Hybrid covalent organic-framework-based electrolytes for optimizing interface resistance in solid-state lithium-ion batteries

Dongming Cheng; Cui Sun; Zhongling Lang; Jinhua Zhang; Ajuan Hu; Jianing Duan; Xinyu Chen; Hong-Ying Zang; Jiajia Chen; Mingsen Zheng; Quanfeng Dong

Cell Reports Physical Science (Mar 2022)

Hybrid covalent organic-framework-based electrolytes for optimizing interface resistance in solid-state lithium-ion batteries

Dongming Cheng,
Cui Sun,
Zhongling Lang,
Jinhua Zhang,
Ajuan Hu,
Jianing Duan,
Xinyu Chen,
Hong-Ying Zang,
Jiajia Chen,
Mingsen Zheng,
Quanfeng Dong

Affiliations

Dongming Cheng: Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education at Universities of Jilin Province, Faculty of Chemistry, Northeast Normal University, Changchun, 130024 Jilin, China
Cui Sun: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Zhongling Lang: Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education at Universities of Jilin Province, Faculty of Chemistry, Northeast Normal University, Changchun, 130024 Jilin, China
Jinhua Zhang: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Ajuan Hu: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Jianing Duan: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Xinyu Chen: Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education at Universities of Jilin Province, Faculty of Chemistry, Northeast Normal University, Changchun, 130024 Jilin, China
Hong-Ying Zang: Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education at Universities of Jilin Province, Faculty of Chemistry, Northeast Normal University, Changchun, 130024 Jilin, China; Corresponding author
Jiajia Chen: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Mingsen Zheng: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China
Quanfeng Dong: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen, 361005 Fujian, China

Journal volume & issue: Vol. 3, no. 3
p. 100731

Abstract

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Summary: High ion conductivity and low electrode-electrolyte interface resistance are intensively pursued topics for the development of solid-state Li-ion batteries with high safety and energy density. Here, we propose a design using keto-enamine covalent organic frameworks (TPBD) and polyethylene oxide (PEO) to prepare a solid-state electrolyte (TPBD-LiPF6@PEO), achieving a high ion conductivity of 0.543 mS cm−1 at 25°C and optimizing the electrode-electrolyte interface resistance in Li-ion batteries. Solid-state nuclear magnetic resonance experiments and density functional theory calculations show that the strong interaction between the –C=O site in TPBD and Li+ ions promotes the dissociation of LiPF6. The assembled LiFePO4|TPBD-LiPF6@PEO|Li batteries without using liquid electrolytes offer a specific capacity of nearly 140 mAh g−1 at 0.2 C with a columbic efficiency of 99.6% after 200 cycles at 25°C. This strategy for preparing solid-state electrolytes provides practical ideas and suggestions in the development of solid-state energy devices.

Published in Cell Reports Physical Science

ISSN: 2666-3864 (Online)
Publisher: Elsevier
Country of publisher: United States
LCC subjects: Science: Physics
Website: https://www.cell.com/cell-reports-physical-science

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