Journal Article

FZJ-2025-00754

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Understanding Degradation and Enhancing Cycling Stabilityfor High-Voltage LiCoO2-Based Li-Metal Batteries

Wu ; Chang ; Chen, Z. ; Windmüller, A.FZJ* ; Tsai, C.-L.FZJ* ; Qin, Z.FZJ*RWTH* ; Danilov, D.FZJ* ; Zhou, L. ; Daniel, D. T.FZJ* ; Schaps, K. ; Ahmed, J.FZJ*RWTH* ; Raijmakers, L.FZJ* ; Yu ; Tempel, H.FZJ* ; Granwehr, J.FZJ*RWTH* ; Chen, C. ; Wei ; Eichel, R.-A.FZJ*RWTH* ; Notten, P. H. L. (Corresponding author)FZJ*

2025
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/aenm.202404028  doi:10.34734/FZJ-2025-00754

Abstract: Improving 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.

Keyword(s): Energy (1st) ; Chemistry (2nd)

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Contributing Institute(s):

1. Grundlagen der Elektrochemie (IET-1)

Research Program(s):

1. 1223 - Batteries in Application (POF4-122) (POF4-122)
2. HITEC - Helmholtz Interdisciplinary Doctoral Training in Energy and Climate Research (HITEC) (HITEC-20170406) (HITEC-20170406)

Appears in the scientific report 2025

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 25 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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