A Comparative Study of Nano and Micro-Sized Silicon in Lithium-Ion Cells with a Nickel-Rich Cathode

Abstract

Reducing particle size has been widely adopted to mitigate the cracking and pulverization of silicon particles and to enhance electrode reaction kinetics for silicon electrodes in cycling. However, the increased surface area promotes parasitic reactions with electrolyte solvents. This work comparatively studies nano-sized silicon (Si-NP) and micro-sized silicon (Si-MP) as anodes in Li-ion cells using nickel-rich LiNi_0.80Co_0.1Mn_0.1O₂ (NCM811) as the cathode. The focus is on capacity, capacity retention, Coulombic efficiency (CE), and rate capability by changing the negative-to-positive capacity (N/P) ratio and charging cutoff voltage. It is found that Si-NP initially exhibits a CE above 90%, however, it rarely exceeds 98% in subsequent cycles, leading to rapid capacity fade. Additionally, increasing the N/P ratio and lowering the charging cutoff voltage does not obviously improve the cycling stability of Si-NP cells. Compared with Si-NP, Si-MP experiences lower capacity and lower CE in the initial several cycles. However, with continued cycling, both the capacity and CE gradually increase to a maximum and stably remain at ∼99.9%. The findings of this work suggest that, with its excellent rate capability, Si-MP may be more advantageous than Si-NP in developing practical Li-ion batteries, provided its low CE during initial cycles can be successfully addressed.