Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics

Sheng Zhao; Yiman Zhang; Hoang Pham; Jan Michael Y. Carrillo; Bobby G. Sumpter; Jagjit Nanda; Nancy J. Dudney; Tomonori Saito; Alexei P. Sokolov; Peng Fei Cao

doi:10.1021/acsaem.0c02079

Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics

Sheng Zhao
, Yiman Zhang
, Hoang Pham
, Jan Michael Y. Carrillo
, Bobby G. Sumpter
, Jagjit Nanda
, Nancy J. Dudney
, Tomonori Saito
, Alexei P. Sokolov
, Peng Fei Cao

Research output: Contribution to journal › Article › peer-review

50 Scopus citations

Abstract

Single-ion conducting polymer electrolytes (SICPEs) have many advantages for solid-state battery applications, while low conductivities remain the bottleneck for their practical applications. Herein, a strategy that can significantly improve the ionic conductivity of SICPEs based on the concept of accelerated segmental dynamics was demonstrated by the evaluation of the thermal property, rheological behavior, morphology analysis, molecular dynamics simulation, and conductivity performance. With both "soft"poly(dimethylsiloxane) (PDMS) backbone and poly(ethylene glycol) (PEG) side chains, the obtained SICPE possesses faster segmental relaxation and higher lithium-ion conductivity. With lithium "transference"number close to unity, the obtained SICPE also shows excellent electrochemical stability against lithium metal electrodes. The clear relationship established between the segmental dynamics of polymer electrolyte and its ionic conductivity should contribute to achieve a solid electrolyte with improved ionic conductivity toward the next-generation solid-state battery.

Original language	English
Pages (from-to)	12540-12548
Number of pages	9
Journal	ACS Applied Energy Materials
Volume	3
Issue number	12
DOIs	https://doi.org/10.1021/acsaem.0c02079
State	Published - Dec 28 2020

Funding

This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division. J.N. and Y.Z. acknowledge support from Asst. Secretary, Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) under the Advanced Battery Materials Research (BMR) Program. The computational/simulation aspect of this work was performed at the Center for Nanophase Materials Sciences, a U.S. Department of Energy Office of Science User Facility. This research also used resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract DE-AC05-00OR22725.

Keywords

"soft" structure
poly(dimethylsiloxane)
polymer electrolyte
segmental dynamics
single ion conducting

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10.1021/acsaem.0c02079

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title = "Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics",

abstract = "Single-ion conducting polymer electrolytes (SICPEs) have many advantages for solid-state battery applications, while low conductivities remain the bottleneck for their practical applications. Herein, a strategy that can significantly improve the ionic conductivity of SICPEs based on the concept of accelerated segmental dynamics was demonstrated by the evaluation of the thermal property, rheological behavior, morphology analysis, molecular dynamics simulation, and conductivity performance. With both {"}soft{"}poly(dimethylsiloxane) (PDMS) backbone and poly(ethylene glycol) (PEG) side chains, the obtained SICPE possesses faster segmental relaxation and higher lithium-ion conductivity. With lithium {"}transference{"}number close to unity, the obtained SICPE also shows excellent electrochemical stability against lithium metal electrodes. The clear relationship established between the segmental dynamics of polymer electrolyte and its ionic conductivity should contribute to achieve a solid electrolyte with improved ionic conductivity toward the next-generation solid-state battery.",

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doi = "10.1021/acsaem.0c02079",

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AU - Pham, Hoang

AU - Carrillo, Jan Michael Y.

AU - Sumpter, Bobby G.

AU - Nanda, Jagjit

AU - Dudney, Nancy J.

AU - Saito, Tomonori

AU - Sokolov, Alexei P.

AU - Cao, Peng Fei

N1 - Publisher Copyright: ©

PY - 2020/12/28

Y1 - 2020/12/28

N2 - Single-ion conducting polymer electrolytes (SICPEs) have many advantages for solid-state battery applications, while low conductivities remain the bottleneck for their practical applications. Herein, a strategy that can significantly improve the ionic conductivity of SICPEs based on the concept of accelerated segmental dynamics was demonstrated by the evaluation of the thermal property, rheological behavior, morphology analysis, molecular dynamics simulation, and conductivity performance. With both "soft"poly(dimethylsiloxane) (PDMS) backbone and poly(ethylene glycol) (PEG) side chains, the obtained SICPE possesses faster segmental relaxation and higher lithium-ion conductivity. With lithium "transference"number close to unity, the obtained SICPE also shows excellent electrochemical stability against lithium metal electrodes. The clear relationship established between the segmental dynamics of polymer electrolyte and its ionic conductivity should contribute to achieve a solid electrolyte with improved ionic conductivity toward the next-generation solid-state battery.

AB - Single-ion conducting polymer electrolytes (SICPEs) have many advantages for solid-state battery applications, while low conductivities remain the bottleneck for their practical applications. Herein, a strategy that can significantly improve the ionic conductivity of SICPEs based on the concept of accelerated segmental dynamics was demonstrated by the evaluation of the thermal property, rheological behavior, morphology analysis, molecular dynamics simulation, and conductivity performance. With both "soft"poly(dimethylsiloxane) (PDMS) backbone and poly(ethylene glycol) (PEG) side chains, the obtained SICPE possesses faster segmental relaxation and higher lithium-ion conductivity. With lithium "transference"number close to unity, the obtained SICPE also shows excellent electrochemical stability against lithium metal electrodes. The clear relationship established between the segmental dynamics of polymer electrolyte and its ionic conductivity should contribute to achieve a solid electrolyte with improved ionic conductivity toward the next-generation solid-state battery.

KW - "soft" structure

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KW - polymer electrolyte

KW - segmental dynamics

KW - single ion conducting

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ER -

Improved Single-Ion Conductivity of Polymer Electrolyte via Accelerated Segmental Dynamics

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