The application of Si-based anodes in lithium-ion batteries (LIBs) has garnered significant attention due to their high theoretical specific capacity yet is still challenged by the substantial volume expansion of silicon particles during the lithiation process, resulting in the instability of the electrode–electrolyte interphase and deteriorative battery performance. Herein, an ortho(trimethylsilyl)oxybenzene electrolyte additive, 1,2-bis((trimethylsilyl)oxy) benzene (referred to as BTMSB), has been investigated as a bifunctional electrolyte additive for Si-based LIBs. The BTMSB can form a uniform and robust LiF-rich solid electrolyte interphase (SEI) on the surface of Si-based material particles, adapting the huge volume expansion of the Si-based electrode and facilitating lithium-ion transport. Additionally, the BTMSB demonstrates the ability to scavenge hydrofluoric acid (HF) to stabilize the electrode–electrolyte interphase. The SiO_x/C∥Li batteries with 2% BTMSB exhibit improved cycle performance and current–rate capabilities, of which the capacity retention retains 69% after 400 cycles. Furthermore, Si-based anode cells with higher theoretical specific capacities (1C = 550 mAh g^–1) and NCM523∥SiO_x/C pouch cells are constructed and evaluated, displaying superior cycle performance. This work provides valuable insights for the development of effective electrolyte additives and the commercialization of high energy density LIBs with Si-based anodes.

中文翻译：

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固体电解质界面成膜和表面稳定双功能1,2-双((三甲基硅基)氧基)苯作为硅基锂离子电池的新型电解质添加剂

硅基负极因其高理论比容量而在锂离子电池（LIB）中的应用引起了广泛关注，但仍面临锂化过程中硅颗粒体积大幅膨胀导致电极不稳定的挑战–电解质界面和电池性能恶化。在此，研究了一种邻（三甲基硅基）氧基苯电解质添加剂1,2-双（（三甲基硅基）氧基）苯（简称BTMSB）作为硅基LIB的双功能电解质添加剂。BTMSB可以在硅基材料颗粒表面形成均匀且坚固的富含LiF的固体电解质界面（SEI），适应硅基电极巨大的体积膨胀并促进锂离子传输。此外，BTMSB 还具有清除氢氟酸（HF）以稳定电极-电解质界面的能力。含有2% BTMSB的SiO _x /C∥Li电池表现出改善的循环性能和倍率能力，其中400次循环后容量保持率仍保持在69%。此外，还构建并评估了具有更高理论比容量（1C = 550 mAh g ^–1）的硅基负极电池和NCM523∥SiO _{x /C软包电池，显示出优异的循环性能。}这项工作为有效电解质添加剂的开发和硅基阳极高能量密度锂离子电池的商业化提供了宝贵的见解。