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

Journal Article · 24 November 2017 · Polymer

DOI: https://doi.org/10.1016/j.polymer.2017.11.055 · OSTI ID:1459399

Soniat, Marielle ^[1]; Tesfaye, Meron ^[2]; Brooks, Daniel ^[3]; Merinov, Boris ^[3]; Goddard, William A. ^[3]; Weber, Adam Z.  ^[4]; Houle, Frances A.  ^[1]

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1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis. Chemical Sciences Division
2. 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
3. California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center (MSC). Beckman Inst.
4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Artificial Photosynthesis. Energy Storage and Distributed Resources Division

In this paper, 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. Finally, 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.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF) (United States); Bosch Energy Research Network
• Grant/Contract Number: AC02-05CH11231; SC0004993
• OSTI ID: 1459399
• Journal Information: Polymer, Journal Name: Polymer Vol. 134; ISSN 0032-3861
• Publisher: ElsevierCopyright Statement
• Country of Publication: United States
• Language: English

Related Subjects

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