硅基负极因具有高的理论比容量而成为极具发展潜力的下一代锂离子电池负极材料，但是其在充放电期间存在巨大的体积波动，导致固态电解质界面（SEI）反复破裂/再生，界面膜不断增厚、阻抗持续增大，甚至出现电极破碎/粉化，严重缩短了电池的使用寿命，制约了该负极的实用化进程。为此，本文拟通过在电解液中引入成膜添加剂，缓解因硅体积波动而导致的上述界面问题。本文分别选择了硼酸三苯酯（TPB）、苯硼酸（PBA）和4-氟苯硼酸酐（TFTB）作为电解液添加剂应用在硅基锂离子电池中，详细探究了各款添加剂对电解液基本理化性质、电极/电解液界面化学和电池电化学性能的影响规律，获得的主要研究结论如下：

1）电解液中适量添加TPB可以明显提高人造石墨和硅碳负极的可逆容量和库仑效率，并改善这两种负极的循环和倍率性能，这是由于TPB能够优先于电解液其他溶剂，在负极表面发生还原分解，形成的含硼产物有效稳定了负极表面，抑制了界面副反应的发生。当TPB的质量百分数为1%时，石墨负极在200次循环后的容量保持率达到97.2%，硅碳负极经50次循环后的容量保持率达到98.1%。

2）添加剂PBA能够在硅碳负极和LiNi_0.5Co_0.2Mn_0.3O₂（NCM523）正极上形成稳定的界面膜，减少电解液的不可逆分解，进而同时提升正负极两侧的循环稳定性。在电解液中添加质量百分数为1%的PBA时，硅碳负极首次库伦效率达到89.4%，在100次循环后的容量保持率为83.8%；NCM523正极在0.5C电流密度下恒流充放电200次后的容量保持率达到81.7%，并具有良好的倍率特性（5 C放电比容量达103 mAh/g）。

3）将TFTB作为多功能添加剂引入电解液中，显著提高了硅基锂离子电池的稳定循环能力。理论计算结合实验表征证明了该添加剂能够优先还原分解，参与硅碳负极表面SEI膜的形成，。同时，TFTB与H2O/HF具有强的结合作用，能够抑制锂盐水解，减少有害HF的产生。此外，TFTB还有助于在正极侧形成致密且均匀的界面钝化膜。当电解液中添加质量百分数为1% TFTB时，硅碳负极在100次后容量保持率为82.1%，平均库伦效率为99.3%；NCM523正极首次放电比容量为180.3 mAh/g，在循环300次后的容量保持率达到87.6%。

Silicon-based anodes have become the next-generation lithium-ion battery anode materials with great development potential due to their high theoretical specific capacity. However, there are huge volume fluctuations during charge and discharge, resulting in repeated rupture/regeneration of the solid electrolyte interface (SEI), continuous thickening of the interface film, continuous increase in impedance, and even electrode breakage/pulverization, which seriously shortens the service life of the battery and restricts the practical process of the anode. Therefore, this paper intends to alleviate the above interface problems caused by the fluctuation of silicon volume by introducing film-forming additives into the electrolyte. In this paper, triphenyl borate (TPB), phenylboronic acid (PBA) and 4-fluorophenylboronic anhydride (TFTB) were selected as electrolyte additives in silicon-based lithium-ion batteries. The effects of various additives on the basic physical and chemical properties of the electrolyte, the interface chemistry of the electrode/electrolyte and the electrochemical performance of the battery were investigated in detail. The main conclusions are as follows:

1) The addition of appropriate amount of TPB in the electrolyte can significantly improve the reversible capacity and coulombic efficiency of the artificial graphite and silicon-carbon anodes, and improve the cycle and rate performance of the two anodes. This is due to the fact that TPB can take precedence over other solvents in the electrolyte, and the reduction decomposition occurs on the surface of the anode electrode. The boron-containing products formed effectively stabilize the surface of the anode electrode and inhibit the occurrence of interfacial side reactions. When the mass percentage of TPB is 1 %, the capacity retention of graphite anode reaches 97.2% after 200 cycles, and the capacity retention of silicon-carbon anode reaches 98.1% after 50 cycles.

2) The additive PBA can form a stable interface film on the silicon carbon anode and the LiNi_0.5Co_0.2Mn_0.3O₂ (NCM523) cathode, reducing the irreversible decomposition of the electrolyte, thereby improving the cycle stability on both sides of the cathode and anode electrodes. When PBA with a mass percentage of 1% was added to the electrolyte, the initial coulombic efficiency of the silicon-carbon anode reached 89.4 %, and the capacity retention after 100 cycles was 83.8 %. The capacity retention of NCM523 cathode reaches 81.7 % after 200 cycles of constant current charge and discharge at a current density of 0.5 C, and it has good rate performance (discharge specific capacity of 103 mAh/g at 5 C).

3) The introduction of TFTB as a multifunctional additive into the electrolyte significantly improves the stable cycling ability of silicon-based lithium-ion batteries. Theoretical calculation combined with experimental characterization proves that the additive can preferentially reduce and decompose, and participate in the formation of SEI film on the surface of silicon carbon anode. At the same time, TFTB has a strong binding effect with H₂O/HF, which can inhibit the hydrolysis of lithium salt and reduce the production of harmful HF. In addition, TFTB also helps to form a dense and uniform interfacial passivation film on the cathode side. When the mass percentage of TFTB added to the electrolyte is 1 %, the capacity retention of the silicon carbon anode is 82.1% after 100 cycles, and the average coulomb efficiency is 99.3%. The initial discharge specific capacity of NCM523 cathode is 180.3 mAh/g, and the capacity retention reaches 87.6% after 300 cycles.

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