Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes

Soniat, Marielle; Tesfaye, Meron; Brooks, Daniel; Merinov, Boris; Goddard, William A.; Weber, Adam Z.; Houle, Frances A.

doi:10.1016/j.polymer.2017.11.055

Title: Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes

Abstract

A multiscale, physically-based, reaction-diffusion kinetics model is developed for non-steady-state transport of simple gases through a rubbery polymer. Experimental data from the literature, new measurements of non-steady-state permeation and a molecular dynamics simulation of a gas-polymer sticking probability for a typical system are used to construct and validate the model framework. Using no adjustable parameters, the model successfully reproduces time-dependent experimental data for two distinct systems: (1) O2 quenching of a phosphorescent dye embedded in poly(n-butyl(amino) thionylphosphazene), and (2) O2, N2, CH4 and CO2 transport through poly(dimethyl siloxane). The calculations show that in the pre-steady-state regime, permeation is only correctly described if the sorbed gas concentration in the polymer is dynamically determined by the rise in pressure. The framework is used to predict selectivity targets for two applications involving rubbery membranes: CO2 capture from air and blocking of methane cross-over in an aged solar fuels device.

Authors:

Soniat, Marielle ^[1]; Tesfaye, Meron ^[2]; Brooks, Daniel ^[3]; Merinov, Boris ^[3]; Goddard, William A. ^[3];

^[4];

^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis. Chemical Sciences Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center (MSC). Beckman Inst.
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis. Energy Storage and Distributed Resources Division

Publication Date:: 2017-11-24

Research Org.:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Bosch Energy Research Network

OSTI Identifier:: 1459399

Alternate Identifier(s):: OSTI ID: 1467629; OSTI ID: 1549186

Grant/Contract Number:: AC02-05CH11231; SC0004993; DGE 1106400; 07.23.CS.15

Resource Type:: Accepted Manuscript

Journal Name:: Polymer

Additional Journal Information:: Journal Volume: 134; Journal ID: ISSN 0032-3861

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; rubbery polymers; reaction-diffusion modeling; gas transport

Citation Formats


                    Soniat, Marielle, Tesfaye, Meron, Brooks, Daniel, Merinov, Boris, Goddard, William A., Weber, Adam Z., and Houle, Frances A.. Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes.  United States: N. p., 2017. 
Web.  doi:10.1016/j.polymer.2017.11.055.

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                    Soniat, Marielle, Tesfaye, Meron, Brooks, Daniel, Merinov, Boris, Goddard, William A., Weber, Adam Z., & Houle, Frances A.. Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes.  United States.  https://doi.org/10.1016/j.polymer.2017.11.055

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                    Soniat, Marielle, Tesfaye, Meron, Brooks, Daniel, Merinov, Boris, Goddard, William A., Weber, Adam Z., and Houle, Frances A.. Fri .  
"Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes".  United States.  https://doi.org/10.1016/j.polymer.2017.11.055.  https://www.osti.gov/servlets/purl/1459399.

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@article{osti_1459399,

  title        = {Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes},

  author       = {Soniat, Marielle and Tesfaye, Meron and Brooks, Daniel and Merinov, Boris and Goddard, William A. and Weber, Adam Z. and Houle, Frances A.},

  abstractNote = {A multiscale, physically-based, reaction-diffusion kinetics model is developed for non-steady-state transport of simple gases through a rubbery polymer. Experimental data from the literature, new measurements of non-steady-state permeation and a molecular dynamics simulation of a gas-polymer sticking probability for a typical system are used to construct and validate the model framework. Using no adjustable parameters, the model successfully reproduces time-dependent experimental data for two distinct systems: (1) O2 quenching of a phosphorescent dye embedded in poly(n-butyl(amino) thionylphosphazene), and (2) O2, N2, CH4 and CO2 transport through poly(dimethyl siloxane). The calculations show that in the pre-steady-state regime, permeation is only correctly described if the sorbed gas concentration in the polymer is dynamically determined by the rise in pressure. The framework is used to predict selectivity targets for two applications involving rubbery membranes: CO2 capture from air and blocking of methane cross-over in an aged solar fuels device.},

  doi          = {10.1016/j.polymer.2017.11.055},

  journal      = {Polymer},

  number       = ,

  volume       = 134,

  place        = {United States},

  year         = {2017},

  month        = {11}

}

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Cited by: 10 works

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Figures / Tables:

Figure 1.: Chemical structures of the phosphorescent dye (a) platinum octa-ethyl porphyrin (PtOEP), and the polymers(b) poly(dimethyl siloxane)(PDMS) and (c) poly[n-butyl(amino)thionylphosphazene] (C4PTP) considered in this work.

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