Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes

Dong, Ban Xuan; Bennington, Peter; Kambe, Yu; Sharon, Daniel; Dolejsi, Moshe; Strzalka, Joseph; Burnett, Veronica F.; Nealey, Paul F.; Patel, Shrayesh N.

doi:10.1039/C9ME00011A

Title: Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes

Journal Article · 01 April 2019 · Molecular Systems Design & Engineering

DOI: https://doi.org/10.1039/C9ME00011A · OSTI ID:1559000

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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)

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 σ_bulk 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 h_int 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1559000

Journal Information:: Molecular Systems Design & Engineering, Vol. 4, Issue 3; ISSN 2058-9689

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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PEO-LiTFSI thin film conductivity
interdigitated electrodes
polymer/substrate interfaces
thickness dependence

Title: Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes

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