Volume 136, Issue 41 e202317016
Forschungsartikel

Enhancing Anion-Selective Catalysis for Stable Lithium Metal Pouch Cells through Charge Separated COF Interlayer

Dr. Peiyu Zhao

Dr. Peiyu Zhao

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

Thses anthors contributed equally to this work.

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Yanhua Zhang

Yanhua Zhang

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

Thses anthors contributed equally to this work.

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Dr. Baoyu Sun

Dr. Baoyu Sun

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

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Rui Qiao

Rui Qiao

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

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Dr. Chao Li

Dr. Chao Li

Instrumental Analysis Center, Xi'an Jiaotong University, 710049 Xi'an, China

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Pengqi Hai

Pengqi Hai

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

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Yingche Wang

Yingche Wang

Xi'an Institute of Electromechanical Information Technology, 710065 Xi'an, China

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Prof. Feng Liu

Prof. Feng Liu

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

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Prof. Jiangxuan Song

Corresponding Author

Prof. Jiangxuan Song

State Key Laboratory for Mechanical Behavior of Materials, Shaanxi International Research Center for Soft Matter, Xi'an Jiaotong University, 710049 Xi'an, China

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First published: 06 September 2024

Abstract

Regulating the composition of solid-electrolyte-interphase (SEI) is the key to construct high-energy density lithium metal batteries. Here we report a selective catalysis anionic decomposition strategy to achieve a lithium fluoride (LiF)-rich SEI for stable lithium metal batteries. To accomplish this, the tris(4-aminophenyl) amine-pyromeletic dianhydride covalent organic frameworks (TP-COF) was adopted as an interlayer on lithium metal anode. The strong donor-acceptor unit structure of TP-COF induces local charge separation, resulting in electron depletion and thus boosting its affinity to FSI. The strong interaction between TP-COF and FSI lowers the lowest unoccupied molecular orbital (LUMO) energy level of FSI, accelerating the decomposition of FSI and generating a stable LiF-rich SEI. This feature facilitates rapid Li+ transfer and suppresses dendritic Li growth. Notably, we demonstrate a 6.5 Ah LiNi0.8Co0.1Mn0.1O2|TP-COF@Li pouch cell with high energy density (473.4 Wh kg−1) and excellent cycling stability (97.4 %, 95 cycles) under lean electrolyte 1.39 g Ah−1, high areal capacity 5.7 mAh cm−2, and high current density 2.7 mA cm−2. Our selective catalysis strategy opens a promising avenue toward the practical applications of high energy-density rechargeable batteries.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

Research data are not shared.

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