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Title: Continuum Model of Gas Uptake for Inhomogeneous Fluids

We describe a continuum model of gas uptake for inhomogeneous fluids (CMGIF) and use it to predict fluid adsorption in porous materials directly from gas-substrate interaction energies determined by first principles calculations or accurate effective force fields. The method uses a perturbation approach to correct bulk fluid interactions for local inhomogeneities caused by gas substrate interactions, and predicts local pressure and density of the adsorbed gas. The accuracy and limitations of the model are tested by comparison with the results of Grand Canonical Monte Carlo simulations of hydrogen uptake in metal-organic frameworks (MOFs). We show that the approach provides accurate predictions at room temperature and at low temperatures for less strongly interacting materials. As a result, the speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nano-porous materials.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [2] ; ORCiD logo [3] ;  [4] ;  [5] ; ORCiD logo [6]
  1. Pohang Univ. of Science and Technology, Pohang (Korea); Univ. of Tennessee, Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Wake Forest Univ., Winston-Salem, NC (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Wake Forest Univ., Winston-Salem, NC (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  5. Pohang Univ. of Science and Technology, Pohang (Korea)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 33; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1399992

Ihm, Yungok, Cooper, Valentino R., Vlcek, Lukas, Canepa, Pieremanuele, Thonhauser, Timo, Shim, Ji Hoon, and Morris, James R.. Continuum Model of Gas Uptake for Inhomogeneous Fluids. United States: N. p., Web. doi:10.1021/acs.jpcc.7b04834.
Ihm, Yungok, Cooper, Valentino R., Vlcek, Lukas, Canepa, Pieremanuele, Thonhauser, Timo, Shim, Ji Hoon, & Morris, James R.. Continuum Model of Gas Uptake for Inhomogeneous Fluids. United States. doi:10.1021/acs.jpcc.7b04834.
Ihm, Yungok, Cooper, Valentino R., Vlcek, Lukas, Canepa, Pieremanuele, Thonhauser, Timo, Shim, Ji Hoon, and Morris, James R.. 2017. "Continuum Model of Gas Uptake for Inhomogeneous Fluids". United States. doi:10.1021/acs.jpcc.7b04834. https://www.osti.gov/servlets/purl/1399992.
@article{osti_1399992,
title = {Continuum Model of Gas Uptake for Inhomogeneous Fluids},
author = {Ihm, Yungok and Cooper, Valentino R. and Vlcek, Lukas and Canepa, Pieremanuele and Thonhauser, Timo and Shim, Ji Hoon and Morris, James R.},
abstractNote = {We describe a continuum model of gas uptake for inhomogeneous fluids (CMGIF) and use it to predict fluid adsorption in porous materials directly from gas-substrate interaction energies determined by first principles calculations or accurate effective force fields. The method uses a perturbation approach to correct bulk fluid interactions for local inhomogeneities caused by gas substrate interactions, and predicts local pressure and density of the adsorbed gas. The accuracy and limitations of the model are tested by comparison with the results of Grand Canonical Monte Carlo simulations of hydrogen uptake in metal-organic frameworks (MOFs). We show that the approach provides accurate predictions at room temperature and at low temperatures for less strongly interacting materials. As a result, the speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nano-porous materials.},
doi = {10.1021/acs.jpcc.7b04834},
journal = {Journal of Physical Chemistry. C},
number = 33,
volume = 121,
place = {United States},
year = {2017},
month = {7}
}