Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes
Abstract
The interfacial region where ion-transporting polymer chains are anchored to a hard, insulating phase is a major factor dictating the limits of ion-conduction in nanostructure-forming electrolytes. In this work, we investigate the effect of an end-grafted poly(ethylene oxide) (20 kg mol–1) surface on the ionic conductivity σ of PEO and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt mixtures. Specifically, we characterize nanothin films in the range of ca. 10 to 250 nm, which amplify the contributions from the polymer/substrate interface that dictate any deviations from expected bulk conductivity σbulk values. Conductivity measurements reveal a monotonic decrease in σ upon decreasing film thickness at all values of r (r = molar ratio of Li+ to EO units). The reduction from bulk-like σ occurs for film thicknesses approximately 100 nm and below for all values of r. This trend in conductivity arises from the presence of the underlying grafted-PEO layer. Through a thickness dependence normalized conductivity study, we observe nanoscale constraints leading to deviation from intrinsic conductivity of bulk PEO–LiTFSI electrolytes. Here, these nanoscale constraints correspond to an immobile interfacial zone whose thickness hint ranges from 9.5 ± 1.4 nm at r = 0.01 to 2.9 ± 1.5 nm at r = 0.15 in ourmore »
- Authors:
-
[1];
[1];
[2];
[1];
[1];
[3];
[1];
[2];
[4]
- Univ. of Chicago, Chicago, IL (United States)
- Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1559000
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Molecular Systems Design & Engineering
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2058-9689
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; PEO-LiTFSI thin film conductivity; interdigitated electrodes; polymer/substrate interfaces; thickness dependence
Citation Formats
Dong, Ban Xuan, Bennington, Peter, Kambe, Yu, Sharon, Daniel, Dolejsi, Moshe, Strzalka, Joseph, Burnett, Veronica F., Nealey, Paul F., and Patel, Shrayesh N. Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes. United States: N. p., 2019.
Web. doi:10.1039/C9ME00011A.
Dong, Ban Xuan, Bennington, Peter, Kambe, Yu, Sharon, Daniel, Dolejsi, Moshe, Strzalka, Joseph, Burnett, Veronica F., Nealey, Paul F., & Patel, Shrayesh N. Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes. United States. https://doi.org/10.1039/C9ME00011A
Dong, Ban Xuan, Bennington, Peter, Kambe, Yu, Sharon, Daniel, Dolejsi, Moshe, Strzalka, Joseph, Burnett, Veronica F., Nealey, Paul F., and Patel, Shrayesh N. Mon .
"Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes". United States. https://doi.org/10.1039/C9ME00011A. https://www.osti.gov/servlets/purl/1559000.
@article{osti_1559000,
title = {Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes},
author = {Dong, Ban Xuan and Bennington, Peter and Kambe, Yu and Sharon, Daniel and Dolejsi, Moshe and Strzalka, Joseph and Burnett, Veronica F. and Nealey, Paul F. and Patel, Shrayesh N.},
abstractNote = {The interfacial region where ion-transporting polymer chains are anchored to a hard, insulating phase is a major factor dictating the limits of ion-conduction in nanostructure-forming electrolytes. In this work, we investigate the effect of an end-grafted poly(ethylene oxide) (20 kg mol–1) surface on the ionic conductivity σ of PEO and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt mixtures. Specifically, we characterize nanothin films in the range of ca. 10 to 250 nm, which amplify the contributions from the polymer/substrate interface that dictate any deviations from expected bulk conductivity σbulk values. Conductivity measurements reveal a monotonic decrease in σ upon decreasing film thickness at all values of r (r = molar ratio of Li+ to EO units). The reduction from bulk-like σ occurs for film thicknesses approximately 100 nm and below for all values of r. This trend in conductivity arises from the presence of the underlying grafted-PEO layer. Through a thickness dependence normalized conductivity study, we observe nanoscale constraints leading to deviation from intrinsic conductivity of bulk PEO–LiTFSI electrolytes. Here, these nanoscale constraints correspond to an immobile interfacial zone whose thickness hint ranges from 9.5 ± 1.4 nm at r = 0.01 to 2.9 ± 1.5 nm at r = 0.15 in our nanothin films that impedes ion transport. Overall, we have presented a robust platform that facilitates probing the role of polymer-grafted surfaces on the σ of polymer electrolytes.},
doi = {10.1039/C9ME00011A},
journal = {Molecular Systems Design & Engineering},
number = 3,
volume = 4,
place = {United States},
year = {2019},
month = {4}
}
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