Abstract
A thorough analysis of the evolution of the voltage profiles of silicon nanoparticle electrodes upon cycling has been conducted. The largest changes to the voltage profiles occur at the earlier stages (> 0.16 V vs Li/Li+) of lithiation of the silicon nanoparticles. The changes in the voltage profiles suggest that the predominant failure mechanism of the silicon electrode is related to incomplete delithiation of the silicon electrode during cycling. The incomplete delithiation is attributed to resistance increases during delithiation, which are predominantly contact and solid electrolyte interface (SEI) resistance. The capacity retention can be significantly improved by lowering delithiation cutoff voltage or by introducing electrolyte additives, which generate a superior SEI. The improved capacity retention is attributed to the reduction of the contact and SEI resistance.
Highlights
Nano-structured silicon electrodes mitigate the tension that polymeric binders are subjected to during lithiation/delithiation preserving the contact between silicon particles and carbon additives.[7]
Efforts to stabilize the large surface area of nano-structured silicon electrodes have utilized electrolyte additives such as fluoroethylene carbonate (FEC) and vinylene carbonate (VC) which lead to the generation of a more effective SEI.[24,25,26,27,28,29,30]
Even though the electrochemical performance of silicon electrodes can be significantly enhanced by the combination of nano-structured silicon, effective binders, and SEI forming electrolyte additives; the capacity retention and efficiency of the silicon electrodes remain insufficient for commercial application
Summary
Capacity Fading Mechanisms of Silicon Nanoparticle Negative Electrodes for Lithium Ion Batteries. In the context of improving the cycling behavior of silicon electrodes, the mechanism of capacity fade has been investigated extensively.
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