Perfluoropolyethers: Development of an All-Atom Force Field for Molecular Simulations and Validation with New Experimental Vapor Pressures and Liquid Densities

Black, Jana E.; Silva, Gonçalo M.  C.; Klein, Christoph; Iacovella, Christopher R.; Morgado, Pedro; Martins, Luís F.  G.; Filipe, Eduardo J.  M.; McCabe, Clare

doi:10.1021/acs.jpcb.7b00891

Title: Perfluoropolyethers: Development of an All-Atom Force Field for Molecular Simulations and Validation with New Experimental Vapor Pressures and Liquid Densities

Journal Article · 30 May 2017 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI: https://doi.org/10.1021/acs.jpcb.7b00891 · OSTI ID:1480285

^[1]; Silva, Gonçalo M. C. ^[2]; Klein, Christoph ^[1]; Iacovella, Christopher R. ^[1]; Morgado, Pedro ^[2]; Martins, Luís F. G. ^[3];

^[2];

^[4]

Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Vanderbilt Univ., Nashville, TN (United States). Multiscale Modeling and Simulation (MuMS)
Univ. de Lisboa, Lisboa (Portugal). Centro de Química Estrutural, Inst. Superior Técnico
Univ. de Lisboa, Lisboa (Portugal). Centro de Química Estrutural, Inst. Superior Técnico; Univ. de Évora, Évora (Portugal). Centro de Química de Évora
Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Vanderbilt Univ., Nashville, TN (United States). Multiscale Modeling and Simulation (MuMS); Vanderbilt Univ., Nashville, TN (United States). Dept. of Chemistry

A force field for perfluoropolyethers (PFPEs) based on the general optimized potentials for liquid simulations all-atom (OPLS-AA) force field has been derived in conjunction with experiments and ab initio quantum mechanical calculations. Vapor pressures and densities of two liquid PFPEs, perfluorodiglyme (CF₃–O–(CF₂–CF₂–O)2–CF₃) and perfluorotriglyme (CF₃–O–(CF₂–CF₂–O)₃–CF₃), have been measured experimentally to validate the force field and increase our understanding of the physical properties of PFPEs. Force field parameters build upon those for related molecules (e.g., ethers and perfluoroalkanes) in the OPLS-AA force field, with new parameters introduced for interactions specific to PFPEs. Molecular dynamics simulations using the new force field demonstrate excellent agreement with ab initio calculations at the RHF/6-31G* level for gas-phase torsional energies (<0.5 kcal mol^–1 error) and molecular structures for several PFPEs, and also accurately reproduce experimentally determined densities (<0.02 g cm^–3 error) and enthalpies of vaporization derived from experimental vapor pressures (<0.3 kcal mol–1). Additional comparisons between experiment and simulation show that polyethers demonstrate a significant decrease in enthalpy of vaporization upon fluorination unlike related molecules (e.g., alkanes and alcohols). Simulation suggests this phenomenon is a result of reduced cohesion in liquid PFPEs due to a reduction in localized associations between backbone oxygen atoms and neighboring molecules.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC); US Dept. of Education

Grant/Contract Number:: AC02-05CH11231; ACI-1047828; ACI-1535150; P200A090323; UID/QUI/0100/2013; SFRH/BPD/81748/2011; PEst-OE/QUI/UI0619/2011

OSTI ID:: 1480285

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 121, Issue 27; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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Title: Perfluoropolyethers: Development of an All-Atom Force Field for Molecular Simulations and Validation with New Experimental Vapor Pressures and Liquid Densities

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