Scalable Interlayer Nanostructure Design for High-Rate (10C) Submicron Silicon-Film Electrode by Incorporating Silver Nanoparticles

ACS Appl Mater Interfaces. 2023 Apr 19;15(15):18845-18856. doi: 10.1021/acsami.2c23279. Epub 2023 Apr 11.

Abstract

High C-rate capability at 10C is a key performance indicator for the commercialization of the next-generation high-charging lithium microbattery. However, silicon (Si) anode satisfying the prerequisite high specific capacity suffers from poor electron/ionic conductivity, seriously limiting the 10C rate capability. Accordingly, we propose the strategy of inserting highly conductive silver nanoparticles (AgNPs) as an interlayer between two RF-sputtered amorphous Si thin films to form an Si/Ag/Si multilayered anode, with the density and spatial distribution of the AgNPs well-controlled by thermal evaporation. This strategy is exclusively beneficial to scale up film thickness for higher capacity. Without AgNPs, the 10C rate performance of the double-layer Si (D_Si) is worse than the single layer (S_Si) in the same total thickness, suggesting the adverse effect of the interface. However, this situation is progressively improved with the AgNPs density incorporated at the interface, where the densest AgNPs anode (D_SiAg3) demonstrated a noticeable improvement reaching 1250 mAh/g at 10 C with a 46% capacity retention rate. By scaling up to triple layers, T_SiAg3 performed the superior 10C rate capability to T_Si, testifying to the scalable potential of the unique design for boosting high-power batteries. Finally, with electrochemical impedance spectroscopy results, a possible mechanism to explain the enhancement in rate capability is subject to where Li-ion diffusion is accelerated by the charge-induced electric field condensing around the AgNPs. This design for a multilayered nanocomposite can contribute to the design and fabrication of high-charging batteries and battery-on-chip.

Keywords: charge-induced lithiation; high-rate battery design strategy; interlayered nanostructure; rate capability; silicon anode; silver nanoparticles.