Enthalpic and Entropic Contributions to Fast Lithium Ion Conduction in Solid-State Aqueous Polymer Electrolytes

Jae Hyun Park; Sungyeb Jung; Puji Lestari Handayani; Narayana Aluru; Taehoon Kim; Sang Bok Lee; U. Hyeok Choi; Jaekwang Lee

doi:10.1021/acs.jpcc.2c03513

Enthalpic and Entropic Contributions to Fast Lithium Ion Conduction in Solid-State Aqueous Polymer Electrolytes

Jae Hyun Park, Sungyeb Jung, Puji Lestari Handayani, Narayana Aluru, Taehoon Kim, Sang Bok Lee, U. Hyeok Choi, Jaekwang Lee

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5 Scopus citations

Abstract

Solid-state aqueous polymer electrolytes (SAPEs), a mixture of hydrophilic polymers and an appropriate amount of water, can produce high Li-ion conductivity while maintaining a solid state. Also, they can overcome the limitations of normal solid electrolytes. This study reports that the very high SAPE ionic conductivity (∼10 mS/cm at T = 298.15 K) originates from a low energy barrier (∼0.28 eV) closely correlated with water-filled ion passages in the medium. The low energy barrier is ascribed to a considerable reduction of the enthalpic barrier due to water addition despite a growth of the entropic barrier incurred by the negative nature of entropy change across water tubes. The extremely high ionic conductivity, coupled with an exceptionally low energy barrier, provides a unique advantage to SAPEs over conventional solid electrolytes.

Original language	English
Pages (from-to)	16777-16784
Number of pages	8
Journal	Journal of Physical Chemistry C
Volume	126
Issue number	39
DOIs	https://doi.org/10.1021/acs.jpcc.2c03513
State	Published - 6 Oct 2022

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title = "Enthalpic and Entropic Contributions to Fast Lithium Ion Conduction in Solid-State Aqueous Polymer Electrolytes",

abstract = "Solid-state aqueous polymer electrolytes (SAPEs), a mixture of hydrophilic polymers and an appropriate amount of water, can produce high Li-ion conductivity while maintaining a solid state. Also, they can overcome the limitations of normal solid electrolytes. This study reports that the very high SAPE ionic conductivity (∼10 mS/cm at T = 298.15 K) originates from a low energy barrier (∼0.28 eV) closely correlated with water-filled ion passages in the medium. The low energy barrier is ascribed to a considerable reduction of the enthalpic barrier due to water addition despite a growth of the entropic barrier incurred by the negative nature of entropy change across water tubes. The extremely high ionic conductivity, coupled with an exceptionally low energy barrier, provides a unique advantage to SAPEs over conventional solid electrolytes.",

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AU - Park, Jae Hyun

AU - Jung, Sungyeb

AU - Handayani, Puji Lestari

AU - Aluru, Narayana

AU - Kim, Taehoon

AU - Lee, Sang Bok

AU - Choi, U. Hyeok

AU - Lee, Jaekwang

PY - 2022/10/6

Y1 - 2022/10/6

N2 - Solid-state aqueous polymer electrolytes (SAPEs), a mixture of hydrophilic polymers and an appropriate amount of water, can produce high Li-ion conductivity while maintaining a solid state. Also, they can overcome the limitations of normal solid electrolytes. This study reports that the very high SAPE ionic conductivity (∼10 mS/cm at T = 298.15 K) originates from a low energy barrier (∼0.28 eV) closely correlated with water-filled ion passages in the medium. The low energy barrier is ascribed to a considerable reduction of the enthalpic barrier due to water addition despite a growth of the entropic barrier incurred by the negative nature of entropy change across water tubes. The extremely high ionic conductivity, coupled with an exceptionally low energy barrier, provides a unique advantage to SAPEs over conventional solid electrolytes.

AB - Solid-state aqueous polymer electrolytes (SAPEs), a mixture of hydrophilic polymers and an appropriate amount of water, can produce high Li-ion conductivity while maintaining a solid state. Also, they can overcome the limitations of normal solid electrolytes. This study reports that the very high SAPE ionic conductivity (∼10 mS/cm at T = 298.15 K) originates from a low energy barrier (∼0.28 eV) closely correlated with water-filled ion passages in the medium. The low energy barrier is ascribed to a considerable reduction of the enthalpic barrier due to water addition despite a growth of the entropic barrier incurred by the negative nature of entropy change across water tubes. The extremely high ionic conductivity, coupled with an exceptionally low energy barrier, provides a unique advantage to SAPEs over conventional solid electrolytes.

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Enthalpic and Entropic Contributions to Fast Lithium Ion Conduction in Solid-State Aqueous Polymer Electrolytes

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