Journal Article

FZJ-2023-05297

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Mechanistic Understanding of Additive Reductive Degradation and SEI Formation in High‐Voltage NMC811||SiO x ‐Containing Cells via Operando ATR‐FTIR Spectroscopy

Weiling, M.FZJ* ; Lechtenfeld, C. ; Pfeiffer, F.FZJ* ; Frankenstein, L. ; Diddens, D.FZJ* ; Wang, J.-F.FZJ* ; Nowak, S. ; Baghernejad, M. (Corresponding author)FZJ*

2024
Wiley-VCH Weinheim

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Please use a persistent id in citations: doi:10.1002/aenm.202303568  doi:10.34734/FZJ-2023-05297

Abstract: The implementation of silicon (Si)-containing negative electrodes is widely discussed as an approach to increase the specific capacity of lithium-ion batteries. However, challenges caused by severe volume changes and continuous (re-)formation of the solid-electrolyte interphase (SEI) on Si need to be overcome. The volume changes lead to electrolyte consumption and active lithium loss, decaying the cell performance and cycle life. Herein, the additive 2 sulfobenzoic acid anhydride (2 SBA) is utilized as an SEI-forming electrolyte additive for SiOx-containing anodes. The addition of 2 SBA to a state-of-the-art carbonate-based electrolyte in high-voltage NMC811||AG+20% SiOx pouch cells leads to improved electrochemical performance, resulting in a doubled cell cycle life. The origin of the enhanced cell performance is mechanistically investigated by developing an advanced experimental technique based on operando attenuated total reflection Fourier-transform infrared (ATR-FTIR) spectroscopy. The operando ATR-FTIR spectroscopy results elucidate the degradation mechanism via anhydride ring-opening reactions after electrochemical reduction on the anode surface. Additionally, ion chromatography conductivity detection mass spectrometry, scanning electron microscopy, energy dispersive X-ray analysis, and quantum chemistry calculations are employed to further elucidate the working mechanisms of the additive and its degradation products.

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Contributing Institute(s):

1. Helmholtz-Institut Münster Ionenleiter für Energiespeicher (IEK-12)

Research Program(s):

1. 1221 - Fundamentals and Materials (POF4-122) (POF4-122)
2. Elektrolytformulierungen für Lithiumbatterien der nächsten Generation mit großer Energiedichte und hoher Beständigkeit (13XP5129) (13XP5129)

Appears in the scientific report 2024

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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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