Improved Li<sup>+</sup>Transport in Polyacetal Electrolytes: Conductivity and Current Fraction in a Series of Polymers

Snyder, RL; Choo, Y; Gao, KW; Halat, DM; Abel, BA; Sundararaman, S; Prendergast, D; Reimer, JA; Balsara, NP; Coates, GW

Improved Li<sup>+</sup>Transport in Polyacetal Electrolytes: Conductivity and Current Fraction in a Series of Polymers

Snyder, RL Choo, Y

Gao, KW Halat, DM Abel, BA Sundararaman, S Prendergast, D Reimer, JA Balsara, NP Coates, GW

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Publisher:: AMER CHEMICAL SOC
Publication Type:: Journal Article
Citation:: ACS Energy Letters, 2021, 6, (5), pp. 1886-1891
Issue Date:: 2021-05-14

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Field	Value	Language
dc.contributor.author	Snyder, RL
dc.contributor.author	Choo, Y https://orcid.org/0000-0003-2715-0618
dc.contributor.author	Gao, KW
dc.contributor.author	Halat, DM
dc.contributor.author	Abel, BA
dc.contributor.author	Sundararaman, S
dc.contributor.author	Prendergast, D
dc.contributor.author	Reimer, JA
dc.contributor.author	Balsara, NP
dc.contributor.author	Coates, GW
dc.date.accessioned	2022-05-04T22:20:36Z
dc.date.available	2022-05-04T22:20:36Z
dc.date.issued	2021-05-14
dc.identifier.citation	ACS Energy Letters, 2021, 6, (5), pp. 1886-1891
dc.identifier.issn	2380-8195
dc.identifier.issn	2380-8195
dc.identifier.uri	http://hdl.handle.net/10453/157021
dc.description.abstract	Polymer electrolytes mitigate safety concerns surrounding flammable liquid electrolytes in lithium-ion batteries. Poly(ethylene oxide) (PEO) electrolytes demonstrate viable conductivity values (∼1 × 10-3 S/cm) at elevated temperatures (>70 °C) but a relatively low Li+ current fraction (≤0.2) because strong Li+ coordination inhibits cation mobility. We have developed a series of polyacetal electrolytes by systematically varying methylene oxide (MO) and ethylene oxide (EO) units in the polymer backbone. These materials maintain high oxygen-to-carbon ratios like PEO but offer improved ion transport, revealing trends of decreasing conductivity and increasing current fraction with respect to polymer composition. In particular, the increasing current fraction measured via the Bruce-Vincent method suggests that MO units improve Li+ mobility relative to anion mobility. We calculate an overall efficacy (product of conductivity and current fraction) for each polymer/salt composition and identify two polymers - P(EO-MO) and P(EO-2MO) - that outperform PEO at high and low salt concentrations, respectively.
dc.language	English
dc.publisher	AMER CHEMICAL SOC
dc.relation.ispartof	ACS Energy Letters
dc.relation.isbasedon	10.1021/acsenergylett.1c00594
dc.rights	info:eu-repo/semantics/closedAccess
dc.title	Improved Li<sup>+</sup>Transport in Polyacetal Electrolytes: Conductivity and Current Fraction in a Series of Polymers
dc.type	Journal Article
utslib.citation.volume	6
pubs.organisational-group	/University of Technology Sydney
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology
pubs.organisational-group	/University of Technology Sydney/Faculty of Engineering and Information Technology/School of Civil and Environmental Engineering
utslib.copyright.status	closed_access	*
dc.date.updated	2022-05-04T22:20:34Z
pubs.issue	5
pubs.publication-status	Published
pubs.volume	6
utslib.citation.issue	5

Abstract:

Polymer electrolytes mitigate safety concerns surrounding flammable liquid electrolytes in lithium-ion batteries. Poly(ethylene oxide) (PEO) electrolytes demonstrate viable conductivity values (∼1 × 10-3 S/cm) at elevated temperatures (>70 °C) but a relatively low Li+ current fraction (≤0.2) because strong Li+ coordination inhibits cation mobility. We have developed a series of polyacetal electrolytes by systematically varying methylene oxide (MO) and ethylene oxide (EO) units in the polymer backbone. These materials maintain high oxygen-to-carbon ratios like PEO but offer improved ion transport, revealing trends of decreasing conductivity and increasing current fraction with respect to polymer composition. In particular, the increasing current fraction measured via the Bruce-Vincent method suggests that MO units improve Li+ mobility relative to anion mobility. We calculate an overall efficacy (product of conductivity and current fraction) for each polymer/salt composition and identify two polymers - P(EO-MO) and P(EO-2MO) - that outperform PEO at high and low salt concentrations, respectively.

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http://hdl.handle.net/10453/157021