Abstract
Silicon monoxide (SiO)-based anode materials are one of the most intensively investigated class of materials for use as high-capacity anodes in lithium-ion batteries. However, their low initial Coulombic efficiency (ICE), resulting from the irreversible electrochemical reaction of the amorphous SiO2 (a-SiO2) phase in the SiO, restricts the wide-spread adoption of SiO-based anode materials in lithium-ion batteries. Pre-emptive formation of an irreversible phase that converts a-SiO2 to a non-reactive state with lithium prior to cell assembly has received much attention for enhancing ICE. However, this process has the drawback of not ensuring long-term cycle performance. Herein, the pre-emptive formation of irreversible phase combined with the high-energy mechanical milling (HEMM) process is proposed to simultaneously improve both the ICE and long-term cycle performance. The resulting porous Si/Ca-Si-O nanocomposite electrode exhibits an impressive ICE of 86.4 % and maintains 55 % of its capacity over 200 cycles. The key factor in the significant ICE improvement is the irreversible Ca-Si-O phase, which is formed by the calciothermic reduction of Si with CaH2. In addition, the microstructural changes induced by the HEMM process effectively mitigate the volume expansion of Si during cycling, resulting in improved long-term cycle stability.
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