Journal Article

FZJ-2023-01323

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Study of a High-Voltage NMC Interphase in the Presence of a Thiophene Additive Realized by Operando SHINERS

Pfeiffer, F.FZJ* ; Diddens, D.FZJ* ; Weiling, M.FZJ* ; Baghernejad, M. (Corresponding author)FZJ*

2023
Soc. Washington, DC

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Please use a persistent id in citations: http://hdl.handle.net/2128/34342  doi:10.1021/acsami.2c17958

Abstract: Improving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study implementing an advanced Raman spectroscopy technique to specifically address the compositional features of interphase during cell operation. Our operando technique, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), provides a reliable platform to investigate the dynamics of the interphase structure and elucidate the compositional changes near the cathode surface. To improve the CEI properties, thiophene was introduced and investigated as an effective, high-voltage film-forming additive by largely diminishing the capacity fading triggered at high potentials in LiNi1/3Co1/3Mn1/3O2 cathodes. While the cells without thiophene show severe capacity fading, cells with an optimized concentration of thiophene exhibit a significant performance improvement. Operando SHINERS detects the presence of a stable CEI. The results suggest that the composition of the CEI is dominated by polythiophene and copolymerization products of ethylene carbonate with thiophene, which protects the electrolyte components from further decomposition. The formation mechanism of the polymeric film was modeled using quantum chemistry calculations, which shows good agreement with the experimental data.

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Contributing Institute(s):

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

Research Program(s):

1. 1223 - Batteries in Application (POF4-122) (POF4-122)
2. Elektrolytformulierungen für Lithiumbatterien der nächsten Generation mit großer Energiedichte und hoher Beständigkeit (13XP5129) (13XP5129)

Appears in the scientific report 2023

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; Essential Science Indicators ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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