To use lithium‐ion batteries (LIBs) as the energy storage system in wearable smart electronic devices, LIBs must be downsized, particularly with respect to their thickness. To address this need, herein a solution‐based fabrication process for thin LIB electrodes is proposed. This process involves the powder synthesis of precursor materials through a wet mechanochemical reaction, electrophoretic deposition (EPD) to coat the current collector, and thermal conversion to attain the final electrode active material. Specifically, the wet mechanochemical synthesis of Li1.81H0.19Ti2O5·xH2O (LHTO) using a planetary ball mill produces a mixture of nanosheet and nanotube particles. These particles are then uniformly coated onto Cu foil through EPD while controlling the film thickness from 5 to 17 μm by varying the applied voltage and coating time. Finally, the LHTO/Cu foils are thermally converted into thin Li4Ti5O12/Cu anodes without added conductive materials. The resulting anodes exhibit a discharge capacity of ≈50 μAh cm−2 and good cycling performance. Wet milling particle synthesis and EPD coating can both be employed in continuous manufacturing processes, thus constituting an efficient route for fabricating electrodes for thin LIBs.
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