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001037569 245__ $$aUnderstanding Degradation and Enhancing Cycling Stabilityfor High-Voltage LiCoO2-Based Li-Metal Batteries
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001037569 520__ $$aImproving the energy density of Lithium (Li)-ion batteries (LIBs) is vital inmeeting the growing demand for high-performance energy storage andconversion systems. Developing high-voltage LIBs using high-capacity andhigh-voltage cathode materials is promising for enhancing energy density.However, conventional cathode and electrolyte materials face seriousdecomposition and structural degradation at high operating voltages. Herein,a dual-salts electrolyte of lithium bis(fluorosulfonyl)imide and lithiumbis(trifluoromethanesulfonyl)imide(LiFSI-LiTFSI) is developed to improve thecycling stability of high-voltage lithium cobalt oxide (LiCoO2, LCO)||Libatteries. Operando X-ray diffraction analysis experiments are carried out tocharacterize the structural stability of cathode materials, suggesting a severeirreversible phase transformation at high voltage levels. Aging simulations,combined with experimental studies, suggest that a fast loss of activematerials is mainly responsible for the capacity loss at high voltages.Carbon-coated LCO cathodes are synthesized to mitigate cycling degradation.The designed LCO||Li cells exhibit a high-capacity retention of over 85% after400 cycles at 4 .7V. The present work provides a novel insight intounderstanding the degradation and enhancing the stability of high-voltageLCO-based Li-metal batteries, thus facilitating their practical applications.
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001037569 7001_ $$0P:(DE-HGF)0$$aChang$$b1
001037569 7001_ $$0P:(DE-Juel1)176976$$aChen, Zhiqiang$$b2
001037569 7001_ $$0P:(DE-Juel1)188297$$aWindmüller, Anna$$b3
001037569 7001_ $$0P:(DE-Juel1)156244$$aTsai, Chih-Long$$b4
001037569 7001_ $$0P:(DE-Juel1)190219$$aQin, Zhizhen$$b5
001037569 7001_ $$0P:(DE-Juel1)173719$$aDanilov, Dmitri$$b6
001037569 7001_ $$0P:(DE-Juel1)173933$$aZhou, Lei$$b7
001037569 7001_ $$0P:(DE-Juel1)185897$$aDaniel, Davis Thomas$$b8
001037569 7001_ $$0P:(DE-Juel1)195868$$aSchaps, Kristian$$b9
001037569 7001_ $$0P:(DE-Juel1)201235$$aAhmed, Jehad$$b10
001037569 7001_ $$0P:(DE-Juel1)176196$$aRaijmakers, Luc$$b11
001037569 7001_ $$0P:(DE-HGF)0$$aYu$$b12
001037569 7001_ $$0P:(DE-Juel1)161208$$aTempel, Hermann$$b13
001037569 7001_ $$0P:(DE-Juel1)162401$$aGranwehr, Josef$$b14
001037569 7001_ $$0P:(DE-Juel1)172735$$aChen, Chunguang$$b15
001037569 7001_ $$0P:(DE-HGF)0$$aWei$$b16
001037569 7001_ $$0P:(DE-Juel1)156123$$aEichel, Rüdiger-A.$$b17
001037569 7001_ $$0P:(DE-Juel1)165918$$aNotten, Peter H. L.$$b18$$eCorresponding author
001037569 773__ $$0PERI:(DE-600)2594556-7$$a10.1002/aenm.202404028$$gp. 2404028$$n7$$p2404028$$tAdvanced energy materials$$v15$$x1614-6832$$y2025
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