<p>Hybridization of Si with SiO<sub>x</sub> has been recognized as an effective strategy to enhance the performance of Si-based Li-ion batteries by mitigating the rapid capacity fade of Si and the low initial coulombic efficiency of SiO<sub>x</sub>. In this work, a 1:2 (wt.) microsized Si/SiO<sub>x</sub> hybrid electrode is employed to elucidate the distinct electrochemical characteristics of Si-based Li-ion cells compared with conventional graphite-based systems. Owing to their fundamentally different Li storage mechanisms, Si-based cells do not need time-consuming formation cycles typically used to form a robust solid electrolyte interphase (SEI) in graphite electrodes. Furthermore, the role of the SEI in stabilizing cycling performance differs substantially between the two systems. Remarkably, Si-based Li-ion cells exhibit excellent tolerance to deep discharge. Testing on Si/LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) coin cells demonstrates stable cycling even when discharged to 0.2&#xa0;V, without detrimental effects on cycling stability. Despite this advantage, relatively fast capacity fading remains a critical challenge, and the underlying mechanisms are analyzed. The findings of this work provide new fundamental insights into the electrochemical characteristics of Si-based Li-ion batteries and offer guidance for improving the cycling performance of Si-based Li-ion batteries.</p> Graphical Abstract <p></p>

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Electrochemical tolerance of silicon-based Li-ion batteries to formation current rate and discharge voltage window

  • Sheng S. Zhang

摘要

Hybridization of Si with SiOx has been recognized as an effective strategy to enhance the performance of Si-based Li-ion batteries by mitigating the rapid capacity fade of Si and the low initial coulombic efficiency of SiOx. In this work, a 1:2 (wt.) microsized Si/SiOx hybrid electrode is employed to elucidate the distinct electrochemical characteristics of Si-based Li-ion cells compared with conventional graphite-based systems. Owing to their fundamentally different Li storage mechanisms, Si-based cells do not need time-consuming formation cycles typically used to form a robust solid electrolyte interphase (SEI) in graphite electrodes. Furthermore, the role of the SEI in stabilizing cycling performance differs substantially between the two systems. Remarkably, Si-based Li-ion cells exhibit excellent tolerance to deep discharge. Testing on Si/LiNi0.8Co0.1Mn0.1O2 (NCM811) coin cells demonstrates stable cycling even when discharged to 0.2 V, without detrimental effects on cycling stability. Despite this advantage, relatively fast capacity fading remains a critical challenge, and the underlying mechanisms are analyzed. The findings of this work provide new fundamental insights into the electrochemical characteristics of Si-based Li-ion batteries and offer guidance for improving the cycling performance of Si-based Li-ion batteries.

Graphical Abstract