Continuum Model of Gas Uptake for Inhomogeneous Fluids

Yungok Ihm; Valentino R. Cooper; Lukas Vlcek; Pieremanuele Canepa; Timo Thonhauser; Ji Hoon Shim; James R. Morris

doi:10.1021/acs.jpcc.7b04834

Continuum Model of Gas Uptake for Inhomogeneous Fluids

Yungok Ihm, Valentino R. Cooper, Lukas Vlcek, Pieremanuele Canepa, Timo Thonhauser, Ji Hoon Shim, James R. Morris

Materials Science and Technology Div

Research output: Contribution to journal › Comment/debate

Abstract

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. The speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nanoporous materials.

Original language	English
Pages (from-to)	17625-17632
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	121
Issue number	33
DOIs	https://doi.org/10.1021/acs.jpcc.7b04834
State	Published - Aug 24 2017

Funding

Y.I. and J.H.S. were supported by the Global Frontier Program through the Global Frontier Hybrid Interface Materials (GFHIM) of the National Research Foundation (NRF) of Korea funded by the Ministry of Science, ICT & Future Planning (2013M3A6B1078870). J.R.M., V.R.C., and the initial work of Y.I. were supported from the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. The Monte Carlo simulation work performed by L.V. was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. This research used resources of the National Energy Research Scientific Computing Center, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DEAC02-05CH11231. P.C. was supported by DOE grant No. DE-FG02-08ER46491 and T.T. acknowledges support from NSF grant No. DMR-1145968. In addition, T.T. acknowledges generous support from the Simons Foundation through Grant No. 391888, which endowed his sabbatical at MIT. T.T. and P.C. acknowledges early calculations by Daniel Johnson at WFU.

Funders	Funder number
National Research Foundation of Korea
Simons Foundation	391888
Advanced Scientific Computing Research
Ministry of Science and Technology
Wake Forest University
Basic Energy Sciences
U.S. Department of Energy
Division of Molecular and Cellular Biosciences
U.S. Department of Energy	DE-FG02-08ER46491
Office of Science
Institute of Materials Research and Engineering
DMR-1145968
Ministry of Science, ICT and Future Planning	2013M3A6B1078870
Frontiers Foundation
Johnson and Johnson
National Research Foundation
Massachusetts Institute of Technology
National Stroke Foundation	DMR-1145968
Interface
Office of Science	DEAC02-05CH11231

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title = "Continuum Model of Gas Uptake for Inhomogeneous Fluids",

abstract = "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. The speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nanoporous materials.",

author = "Yungok Ihm and Cooper, {Valentino R.} and Lukas Vlcek and Pieremanuele Canepa and Timo Thonhauser and Shim, {Ji Hoon} and Morris, {James R.}",

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AU - Ihm, Yungok

AU - Cooper, Valentino R.

AU - Vlcek, Lukas

AU - Canepa, Pieremanuele

AU - Thonhauser, Timo

AU - Shim, Ji Hoon

AU - Morris, James R.

PY - 2017/8/24

Y1 - 2017/8/24

N2 - 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. The speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nanoporous materials.

AB - 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. The speed of the CMGIF method makes it a promising candidate for high-throughput materials discovery in connection with existing databases of nanoporous materials.

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Continuum Model of Gas Uptake for Inhomogeneous Fluids

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