Ultrastable Interfacial Contacts Enabling Unimpeded Charge Transfer and Ion Diffusion in Flexible Lithium‐Ion Batteries

Deteriorating interfacial contact under mechanical deformation induces large cracks and high charge transfer resistance, resulting in a severe capacity fading of flexible lithium‐ion batteries (LIBs). Herein, an oxygen plasma treatment on a polymer separator combined with high‐speed centrifugal spraying to construct ultrastable interfacial contacts is reported. With the treatment, abundant hydrophilic oxygen‐containing functional groups are produced and ensure strong chemical adhesion between the separator and the active materials. With single walled carbon nanotubes (SWCNTs) sprayed onto the active materials, a dense thin film is formed as the current collector. Meanwhile, the centrifugal force caused by high‐speed rotation together with van der Waals forces under fast evaporation produces a much closer interface between the current collector and the active materials. As a result of this ultrastable interfacial interaction, the integrated electrode shows no structural failure after 5000 bending cycles with the charge‐transfer resistance as low as 35.8% and a Li‐ion diffusion coefficient nearly 19 times of the untreated electrode. Flexible LIBs assembled with these integrated electrodes show excellent structural and electrochemical stability, and can work steadily under various deformed states and repeated bending. This work provides a new technique toward rational design of electrode configuration for flexible LIBs.