In addressing the critical challenge of calendar aging in silicon (Si)-based lithium-ion batteries, this study introduces a groundbreaking strategy utilizing glyme-type dual-salt electrolytes (lithium bis(trifluoromethanesulfonyl)imide [LiTFSI] and lithium difluoro(oxalato)borate [LiDFOB]). These electrolytes are demonstrated to significantly mitigate parasitic reactions and capacity loss in Si-NMC (lithium nickel manganese cobalt oxide) full cells, especially when compared with traditional carbonate-based electrolytes. Our exhaustive mechanistic analysis reveals that such electrolytes not only preserve the integrity of the Si anode but also improve the cathode/electrolyte interphases (CEI) through the formation of a conformal coating on the high-voltage cathode surface. This dual-salt approach, enhanced by the addition of a phosphate additive, effectively decelerates calendar aging, marking a substantial advance in the quest for durable and reliable Si-based energy storage technologies. The findings underscore the vital role of electrolyte composition in extending the calendar life of Si batteries, offering an alternative avenue toward maximizing the performance and longevity of next-generation Li–Si batteries.

中文翻译：

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使用先进的双盐 Glyme 电解质缓解 Si-NMC 电池的日历老化


为了解决硅 （Si） 基锂离子电池日历老化的关键挑战，本研究引入了一种利用 glyme 型双盐电解质（双（三氟甲烷磺酰基）酰亚胺锂 [LiTFSI] 和二氟（草酸）硼酸锂 [LiDFOB]）的开创性策略。这些电解质被证明可以显著减轻 Si-NMC（锂镍锰钴氧化物）全电池中的寄生反应和容量损失，尤其是与传统的碳酸盐基电解质相比。我们详尽的机理分析表明，这种电解质不仅可以保持硅阳极的完整性，还可以通过在高压阴极表面形成保形涂层来改善阴极/电解质界面 （CEI）。这种双盐方法通过添加磷酸盐添加剂得到增强，有效地减缓了日历老化，标志着在寻求耐用可靠的硅基储能技术方面取得了重大进步。研究结果强调了电解质成分在延长硅电池的日历寿命方面的重要作用，为最大限度地提高下一代锂-硅电池的性能和寿命提供了另一种途径。