Tailored Interphases Construction for Enhanced Si Anode and Ni-Rich Cathode Performance in Lithium-Ion Batteries

As promising candidates for high-energy-density lithium-ion batteries, both silicon (Si) anodes and nickel-rich cathodes face significant challenges due to structural instability arising from interphases. In this study, we introduce tetravinylsilane (TVSi) as a multifunctional electrolyte additive to engineer tailored interphases simultaneously on Si anode and LiNi_0.92Mn_0.05Co_0.03O₂ cathode, thereby enhancing their electrochemical performance. On one front, TVSi undergoes polymerization, leading to the formation of a composite solid electrolyte interphase (SEI) with an interpenetrating network structure on the Si surface. This SEI effectively accommodates the volume changes during cycling, inhibiting SEI growth and thereby preserving the capacity. On the other front, the TVSi-induced cathode-electrolyte interphase (CEI) exhibits a dense structure comprising a chemically bonded silicate-silane polymer. This CEI effectively mitigates transition metal dissolution by scavenging hydrofluoric acid and reduces irreversible phase transitions by minimizing side reactions. As a result of the enhanced interfacial stability achieved on both electrodes, TVSi enables improved performance in full cells with a LiNi_0.92Mn_0.05Co_0.03O₂ cathode paired with a silicon anode. This multifunctional additive strategy offers a novel perspective on additive design for high-energy-density lithium-ion batteries, showcasing its potential for advancing battery technology.

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