Volume 63, Issue 24 e202403661
Research Article

Revealing the Influence of Electron Migration Inside Polymer Electrolyte on Li+ Transport and Interphase Reconfiguration for Li Metal Batteries

Dr. Yingmin Jin

Dr. Yingmin Jin

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 China

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Ruifan Lin

Ruifan Lin

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 China

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Yumeng Li

Yumeng Li

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 China

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Xuebai Zhang

Xuebai Zhang

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 China

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Dr. Siping Tan

Dr. Siping Tan

State Key Laboratory of Advanced Chemical Power Sources, Guizhou Meiling Power Sources Co. Ltd., Zunyi, Guizhou, 563003 China

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Prof. Yong Shuai

Corresponding Author

Prof. Yong Shuai

Key Laboratory of Aerospace Thermophysics of MIIT, School of Energy Science and Engineering, Harbin Institute of Technology, Harbin, 150001 China

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Prof. Yueping Xiong

Corresponding Author

Prof. Yueping Xiong

MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001 China

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First published: 13 April 2024
Citations: 36

Graphical Abstract

In this work, La0.6Sr0.4CoO3−δ (LSC) enriched with high valence-state Co species and oxygen vacancies is developed as electronically conductive nanofillers embedded within ZnO/Zn3N2-functionalized polyimide nanofiber framework to establish Li+ transport highways for poly vinylene carbonate electrolyte and eliminate nonuniform Li deposits.

Abstract

The development of highly producible and interfacial compatible in situ polymerized electrolytes for solid-state lithium metal batteries (SSLMBs) have been plagued by insufficient transport kinetics and uncontrollable dendrite propagation. Herein, we seek to explore a rationally designed nanofiber architecture to balance all the criteria of SSLMBs, in which La0.6Sr0.4CoO3−δ (LSC) enriched with high valence-state Co species and oxygen vacancies is developed as electronically conductive nanofillers embedded within ZnO/Zn3N2-functionalized polyimide (Zn-PI) nanofiber framework for the first time, to establish Li+ transport highways for poly vinylene carbonate (PVC) electrolyte and eliminate nonuniform Li deposits. Revealed by characterization and theoretical calculation under electric field, the positive-negative electrical dipole layer in LSC derived from electron migration between Co and O atoms aids in accelerating Li+ diffusion kinetics through densified electric field around filler particle, featuring a remarkable ionic conductivity of 1.50 mS cm−1 at 25 °C and a high Li+ transference number of 0.91 without the risk of electron leakage. Integrating with the preferential sacrifice of ZnO/Zn3N2 on PI nanofiber upon immediate detection of dendritic Li, which takes part in reconfiguring hierarchical SEI chemistry dominated by LixNy/Li−Zn alloy inner layer and LiF outer layer, SSLMBs are further endowed with prolonged cycling lifespan and exceptional rate capability.

Conflict of interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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