Reactivating the Dead Lithium by Redox Shuttle to Promote the Efficient Utilization of Lithium for Anode Free Lithium Metal Batteries,Advanced Functional Materials

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Reactivating the Dead Lithium by Redox Shuttle to Promote the Efficient Utilization of Lithium for Anode Free Lithium Metal Batteries
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-06-04 , DOI: 10.1002/adfm.202301332
Yuhao Zhang ₁ , Jie Liu ₂ , Yufei Li ₃ , Dongchen Zhao ₄ , Wei Huang ₄ , Yiwei Zheng ₁ , Jinqiu Zhou ₂ , Changhao Zhu ₂ , Chengwei Deng ₅ , Yi Sun ₅ , Tao Qian _{2,

6} , Chenglin Yan _{1,

6}

Affiliation

Anode free lithium metal batteries (AFLMBs), as a kind of novel battery configuration with zero excess lithium, can improve the energy density to the limit compared with lithium metal batteries and effectively ensure the safety. However, the lifespan of AFLMBs is a tricky problem because there is no extra lithium source to compensate for the irreversible loss of active lithium, which is mainly caused by the continuous decomposition of electrolyte and the formation of dead lithium. Herein, a redox shuttle additive, which can be oxidized in the cathode and reduced in the electrolyte reversibly, is introduced to improve the lithium utilization and lifespan of AFLMBs by reactivating the dead lithium. During the charging process, the redox shuttle additive can be oxidized on the cathode surface and serve as electron acceptor toward dead lithium. The electrically isolated dead lithium in the electrolyte can be re-activated into active lithium ions when captured by oxidized redox shuttle additive.As a result, electrolyte with redox shuttle achieves average higher coulombic efficiency of 99.13% than electrolyte without redox shuttle (97.71%). In addition, the AFLMB with redox shuttle exhibits improved cycling performance with extended lifespan.

中文翻译：

利用氧化还原穿梭重新激活死锂促进无阳极锂金属电池锂的高效利用

无阳极锂金属电池（AFLMBs）作为一种零过量锂的新型电池配置，与锂金属电池相比，可以将能量密度提高到极限，并有效保证安全性。然而，AFLMB的寿命是一个棘手的问题，因为没有额外的锂源来补偿活性锂的不可逆损失，这主要是由于电解质的持续分解和死锂的形成造成的。本文引入了一种氧化还原梭添加剂，它可以在阴极中可逆地氧化并在电解质中可逆地还原，通过重新激活死锂来提高AFLMB的锂利用率和寿命。在充电过程中，氧化还原梭添加剂可以在正极表面被氧化，并充当死锂的电子受体。当电解液中电隔离的死锂被氧化的氧化还原梭添加剂捕获时，可以重新激活为活性锂离子。因此，具有氧化还原梭的电解液比不具有氧化还原梭的电解液实现了平均更高的库仑效率（99.13％）（97.71％）。此外，带有氧化还原梭的 AFLMB 表现出改进的循环性能和更长的使用寿命。

更新日期：2023-06-04

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