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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 SiOx‐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 SiOx nanoparticles, carbon nanotubes, and polytetrafluoroethylene. The thin‐film SiOx/PPFC (plasma‐polymerized fluorocarbon) involves a combination of SiOx and conductive carbon within the PPFC matrix. This results in enhanced electronic conductivity and superior elasticity and hardness in comparison to a conventional pure SiOx‐based thin‐film. The electrochemical performance of the half‐cell consisting of thin‐film SiOx/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 LiNi0.6Co0.2Mn0.2O2 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.
SiOx‐based thin‐film electrodes are designed similar to traditional lithium‐ion battery (LIB) slurry formulations, including active material, conductive agent, and binder. Using mid‐frequency sputtering with a hybrid target containing SiOx nanoparticles, carbon nanotubes, and polytetrafluoroethylene, a thin‐film SiOx‐based composite electrode is successfully fabricated within plasma‐polymerized fluorocarbon (PPFC). The SiOx/PPFC composite thin‐film exhibits improved electronic conductivity, elasticity, and hardness compared to pure SiOx‐based thin‐film. The electrochemical performance of the SiOx/PPFC composite thin‐film shows remarkable cycling stability.