Bicontinuous phase separation of lithium-ion battery electrodes for ultrahigh areal loading

Ultrathick battery electrodes are appealing as they reduce the fraction of inactive battery parts such as current collectors and separators. However, thick electrodes are difficult to dry and tend to crack or flake during production. Moreover, the electrochemical performance of thick electrodes is constrained by ion and electron transport as well as fast capacity degradation. Here, we report a thermally induced phase separation (TIPS) process for fabricating thick Li-ion battery electrodes, which incorporates the electrolyte directly in the electrode and alleviates the need to dry the electrode. The proposed TIPS process creates a bicontinuous electrolyte and electrode network with excellent ion and electron transport, respectively, and consequently achieves better rate performance. Using this process, electrodes with areal capacities of more than 30 mAh/cm² are demonstrated. Capacity retentions of 87% are attained over 500 cycles in full cells with 1-mm-thick anodes and cathodes. Finally, we verified the scalability of the TIPS process by coating thick electrodes continuously on a pilot-scale roll-to-roll coating tool.