1021/acs.jpcc.6b03393
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Mercado, Rocio, Vlaisavljevich, Bess, Lin, Li-Chiang, Lee, Kyuho, Lee, Yongjin, Mason, Jarad A., Xiao, Dianne J., Gonzalez, Miguel I., Kapelewski, Matthew T., Neaton, Jeffrey B., and Smit, Berend. Wed . "Force Field Development from Periodic Density Functional Theory Calculations for Gas Separation Applications Using Metal–Organic Frameworks". United States. https://doi.org/10.1021/acs.jpcc.6b03393.
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@article{osti_1257491,
title = {Force Field Development from Periodic Density Functional Theory Calculations for Gas Separation Applications Using Metal–Organic Frameworks},
author = {Mercado, Rocio and Vlaisavljevich, Bess and Lin, Li-Chiang and Lee, Kyuho and Lee, Yongjin and Mason, Jarad A. and Xiao, Dianne J. and Gonzalez, Miguel I. and Kapelewski, Matthew T. and Neaton, Jeffrey B. and Smit, Berend},
abstractNote = {We present accurate force fields developed from density functional theory (DFT) calculations with periodic boundary conditions for use in molecular simulations involving M2(dobdc) (M-MOF-74; dobdc4– = 2,5-dioxidobenzenedicarboxylate; M = Mg, Mn, Fe, Co, Ni, Zn) and frameworks of similar topology. In these systems, conventional force fields fail to accurately model gas adsorption due to the strongly binding open-metal sites. The DFT-derived force fields predict the adsorption of CO2, H2O, and CH4 inside these frameworks much more accurately than other common force fields. We show that these force fields can also be used for M2(dobpdc) (dobpdc4– = 4,4'-dioxidobiphenyl-3,3'-dicarboxylate), an extended version of MOF-74, and thus are a promising alternative to common force fields for studying materials similar to MOF-74 for carbon capture applications. Furthermore, it is anticipated that the approach can be applied to other metal–organic framework topologies to obtain force fields for different systems. We have used this force field to study the effect of contaminants such as H2O and N2 upon these materials’ performance for the separation of CO2 from the emissions of natural gas reservoirs and coal-fired power plants. Specifically, mixture adsorption isotherms calculated with these DFT-derived force fields showed a significant reduction in the uptake of many gas components in the presence of even trace amounts of H2O vapor. The extent to which the various gases are affected by the concentration of H2O in the reservoir is quantitatively different for the different frameworks and is related to their heats of adsorption. Additionally, significant increases in CO2 selectivities over CH4 and N2 are observed as the temperature of the systems is lowered.},
doi = {10.1021/acs.jpcc.6b03393},
journal = {Journal of Physical Chemistry. C},
number = 23,
volume = 120,
place = {United States},
year = {Wed Jun 08 00:00:00 EDT 2016},
month = {Wed Jun 08 00:00:00 EDT 2016}
}
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Works referenced in this record:

In silico screening of carbon-capture materials
journal, May 2012

  • Lin, Li-Chiang; Berger, Adam H.; Martin, Richard L.
  • Nature Materials, Vol. 11, Issue 7
  • DOI: 10.1038/nmat3336

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Carbon Dioxide's Liquid-Vapor Coexistence Curve And Critical Properties as Predicted by a Simple Molecular Model
journal, August 1995

  • Harris, Jonathan G.; Yung, Kwong H.
  • The Journal of Physical Chemistry, Vol. 99, Issue 31
  • DOI: 10.1021/j100031a034

Carbon capture in metal–organic frameworks—a comparative study
journal, January 2011

  • Simmons, Jason M.; Wu, Hui; Zhou, Wei
  • Energy & Environmental Science, Vol. 4, Issue 6
  • DOI: 10.1039/c0ee00700e

Projector augmented-wave method
journal, December 1994

CO 2 Dynamics in a Metal–Organic Framework with Open Metal Sites
journal, August 2012

  • Kong, Xueqian; Scott, Eric; Ding, Wen
  • Journal of the American Chemical Society, Vol. 134, Issue 35
  • DOI: 10.1021/ja306822p

UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations
journal, December 1992

  • Rappe, A. K.; Casewit, C. J.; Colwell, K. S.
  • Journal of the American Chemical Society, Vol. 114, Issue 25, p. 10024-10035
  • DOI: 10.1021/ja00051a040

The materials genome in action: identifying the performance limits for methane storage
journal, January 2015

  • Simon, Cory M.; Kim, Jihan; Gomez-Gualdron, Diego A.
  • Energy & Environmental Science, Vol. 8, Issue 4
  • DOI: 10.1039/C4EE03515A

Charge equilibration for molecular dynamics simulations
journal, April 1991

  • Rappe, Anthony K.; Goddard, William A.
  • The Journal of Physical Chemistry, Vol. 95, Issue 8
  • DOI: 10.1021/j100161a070

Understanding CO 2 Dynamics in Metal-Organic Frameworks with Open Metal Sites
journal, March 2013

Ab initio carbon capture in open-site metal–organic frameworks
journal, August 2012

  • Dzubak, Allison L.; Lin, Li-Chiang; Kim, Jihan
  • Nature Chemistry, Vol. 4, Issue 10
  • DOI: 10.1038/nchem.1432

DREIDING: a generic force field for molecular simulations
journal, December 1990

  • Mayo, Stephen L.; Olafson, Barry D.; Goddard, William A.
  • The Journal of Physical Chemistry, Vol. 94, Issue 26, p. 8897-8909
  • DOI: 10.1021/j100389a010

In silico screening of metal–organic frameworks in separation applications
journal, January 2011

  • Krishna, Rajamani; van Baten, Jasper M.
  • Physical Chemistry Chemical Physics, Vol. 13, Issue 22
  • DOI: 10.1039/c1cp20282k

Prediction of CO 2 Adsorption Properties in Zeolites Using Force Fields Derived from Periodic Dispersion-Corrected DFT Calculations
journal, May 2012

  • Fang, Hanjun; Kamakoti, Preeti; Zang, Ji
  • The Journal of Physical Chemistry C, Vol. 116, Issue 19
  • DOI: 10.1021/jp302433b

Carbon Dioxide Capture: Prospects for New Materials
journal, July 2010

  • D'Alessandro, Deanna M.; Smit, Berend; Long, Jeffrey R.
  • Angewandte Chemie International Edition, Vol. 49, Issue 35, p. 6058-6082
  • DOI: 10.1002/anie.201000431

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Small-Molecule Adsorption in Open-Site Metal–Organic Frameworks: A Systematic Density Functional Theory Study for Rational Design
journal, January 2015

  • Lee, Kyuho; Howe, Joshua D.; Lin, Li-Chiang
  • Chemistry of Materials, Vol. 27, Issue 3, p. 668-678
  • DOI: 10.1021/cm502760q

A five-site model for liquid water and the reproduction of the density anomaly by rigid, nonpolarizable potential functions
journal, May 2000

  • Mahoney, Michael W.; Jorgensen, William L.
  • The Journal of Chemical Physics, Vol. 112, Issue 20
  • DOI: 10.1063/1.481505

A reoptimization of the five-site water potential (TIP5P) for use with Ewald sums
journal, April 2004

  • Rick, Steven W.
  • The Journal of Chemical Physics, Vol. 120, Issue 13
  • DOI: 10.1063/1.1652434

Comparison of simple potential functions for simulating liquid water
journal, July 1983

  • Jorgensen, William L.; Chandrasekhar, Jayaraman; Madura, Jeffry D.
  • The Journal of Chemical Physics, Vol. 79, Issue 2
  • DOI: 10.1063/1.445869

Highly efficient separation of carbon dioxide by a metal-organic framework replete with open metal sites
journal, November 2009

  • Britt, D.; Furukawa, H.; Wang, B.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 49, p. 20637-20640
  • DOI: 10.1073/pnas.0909718106

Synthesis of a honeycomb-like Cu-based metal–organic framework and its carbon dioxide adsorption behaviour
journal, January 2013

  • Sanz, Raúl; Martínez, Fernando; Orcajo, Gisela
  • Dalton Trans., Vol. 42, Issue 7
  • DOI: 10.1039/C2DT32138F

Effect of Water Adsorption on Retention of Structure and Surface Area of Metal–Organic Frameworks
journal, April 2012

  • Schoenecker, Paul M.; Carson, Cantwell G.; Jasuja, Himanshu
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 18
  • DOI: 10.1021/ie202325p

Multiscale Modeling of Water in Mg-MOF-74: From Electronic Structure Calculations to Adsorption Isotherms
journal, July 2014

  • Rudenko, A. N.; Bendt, S.; Keil, F. J.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 29
  • DOI: 10.1021/jp503778m

Understanding Trends in CO 2 Adsorption in Metal–Organic Frameworks with Open-Metal Sites
journal, February 2014

  • Poloni, Roberta; Lee, Kyuho; Berger, Robert F.
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 5
  • DOI: 10.1021/jz500202x

Ab Initio Derived Force Fields for Predicting CO 2 Adsorption and Accessibility of Metal Sites in the Metal–Organic Frameworks M-MOF-74 (M = Mn, Co, Ni, Cu)
journal, June 2015

  • Haldoupis, Emmanuel; Borycz, Joshua; Shi, Huiliang
  • The Journal of Physical Chemistry C, Vol. 119, Issue 28
  • DOI: 10.1021/acs.jpcc.5b03700

Force-Field Development from Electronic Structure Calculations with Periodic Boundary Conditions: Applications to Gaseous Adsorption and Transport in Metal–Organic Frameworks
journal, March 2014

  • Lin, Li-Chiang; Lee, Kyuho; Gagliardi, Laura
  • Journal of Chemical Theory and Computation, Vol. 10, Issue 4
  • DOI: 10.1021/ct500094w

The melting temperature of the most common models of water
journal, March 2005

  • Vega, C.; Sanz, E.; Abascal, J. L. F.
  • The Journal of Chemical Physics, Vol. 122, Issue 11
  • DOI: 10.1063/1.1862245

Structure and Dynamics of the TIP3P, SPC, and SPC/E Water Models at 298 K
journal, November 2001

  • Mark, Pekka; Nilsson, Lennart
  • The Journal of Physical Chemistry A, Vol. 105, Issue 43
  • DOI: 10.1021/jp003020w

Utilization of Dual-PSA Technology for Natural Gas Upgrading and Integrated CO2 Capture
journal, January 2012

Can Metal-Organic Framework Materials Play a Useful Role in Large-Scale Carbon Dioxide Separations?
journal, August 2010

  • Keskin, Seda; van Heest, Timothy M.; Sholl, David S.
  • ChemSusChem, Vol. 3, Issue 8
  • DOI: 10.1002/cssc.201000114

Selective adsorption of ethylene over ethane and propylene over propane in the metal–organic frameworks M2(dobdc) (M = Mg, Mn, Fe, Co, Ni, Zn)
journal, January 2013

  • Geier, Stephen J.; Mason, Jarad A.; Bloch, Eric D.
  • Chemical Science, Vol. 4, Issue 5
  • DOI: 10.1039/c3sc00032j

Dramatic Tuning of Carbon Dioxide Uptake via Metal Substitution in a Coordination Polymer with Cylindrical Pores
journal, August 2008

  • Caskey, Stephen R.; Wong-Foy, Antek G.; Matzger, Adam J.
  • Journal of the American Chemical Society, Vol. 130, Issue 33, p. 10870-10871
  • DOI: 10.1021/ja8036096

Evaluating metal–organic frameworks for natural gas storage
journal, January 2014

  • Mason, Jarad A.; Veenstra, Mike; Long, Jeffrey R.
  • Chemical Science, Vol. 5, Issue 1, p. 32-51
  • DOI: 10.1039/C3SC52633J

DFT-based force field development for noble gas adsorption in metal organic frameworks
journal, January 2015

  • Demir, Hakan; Greathouse, Jeffery A.; Staiger, Chad L.
  • Journal of Materials Chemistry A, Vol. 3, Issue 46
  • DOI: 10.1039/C5TA06201B

Molecular simulation of adsorption sites of light gases in the metal-organic framework IRMOF-1
journal, December 2007

Open Babel: An open chemical toolbox
journal, October 2011

  • O'Boyle, Noel M.; Banck, Michael; James, Craig A.
  • Journal of Cheminformatics, Vol. 3, Issue 1
  • DOI: 10.1186/1758-2946-3-33

Characterization of the TIP4P-Ew water model: Vapor pressure and boiling point
journal, November 2005

  • Horn, Hans W.; Swope, William C.; Pitera, Jed W.
  • The Journal of Chemical Physics, Vol. 123, Issue 19
  • DOI: 10.1063/1.2085031

Higher-accuracy van der Waals density functional
journal, August 2010

Carbon Dioxide Capture in Metal–Organic Frameworks
journal, September 2011

  • Sumida, Kenji; Rogow, David L.; Mason, Jarad A.
  • Chemical Reviews, Vol. 112, Issue 2, p. 724-781
  • DOI: 10.1021/cr2003272

Application of a High-Throughput Analyzer in Evaluating Solid Adsorbents for Post-Combustion Carbon Capture via Multicomponent Adsorption of CO 2 , N 2 , and H 2 O
journal, April 2015

  • Mason, Jarad A.; McDonald, Thomas M.; Bae, Tae-Hyun
  • Journal of the American Chemical Society, Vol. 137, Issue 14
  • DOI: 10.1021/jacs.5b00838

Prediction of the Temperature-Dependent Thermal Conductivity and Shear Viscosity for Rigid Water Models
journal, August 2012

  • Mao, Yijin; Zhang, Yuwen
  • Journal of Nanotechnology in Engineering and Medicine, Vol. 3, Issue 3
  • DOI: 10.1115/1.4007135

An intermolecular potential model for the simulation of ice and water near the melting point: A six-site model of H[sub 2]O
journal, January 2003

  • Nada, Hiroki; van der Eerden, Jan P. J. M.
  • The Journal of Chemical Physics, Vol. 118, Issue 16
  • DOI: 10.1063/1.1562610

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Electrostatic Potential Derived Atomic Charges for Periodic Systems Using a Modified Error Functional
journal, August 2009

  • Campañá, Carlos; Mussard, Bastien; Woo, Tom K.
  • Journal of Chemical Theory and Computation, Vol. 5, Issue 10
  • DOI: 10.1021/ct9003405

In silico screening of zeolite membranes for CO2 capture
journal, September 2010

Rod Packings and Metal−Organic Frameworks Constructed from Rod-Shaped Secondary Building Units
journal, February 2005

  • Rosi, Nathaniel L.; Kim, Jaheon; Eddaoudi, Mohamed
  • Journal of the American Chemical Society, Vol. 127, Issue 5, p. 1504-1518
  • DOI: 10.1021/ja045123o

MOF-74 building unit has a direct impact on toxic gas adsorption
journal, January 2011

  • Grant Glover, T.; Peterson, Gregory W.; Schindler, Bryan J.
  • Chemical Engineering Science, Vol. 66, Issue 2, p. 163-170
  • DOI: 10.1016/j.ces.2010.10.002

Evaluating metal–organic frameworks for post-combustion carbon dioxide capture via temperature swing adsorption
journal, January 2011

  • Mason, Jarad A.; Sumida, Kenji; Herm, Zoey R.
  • Energy & Environmental Science, Vol. 4, Issue 8, p. 3030-3040
  • DOI: 10.1039/c1ee01720a

Improving Predictions of Gas Adsorption in Metal–Organic Frameworks with Coordinatively Unsaturated Metal Sites: Model Potentials, ab initio Parameterization, and GCMC Simulations
journal, August 2012

  • Chen, Linjiang; Morrison, Carole A.; Düren, Tina
  • The Journal of Physical Chemistry C, Vol. 116, Issue 35
  • DOI: 10.1021/jp3062527

Water adsorption in metal-organic frameworks with open-metal sites
journal, December 2014

  • Peng, Xuan; Lin, Li-Chiang; Sun, Weizhen
  • AIChE Journal, Vol. 61, Issue 2
  • DOI: 10.1002/aic.14707

Development of an improved four-site water model for biomolecular simulations: TIP4P-Ew
journal, May 2004

  • Horn, Hans W.; Swope, William C.; Pitera, Jed W.
  • The Journal of Chemical Physics, Vol. 120, Issue 20
  • DOI: 10.1063/1.1683075

Synthesis of MIL-102, a Chromium Carboxylate Metal−Organic Framework, with Gas Sorption Analysis
journal, November 2006

  • Surblé, Suzy; Millange, Franck; Serre, Christian
  • Journal of the American Chemical Society, Vol. 128, Issue 46
  • DOI: 10.1021/ja064343u

CO 2 capture and conversion using Mg-MOF-74 prepared by a sonochemical method
journal, January 2012

  • Yang, Da-Ae; Cho, Hye-Young; Kim, Jun
  • Energy Environ. Sci., Vol. 5, Issue 4
  • DOI: 10.1039/C1EE02234B

Metal−Organic Frameworks with Exceptionally High Capacity for Storage of Carbon Dioxide at Room Temperature
journal, December 2005

  • Millward, Andrew R.; Yaghi, Omar M.
  • Journal of the American Chemical Society, Vol. 127, Issue 51, p. 17998-17999
  • DOI: 10.1021/ja0570032

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

Cooperative insertion of CO2 in diamine-appended metal-organic frameworks
journal, March 2015

  • McDonald, Thomas M.; Mason, Jarad A.; Kong, Xueqian
  • Nature, Vol. 519, Issue 7543
  • DOI: 10.1038/nature14327

Evaluation of various water models for simulation of adsorption in hydrophobic zeolites
journal, October 2009

Comprehensive study of carbon dioxide adsorption in the metal–organic frameworks M 2 (dobdc) (M = Mg, Mn, Fe, Co, Ni, Cu, Zn)
journal, January 2014

  • Queen, Wendy L.; Hudson, Matthew R.; Bloch, Eric D.
  • Chem. Sci., Vol. 5, Issue 12
  • DOI: 10.1039/C4SC02064B

Oxidation energies of transition metal oxides within the GGA + U framework
journal, May 2006

The Chemistry and Applications of Metal-Organic Frameworks
journal, August 2013

  • Furukawa, H.; Cordova, K. E.; O'Keeffe, M.
  • Science, Vol. 341, Issue 6149, p. 1230444-1230444
  • DOI: 10.1126/science.1230444

Large-Scale Screening of Zeolite Structures for CO 2 Membrane Separations
journal, May 2013

  • Kim, Jihan; Abouelnasr, Mahmoud; Lin, Li-Chiang
  • Journal of the American Chemical Society, Vol. 135, Issue 20
  • DOI: 10.1021/ja400267g

CO 2 Adsorption in Fe 2 (dobdc): A Classical Force Field Parameterized from Quantum Mechanical Calculations
journal, May 2014

  • Borycz, Joshua; Lin, Li-Chiang; Bloch, Eric D.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 23
  • DOI: 10.1021/jp500313j
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