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001005135 1001_ $$0P:(DE-Juel1)188450$$aPfeiffer, Felix$$b0
001005135 245__ $$aStudy of a High-Voltage NMC Interphase in the Presence of a Thiophene Additive Realized by Operando SHINERS
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001005135 520__ $$aImproving the electrochemical properties and cycle life of high-voltage cathodes in lithium-ion batteries requires a deep understanding of the structural properties and failure mechanisms at the cathode electrolyte interphase (CEI). We present a study implementing an advanced Raman spectroscopy technique to specifically address the compositional features of interphase during cell operation. Our operando technique, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), provides a reliable platform to investigate the dynamics of the interphase structure and elucidate the compositional changes near the cathode surface. To improve the CEI properties, thiophene was introduced and investigated as an effective, high-voltage film-forming additive by largely diminishing the capacity fading triggered at high potentials in LiNi1/3Co1/3Mn1/3O2 cathodes. While the cells without thiophene show severe capacity fading, cells with an optimized concentration of thiophene exhibit a significant performance improvement. Operando SHINERS detects the presence of a stable CEI. The results suggest that the composition of the CEI is dominated by polythiophene and copolymerization products of ethylene carbonate with thiophene, which protects the electrolyte components from further decomposition. The formation mechanism of the polymeric film was modeled using quantum chemistry calculations, which shows good agreement with the experimental data.
001005135 536__ $$0G:(DE-HGF)POF4-1223$$a1223 - Batteries in Application (POF4-122)$$cPOF4-122$$fPOF IV$$x0
001005135 536__ $$0G:(BMBF)13XP5129$$aElektrolytformulierungen für Lithiumbatterien der nächsten Generation mit großer Energiedichte und hoher Beständigkeit (13XP5129)$$c13XP5129$$x1
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001005135 7001_ $$0P:(DE-Juel1)169877$$aDiddens, Diddo$$b1
001005135 7001_ $$0P:(DE-Juel1)190810$$aWeiling, Matthias$$b2
001005135 7001_ $$00000-0002-2754-6623$$aBaghernejad, Masoud$$b3$$eCorresponding author
001005135 773__ $$0PERI:(DE-600)2467494-1$$a10.1021/acsami.2c17958$$gVol. 15, no. 5, p. 6676 - 6686$$n5$$p6676 - 6686$$tACS applied materials & interfaces$$v15$$x1944-8244$$y2023
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