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

Soniat, Marielle and Tesfaye, Meron and Brooks, Daniel and Merinov, Boris and Goddard, William A., III and Weber, Adam Z. and Houle, Frances A. (2018) Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes. Polymer, 134 . pp. 125-142. ISSN 0032-3861. doi:10.1016/j.polymer.2017.11.055.

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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) O_2 quenching of a phosphorescent dye embedded in poly(n-butyl(amino) thionylphosphazene), and (2) O_2, N_2, CH_4 and CO_2 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: CO_2 capture from air and blocking of methane cross-over in an aged solar fuels device.

Item Type:Article
Related URLs:
URLURL TypeDescription Data
Merinov, Boris0000-0002-2783-4262
Goddard, William A., III0000-0003-0097-5716
Weber, Adam Z.0000-0002-7749-1624
Houle, Frances A.0000-0001-5571-2548
Additional Information:© 2017 Published by Elsevier Ltd. Received 22 August 2017, Revised 14 October 2017, Accepted 22 November 2017, Available online 24 November 2017. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: The reaction-diffusion simulations were performed by M. S. and F. H., and experimental measurements were performed by M. T. and A. W., supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. M. T. thanks the National Science Foundation Graduate Research Fellowship under Grant No. DGE 1106400. D. B., B. M. and W. A. G. acknowledge funding from Bosch Energy Research Network Grant No 07.23.CS.15 for the MD simulation work. Bosch Energy Research had no involvement in decisions concerning data collection, data processing, writing, or article submission. The authors are grateful to Dr. Daniel J. Miller (JCAP, LBNL) for many helpful discussions on membrane polymer science, to Mr. Ezra L. Clark (JCAP, LBNL) for data on photoelectrochemical production of methane, and to Dr. William D. Hinsberg (Columbia Hill Technical Consulting) for discussions on the use of Kinetiscope in this work.
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSF Graduate Research FellowshipDGE 1106400
Bosch Energy Research Network07.23.CS.15
Subject Keywords:Rubbery polymers; Reaction-diffusion modeling; Gas transport
Record Number:CaltechAUTHORS:20171127-141541426
Persistent URL:
Official Citation:Marielle Soniat, Meron Tesfaye, Daniel Brooks, Boris Merinov, William A. Goddard III, Adam Z. Weber, Frances A. Houle, Predictive simulation of non-steady-state transport of gases through rubbery polymer membranes, Polymer, Volume 134, 3 January 2018, Pages 125-142, ISSN 0032-3861, (
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:83453
Deposited By: Tony Diaz
Deposited On:27 Nov 2017 22:21
Last Modified:15 Nov 2021 19:58

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