Analogous Design of a Microlayered Silicon Oxide‐Based Electrode to the General Electrode Structure for Thin‐Film Lithium‐Ion Batteries

Abstract

Development of miniaturized thin-film lithium-ion batteries (TF-LIBs) using vacuum deposition techniques is crucial for low-scale applications, but addressing low energy density remains a challenge. In this work, structures analogous to SiO_x-based thin-film electrodes are designed with close resemblance to traditional LIB slurry formulations including active material, conductive agent, and binder. The thin-film is produced using mid-frequency sputtering with a single hybrid target consisting of SiO_x nanoparticles, carbon nanotubes, and polytetrafluoroethylene. The thin-film SiO_x/PPFC (plasma-polymerized fluorocarbon) involves a combination of SiO_x and conductive carbon within the PPFC matrix. This results in enhanced electronic conductivity and superior elasticity and hardness in comparison to a conventional pure SiO_x-based thin-film. The electrochemical performance of the half-cell consisting of thin-film SiO_x/PPFC demonstrates remarkable cycling stability, with a capacity retention of 74.8% up to the 1000th cycle at 0.5 C. In addition, a full cell using the LiNi_0.6Co_0.2Mn_0.2O₂ thin-film as the cathode material exhibits an exceptional initial capacity of ≈120 mAh g^-1 at 0.1 C and cycle performance, marked by a capacity retention of 90.8% from the first cycle to the 500th cycle at a 1 C rate. This work will be a stepping stone for the AM/CB/B composite electrodes in TF-LIBs.