Revealing the Anion Chemistry Effect on Transport Properties of Ternary Gel Polymer Electrolytes

Maria Martinez-Ibañez; Nicola Boaretto; Leire Meabe; Xiaoen Wang; Haijin Zhu; Alexander Santiago; Oihane Zugazua; Maria Forsyth; Michel Armand; Heng Zhang

doi:10.1021/acs.chemmater.2c00260

Revealing the Anion Chemistry Effect on Transport Properties of Ternary Gel Polymer Electrolytes

Maria Martinez-Ibañez^*, Nicola Boaretto, Leire Meabe, Xiaoen Wang, Haijin Zhu, Alexander Santiago, Oihane Zugazua, Maria Forsyth, Michel Armand, Heng Zhang

^*Corresponding author for this work

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

Abstract

Gel polymer electrolytes (GPEs) are promising candidates to enable safe and room temperature lithium metal (Li°) polymer batteries (LMPBs). Among the different available plasticizers, ionic liquids (ILs) have captured much interest due to their extremely low vapor pressure and high chemical, thermal, and electrochemical stability. Plasticizing polymerized ionic liquid (PIL)-based electrolytes with ILs may lead to intrinsically safe and highly ionically conductive GPEs even at low temperature. Herein, we report the fundamental properties of some representative PIL-based GPEs utilizing sulfonimide anions ([N(SO2RF1)(SO2RF2)]- RF1, RF2 = F or CF3), with the goal to provide a detailed understanding of the diffusion and conduction properties of this intriguing electrolyte family when different anions are involved. Our results suggest that the full bis(fluorosulfonyl)imide (FSI)-based system exhibits higher ionic conductivities and better selectivity in cationic transport as compared to other systems, due to the higher mobility of free ions and the lower content in ion aggregates. It is anticipated that the present work may set the course to design new GPEs rendering an overall improved electrochemical performance.

Original language	English
Pages (from-to)	7493-7502
Number of pages	10
Journal	Chemistry of Materials
Volume	34
Issue number	16
DOIs	https://doi.org/10.1021/acs.chemmater.2c00260
State	Published - 23 Aug 2022
Externally published	Yes

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title = "Revealing the Anion Chemistry Effect on Transport Properties of Ternary Gel Polymer Electrolytes",

abstract = "Gel polymer electrolytes (GPEs) are promising candidates to enable safe and room temperature lithium metal (Li°) polymer batteries (LMPBs). Among the different available plasticizers, ionic liquids (ILs) have captured much interest due to their extremely low vapor pressure and high chemical, thermal, and electrochemical stability. Plasticizing polymerized ionic liquid (PIL)-based electrolytes with ILs may lead to intrinsically safe and highly ionically conductive GPEs even at low temperature. Herein, we report the fundamental properties of some representative PIL-based GPEs utilizing sulfonimide anions ([N(SO2RF1)(SO2RF2)]- RF1, RF2 = F or CF3), with the goal to provide a detailed understanding of the diffusion and conduction properties of this intriguing electrolyte family when different anions are involved. Our results suggest that the full bis(fluorosulfonyl)imide (FSI)-based system exhibits higher ionic conductivities and better selectivity in cationic transport as compared to other systems, due to the higher mobility of free ions and the lower content in ion aggregates. It is anticipated that the present work may set the course to design new GPEs rendering an overall improved electrochemical performance.",

author = "Maria Martinez-Iba{\~n}ez and Nicola Boaretto and Leire Meabe and Xiaoen Wang and Haijin Zhu and Alexander Santiago and Oihane Zugazua and Maria Forsyth and Michel Armand and Heng Zhang",

note = "Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = aug,

day = "23",

doi = "10.1021/acs.chemmater.2c00260",

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T1 - Revealing the Anion Chemistry Effect on Transport Properties of Ternary Gel Polymer Electrolytes

AU - Martinez-Ibañez, Maria

AU - Boaretto, Nicola

AU - Meabe, Leire

AU - Wang, Xiaoen

AU - Zhu, Haijin

AU - Santiago, Alexander

AU - Zugazua, Oihane

AU - Forsyth, Maria

AU - Armand, Michel

AU - Zhang, Heng

PY - 2022/8/23

Y1 - 2022/8/23

N2 - Gel polymer electrolytes (GPEs) are promising candidates to enable safe and room temperature lithium metal (Li°) polymer batteries (LMPBs). Among the different available plasticizers, ionic liquids (ILs) have captured much interest due to their extremely low vapor pressure and high chemical, thermal, and electrochemical stability. Plasticizing polymerized ionic liquid (PIL)-based electrolytes with ILs may lead to intrinsically safe and highly ionically conductive GPEs even at low temperature. Herein, we report the fundamental properties of some representative PIL-based GPEs utilizing sulfonimide anions ([N(SO2RF1)(SO2RF2)]- RF1, RF2 = F or CF3), with the goal to provide a detailed understanding of the diffusion and conduction properties of this intriguing electrolyte family when different anions are involved. Our results suggest that the full bis(fluorosulfonyl)imide (FSI)-based system exhibits higher ionic conductivities and better selectivity in cationic transport as compared to other systems, due to the higher mobility of free ions and the lower content in ion aggregates. It is anticipated that the present work may set the course to design new GPEs rendering an overall improved electrochemical performance.

AB - Gel polymer electrolytes (GPEs) are promising candidates to enable safe and room temperature lithium metal (Li°) polymer batteries (LMPBs). Among the different available plasticizers, ionic liquids (ILs) have captured much interest due to their extremely low vapor pressure and high chemical, thermal, and electrochemical stability. Plasticizing polymerized ionic liquid (PIL)-based electrolytes with ILs may lead to intrinsically safe and highly ionically conductive GPEs even at low temperature. Herein, we report the fundamental properties of some representative PIL-based GPEs utilizing sulfonimide anions ([N(SO2RF1)(SO2RF2)]- RF1, RF2 = F or CF3), with the goal to provide a detailed understanding of the diffusion and conduction properties of this intriguing electrolyte family when different anions are involved. Our results suggest that the full bis(fluorosulfonyl)imide (FSI)-based system exhibits higher ionic conductivities and better selectivity in cationic transport as compared to other systems, due to the higher mobility of free ions and the lower content in ion aggregates. It is anticipated that the present work may set the course to design new GPEs rendering an overall improved electrochemical performance.

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DO - 10.1021/acs.chemmater.2c00260

M3 - 文章

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SN - 0897-4756

VL - 34

SP - 7493

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JO - Chemistry of Materials

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Revealing the Anion Chemistry Effect on Transport Properties of Ternary Gel Polymer Electrolytes

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