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Influence of LiNO3 on the Lithium Metal Deposition Behavior in Carbonate-Based Liquid Electrolytes and on the Electrochemical Performance in Zero-Excess Lithium Metal Batteries
Small ( IF 13.0 ) Pub Date : 2023-10-05 , DOI: 10.1002/smll.202305203
Silvan Stuckenberg 1 , Marlena Maria Bela 1 , Christian-Timo Lechtenfeld 1 , Maximilian Mense 1 , Verena Küpers 1 , Tjark Thorben Klaus Ingber 1 , Martin Winter 1, 2 , Marian Cristian Stan 1
Small ( IF 13.0 ) Pub Date : 2023-10-05 , DOI: 10.1002/smll.202305203
Silvan Stuckenberg 1 , Marlena Maria Bela 1 , Christian-Timo Lechtenfeld 1 , Maximilian Mense 1 , Verena Küpers 1 , Tjark Thorben Klaus Ingber 1 , Martin Winter 1, 2 , Marian Cristian Stan 1
Affiliation
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Continuous lithium (Li) depletion shadows the increase in energy density and safety properties promised by zero-excess lithium metal batteries (ZELMBs). Guiding the Li deposits toward more homogeneous and denser lithium morphology results in improved electrochemical performance. Herein, a lithium nitrate (LiNO3) enriched separator that improves the morphology of the Li deposits and facilitates the formation of an inorganic-rich solid–electrolyte interphase (SEI) resulting in an extended cycle life in Li||Li-cells as well as an increase of the Coulombic efficiency in Cu||Li-cells is reported. Using a LiNi0.6Co0.2Mn0.2O2 positive electrode in NCM622||Cu-cells, a carbonate-based electrolyte, and a LiNO3 enriched separator, an extension of the cycle life by more than 50 cycles with a moderate capacity fading compared to the unmodified separator is obtained. The relative constant level of LiNO3 in the electrolyte, maintained by the LiNO3 enriched separator throughout the cycling process stems at the origin of the improved performance. Ion chromatography measurements carried out at different cycles support the proposed mechanism of a slow and constant release of LiNO3 from the separator. The results indicate that the strategy of using a LiNO3 enriched separator instead of LiNO3 as a sacrificial electrolyte additive can improve the performance of ZELMBs further by maintaining a compact and thus stable SEI layer on Li deposits.
中文翻译：
LiNO3 对碳酸盐基液体电解质中锂金属沉积行为及零过量锂金属电池电化学性能的影响
锂 (Li) 的持续耗尽给零过量锂金属电池 (ZELMB) 所承诺的能量密度和安全性能的提高带来了影响。引导锂沉积物朝着更均匀和更致密的锂形态发展，可以改善电化学性能。本文中，富含硝酸锂（LiNO 3 ）的隔膜可改善锂沉积物的形态，并促进富含无机物的固体电解质界面（SEI）的形成，从而延长Li||Li电池的循环寿命据报道，Cu||Li 电池的库仑效率有所提高。在NCM622||Cu电池中使用LiNi 0.6 Co 0.2 Mn 0.2 O 2正极、碳酸盐基电解质和富含LiNO 3 的隔膜，与相比，循环寿命延长了50次以上，且容量衰减适度获得未修改的分离器。在整个循环过程中，由富含LiNO 3 的分离器维持电解质中LiNO 3的相对恒定水平是性能改进的根源。在不同循环下进行的离子色谱测量支持所提出的从分离器缓慢且持续释放LiNO 3的机制。结果表明，使用富含LiNO 3 的隔膜代替LiNO 3作为牺牲电解质添加剂的策略可以通过在Li沉积物上保持致密且稳定的SEI层来进一步提高ZELMB的性能。
更新日期：2023-10-05
中文翻译：
LiNO3 对碳酸盐基液体电解质中锂金属沉积行为及零过量锂金属电池电化学性能的影响
锂 (Li) 的持续耗尽给零过量锂金属电池 (ZELMB) 所承诺的能量密度和安全性能的提高带来了影响。引导锂沉积物朝着更均匀和更致密的锂形态发展，可以改善电化学性能。本文中，富含硝酸锂（LiNO 3 ）的隔膜可改善锂沉积物的形态，并促进富含无机物的固体电解质界面（SEI）的形成，从而延长Li||Li电池的循环寿命据报道，Cu||Li 电池的库仑效率有所提高。在NCM622||Cu电池中使用LiNi 0.6 Co 0.2 Mn 0.2 O 2正极、碳酸盐基电解质和富含LiNO 3 的隔膜，与相比，循环寿命延长了50次以上，且容量衰减适度获得未修改的分离器。在整个循环过程中，由富含LiNO 3 的分离器维持电解质中LiNO 3的相对恒定水平是性能改进的根源。在不同循环下进行的离子色谱测量支持所提出的从分离器缓慢且持续释放LiNO 3的机制。结果表明，使用富含LiNO 3 的隔膜代替LiNO 3作为牺牲电解质添加剂的策略可以通过在Li沉积物上保持致密且稳定的SEI层来进一步提高ZELMB的性能。
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