Volume 136, Issue 52 e202412434
Forschungsartikel

Organic Cationic-Coordinated Perfluoropolymer Electrolytes with Strong Li+-Solvent Interaction for Solid State Li-Metal Batteries

Shi Wang

Shi Wang

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

These authors contributed equally to this work.

Contribution: Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (lead), Writing - original draft (lead), Writing - review & editing (supporting)

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Shijun Xiao

Shijun Xiao

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

These authors contributed equally to this work.

Contribution: Data curation (equal), Formal analysis (equal), ​Investigation (equal), Methodology (equal), Writing - original draft (equal)

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Shuanghan Li

Shuanghan Li

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Data curation (supporting), Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting), Writing - original draft (supporting)

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Chao Liu

Chao Liu

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Data curation (supporting), Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting), Writing - original draft (supporting)

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Henan Cai

Henan Cai

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Data curation (supporting), Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting), Writing - original draft (supporting)

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Wenqing Sun

Wenqing Sun

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Data curation (supporting), Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting)

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Zhen-Dong Huang

Zhen-Dong Huang

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Data curation (supporting), Formal analysis (supporting), ​Investigation (supporting), Methodology (supporting)

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Wen-Yong Lai

Corresponding Author

Wen-Yong Lai

State Key Laboratory of Organic Electronics and Information Displays (SKLOEID), Institute of Advanced Materials (IAM), School of Chemistry and Life Sciences, Nanjing University of Posts & Telecommunications, 9 Wenyuan Road, Nanjing, 210023 China

Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Funding acquisition (lead), Project administration (lead), Resources (lead), Supervision (lead), Writing - review & editing (lead)

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First published: 23 August 2024

Abstract

The practical application of solid-state polymer lithium-metal batteries (LMBs) is plagued by the inferior ionic conductivity of the applied polymer electrolytes (PEs), which is caused by the coupling of ion transport with the motion of polymer segments. Here, solvated molecules based on ionic liquid and lithium salt with strong Li+-solvent interaction are inserted into an elaborately engineered perfluoropolymer electrolyte via ionic dipole interaction, extensively facilitating Li+ transport and improving mechanical properties. The intensified formation of solvation structures of contact ion pairs and ionic aggregates, as well as the strong electron-withdrawal properties of the F atoms in perfluoropolymers, give the PE high electrochemical stability and excellent interfacial stability. As a result, Li||Li symmetric cells demonstrate a lifetime of 2500 h and an exceptionally high critical current density above 2.3 mA cm−2, Li||LiFePO4 batteries exhibit consistent cycling for 550 cycles at 10 C, and Li||uncoated LiNi0.8Co0.1Mn0.1O2 cells achieve 1000 cycles at 0.5 C with an average Coulombic efficiency of 98.45 %, one of the best results reported to date based on PEs. Our discovery sheds fresh light on the targeted synergistic regulation of the electro-chemo-mechanical properties of PEs to extend the cycle life of LMBs.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

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