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Polymers are commonly used to fabricate triboelectric nanogenerators (TENGs). Here, several polymer films with similar main chains but different functional groups on the side chain are employed to clarify the contributions of each functional group to contact electrification (CE). The results show that the electron‐withdrawing (EW) ability and density of these functional groups on the main chain can determine both the polarity and density of CE‐induced surface charges. Similar results are obtained for CE in both the polymer–polymer and polymer–liquid modes. A theoretical mechanism involving electron cloud overlap is proposed to explain all of these results. More importantly, the unsaturated groups on poly(tetrafluoroethylene) molecular chain are proved to have a much stronger EW ability than the saturated groups. The density of these unsaturated groups can be increased using a sputtering technique, suggesting that this is a facile and effective method of enhancing the performance of TENGs. These results clarify the correlation between the molecular structure and macroscopic electrification behavior of polymers.
A series of polymer films with different functional groups on the side chain are employed for clarifying the contribution of functional groups to their contact electrification (CE) processes with both solids and liquids. The unsaturated groups of PTFE can enhance the electronegativity of the whole functional group.