A Polymer Electrolyte with High Cationic Transport Number for Safe and Stable Solid Li-Metal Batteries

Xinyuan Shan; Madison Morey; Zhenxi Li; Sheng Zhao; Shenghan Song; Zhenxue Xiao; Hao Feng; Shilun Gao; Guoran Li; Alexei P. Sokolov; Emily Ryan; Kang Xu; Ming Tian; Yi He; Huabin Yang; Peng Fei Cao

doi:10.1021/acsenergylett.2c02349

A Polymer Electrolyte with High Cationic Transport Number for Safe and Stable Solid Li-Metal Batteries

Xinyuan Shan, Madison Morey, Zhenxi Li, Sheng Zhao, Shenghan Song, Zhenxue Xiao, Hao Feng, Shilun Gao, Guoran Li, Alexei P. Sokolov, Emily Ryan, Kang Xu, Ming Tian, Yi He, Huabin Yang, Peng Fei Cao

Soft Materials and Membranes

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

39 Scopus citations

Abstract

The strategies for achieving a high cationic transport polymer electrolyte (HTPE) have mostly focused on developing single-ion conducting polymer electrolytes, which is far from being practical due to sluggish ion transport. Herein, we present an unprecedented approach on designing an HTPE via in situ copolymerization of regular ionic conducting and single-ion conducting monomers in the presence of a lithium salt. The HTPE, i.e., poly(VEC10-r-LiSTFSI), exhibits a combination of impressive properties, including high cationic transport number (0.73), high ionic conductivity (1.60 mS cm^-1), tolerance of high current density (10 mA cm^-2), and high anodic stability (5 V). A lithium-metal battery constructed with the developed HTPE retains 70% capacity after 1200 cycles at 1 C, and it also operates in a wide temperature range and with a high mass loading of the cathode. Advanced characterizations and computations reveal that the high t_Li⁺and high ionic conductivity effectively suppress Li⁰-dendrite growth by circumventing concentration polarizations that plague most polymer electrolytes.

Original language	English
Pages (from-to)	4342-4351
Number of pages	10
Journal	ACS Energy Letters
Volume	7
Issue number	12
DOIs	https://doi.org/10.1021/acsenergylett.2c02349
State	Published - Dec 9 2022

Funding

This work was financially supported by the Natural Science Foundation of China (21421001), the Natural Science Foundation of Tianjin, China (18JCZDJC31400), and the MOE Innovation Team (IRT13022). This work was also supported by Fundamental Research Funds for the Central Universities (buctrc202222). A.P.S. acknowledges partial financial support on idea conception and manuscript revision by the US Department of Energy, Office of Science, Basic Energy Science, Material Science, and Engineering Division. Partial financial support for this research was provided by the National Science Foundation through award 2034154 and the Hariri Institute for Computing and Computational Science and Engineering at Boston University through their Focused Research Program.

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title = "A Polymer Electrolyte with High Cationic Transport Number for Safe and Stable Solid Li-Metal Batteries",

abstract = "The strategies for achieving a high cationic transport polymer electrolyte (HTPE) have mostly focused on developing single-ion conducting polymer electrolytes, which is far from being practical due to sluggish ion transport. Herein, we present an unprecedented approach on designing an HTPE via in situ copolymerization of regular ionic conducting and single-ion conducting monomers in the presence of a lithium salt. The HTPE, i.e., poly(VEC10-r-LiSTFSI), exhibits a combination of impressive properties, including high cationic transport number (0.73), high ionic conductivity (1.60 mS cm-1), tolerance of high current density (10 mA cm-2), and high anodic stability (5 V). A lithium-metal battery constructed with the developed HTPE retains 70% capacity after 1200 cycles at 1 C, and it also operates in a wide temperature range and with a high mass loading of the cathode. Advanced characterizations and computations reveal that the high tLi+and high ionic conductivity effectively suppress Li0-dendrite growth by circumventing concentration polarizations that plague most polymer electrolytes.",

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AU - Xiao, Zhenxue

AU - Feng, Hao

AU - Gao, Shilun

AU - Li, Guoran

AU - Sokolov, Alexei P.

AU - Ryan, Emily

AU - Xu, Kang

AU - Tian, Ming

AU - He, Yi

AU - Yang, Huabin

AU - Cao, Peng Fei

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AB - The strategies for achieving a high cationic transport polymer electrolyte (HTPE) have mostly focused on developing single-ion conducting polymer electrolytes, which is far from being practical due to sluggish ion transport. Herein, we present an unprecedented approach on designing an HTPE via in situ copolymerization of regular ionic conducting and single-ion conducting monomers in the presence of a lithium salt. The HTPE, i.e., poly(VEC10-r-LiSTFSI), exhibits a combination of impressive properties, including high cationic transport number (0.73), high ionic conductivity (1.60 mS cm-1), tolerance of high current density (10 mA cm-2), and high anodic stability (5 V). A lithium-metal battery constructed with the developed HTPE retains 70% capacity after 1200 cycles at 1 C, and it also operates in a wide temperature range and with a high mass loading of the cathode. Advanced characterizations and computations reveal that the high tLi+and high ionic conductivity effectively suppress Li0-dendrite growth by circumventing concentration polarizations that plague most polymer electrolytes.

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A Polymer Electrolyte with High Cationic Transport Number for Safe and Stable Solid Li-Metal Batteries

Abstract

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