Preparation and Characterization of Fluorine-Containing Polyimide Films with Enhanced Output Performance for Potential Applications as Negative Friction Layers for Triboelectric Nanogenerators

Nanotechnologies are being increasingly widely used in advanced energy fields. Triboelectric nanogenerators (TENGs) represent a class of new-type flexible energy-harvesting devices with promising application prospects in future human societies. As one of the most important parts of TENG devices, triboelectric materials play key roles in the achievement of high-efficiency power generation. Conventional polymer tribo-negative materials, such as polytetrafluoroethylene (PTFE), polyvinylidene difluoride (PVDF), and the standard polyimide (PI) film with the Kapton® trademark based on pyromellitic anhydride (PMDA) and 4,4′-oxydianiline (ODA), usually suffer from low output performance. In addition, the relationship between molecular structure and triboelectric properties remains a challenge in the search for novel triboelectric materials. In the current work, by incorporating functional groups of trifluoromethyl (–CF3) with strong electron withdrawal into the backbone, a series of fluorine-containing polyimide (FPI) negative friction layers have been designed and prepared. The derived FPI-1 (6FDA-6FODA), FPI-2 (6FDA-TFMB), and FPI-3 (6FDA-TFMDA) resins possessed good solubility in polar aprotic solvents, such as the N,N-dimethylacetamide (DMAc) and N-methyl-2-pyrrolidone (NMP). The PI films obtained via the solution-casting procedure showed glass transition temperatures (Tg) higher than 280 °C with differential scanning calorimetry (DSC) analyses. The TENG prototypes were successfully fabricated using the developed PI films as the tribo-negative layers. The electron-withdrawing trifluoromethyl (–CF3) units in the molecular backbones of the PI layers provided the devices with an apparently enhanced output performance. The FPI-3 (6FDA-TFMDA) layer-based TENG devices showcased an especially impressive open-circuit voltage and short-circuit current, measuring 277.8 V and 9.54 μA, respectively. These values were 4~5 times greater when compared to the TENGs manufactured using the readily accessible Kapton® film.