One-step fabrication of robust lithium ion battery separators by polymerization-induced phase separation
Abstract
Conventional lithium ion battery separators are microporous polyolefin membranes that play a passive role in the electrochemical cell. Next generation separators should offer significant performance enhancements, while being fabricated through facile, low cost approaches with the ability to readily tune physicochemical properties. This study presents a single-step manufacturing technique based on UV-initiated polymerization-induced phase separation (PIPS), wherein microporous separators are fabricated from multifunctional monomers and ethylene carbonate (EC), which functions as both the pore-forming agent (porogen) and electrolyte component in the electrochemical cell. By controlling the ratio of the 1,4-butanediol diacrylate (BDDA) monomer to ethylene carbonate, monolithic microporous membranes are readily prepared with 25 μm thickness and pore sizes and porosities ranging from 6.8 to 22 nm and 15.4% to 38.5%, respectively. With 38.5% apparent porosity and an average pore size of 22 nm, the poly(1,4-butanediol diacrylate) (pBDDA) separator takes up 127% liquid electrolyte, resulting in an ionic conductivity of 1.98 mS cm–1, which is greater than in conventional Celgard 2500. Lithium ion battery half cells consisting of LiNi0.5Mn0.3Co0.2O2 cathodes and pBDDA separators were shown to undergo reversible charge/discharge cycling with an average discharge capacity of 142 mA h g–1 and a capacity retention of 98.4% over 100 cycles –more »
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States). Cell Analysis, Modeling and Prototyping (CAMP) Facility
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Science Foundation (NSF); USDOE
- OSTI Identifier:
- 1982228
- Alternate Identifier(s):
- OSTI ID: 1863102
- Grant/Contract Number:
- AC02-06CH11357; 1845805
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Materials Chemistry. A
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 19; Journal ID: ISSN 2050-7488
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Energy & Fuels; Materials Science
Citation Formats
Manly, Alexander J., and Tenhaeff, Wyatt E. One-step fabrication of robust lithium ion battery separators by polymerization-induced phase separation. United States: N. p., 2022.
Web. doi:10.1039/d1ta10730e.
Manly, Alexander J., & Tenhaeff, Wyatt E. One-step fabrication of robust lithium ion battery separators by polymerization-induced phase separation. United States. https://doi.org/10.1039/d1ta10730e
Manly, Alexander J., and Tenhaeff, Wyatt E. Fri .
"One-step fabrication of robust lithium ion battery separators by polymerization-induced phase separation". United States. https://doi.org/10.1039/d1ta10730e. https://www.osti.gov/servlets/purl/1982228.
@article{osti_1982228,
title = {One-step fabrication of robust lithium ion battery separators by polymerization-induced phase separation},
author = {Manly, Alexander J. and Tenhaeff, Wyatt E.},
abstractNote = {Conventional lithium ion battery separators are microporous polyolefin membranes that play a passive role in the electrochemical cell. Next generation separators should offer significant performance enhancements, while being fabricated through facile, low cost approaches with the ability to readily tune physicochemical properties. This study presents a single-step manufacturing technique based on UV-initiated polymerization-induced phase separation (PIPS), wherein microporous separators are fabricated from multifunctional monomers and ethylene carbonate (EC), which functions as both the pore-forming agent (porogen) and electrolyte component in the electrochemical cell. By controlling the ratio of the 1,4-butanediol diacrylate (BDDA) monomer to ethylene carbonate, monolithic microporous membranes are readily prepared with 25 μm thickness and pore sizes and porosities ranging from 6.8 to 22 nm and 15.4% to 38.5%, respectively. With 38.5% apparent porosity and an average pore size of 22 nm, the poly(1,4-butanediol diacrylate) (pBDDA) separator takes up 127% liquid electrolyte, resulting in an ionic conductivity of 1.98 mS cm–1, which is greater than in conventional Celgard 2500. Lithium ion battery half cells consisting of LiNi0.5Mn0.3Co0.2O2 cathodes and pBDDA separators were shown to undergo reversible charge/discharge cycling with an average discharge capacity of 142 mA h g–1 and a capacity retention of 98.4% over 100 cycles – comparable to cells using state-of-the-art separators. Moreover, similar discharge capacities were achieved in rate performance tests due to the high ionic conductivity and electrolyte uptake of the film. Finally, the pBDDA separators were shown to be thermally stable to 374 °C, lack low temperature thermal transitions that can compromise cell safety, and exhibit no thermal shrinkage up to 150 °C.},
doi = {10.1039/d1ta10730e},
journal = {Journal of Materials Chemistry. A},
number = 19,
volume = 10,
place = {United States},
year = {Fri Apr 08 00:00:00 EDT 2022},
month = {Fri Apr 08 00:00:00 EDT 2022}
}
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Fig. 1 : Outline of the fabrication of a porous monolith using monomer 1,4-butanediol diacrylate (BDDA) and porogen ethylene carbonate (EC). UV polymerization induces a microphase separation and results in a porous film that is incorporated into an electrochemical cell.
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