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Regulating the ranking of polymer in triboelectric series over a wide range is of great help for material's selection of triboelectric nanogenerators (TENGs). Herein, fluorinated poly(phthalazinone ether)s (FPPEs) with tunable molecular structure and aggregate structure are synthesized by co‐polycondensation, while the large positive ranking shift in the triboelectric series can be achieved by introducing phthalazinone moieties with strong electron donating capability. FPPE‐5, which includes abundant phthalazinone moieties, is more positive than all of the previously reported triboelectric polymers. Hence, the regulating range of FPPEs in this work updates a new record in triboelectric series, which is wider than that of previous works. A peculiar crystallization behavior, capable of trapping and storing more electrons, has been observed in FPPE‐2 with 25% phthalazinone moieties. Correspondingly, FPPE‐2 is more negative than FPPE‐1 without a phthalazinone moiety, which is an unexpected shift against the common changing tendency in triboelectric series. With FPPEs films as the probing material, a tactile TENG sensor is applied to enable material identification via electrical signal polarity. Hence, this study demonstrates a strategy to regulate the series of triboelectric polymers by copolymerization using monomers with distinct electrification capabilities, where both the monomer ratio and the peculiar nonlinear behavior can control triboelectric performance. [ABSTRACT FROM AUTHOR]

Due to the thermionic emission effect, the electron transferred to dielectric surface can be released into vacuum after the contact electrification (CE). Therefore, triboelectric nanogenerator (TENG) cannot maintain effective electrical output under high temperature conditions. In order to obtain high thermal charge stability, polyimide is modified with strong electron withdrawing groups like trifluoromethyl (CF3) and sulfone group (SO2) in backbone. The fluorinated polyimides (F‐PI) with a big band gap can provide a tribocharge density of 170 µC m−2 (4 times of common Kapton film) and become more negative than polytetrafluoroethylene in triboelectric series. In addition, BaTiO3 nanoparticles are doped in F‐PI film for inducing deep traps and interfacial polarizations for CE, which can further enhance the charge density (200 µC m−2) and thermal charge stability. Finally, a flutter‐driven TENG (FD‐TENG) is designed based on this BaTiO3‐doped F‐PI film to harvest wind energy and sense wind velocity. This FD‐TENG can maintain 32% of its output performance at 200 °C in comparison with room temperature, which is the highest thermal charge stability reported for triboelectric polymers. Therefore, this BaTiO3‐doped F‐PI has great application prospects for energy generation and motion detection in hot wind tunnel and many other harsh environments. [ABSTRACT FROM AUTHOR]