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Triboelectric nanogenerators (TENG) are a possible power source for wearable electronics, but the conventional electrode materials for TENG are metals such as Cu and Al that are easy to be oxidized or corroded in some harsh environments. In this paper, metal electrode material is replaced by an electrical conducting polymer, polypyrrole (PPy), for the first time. Moreover, by utilizing PPy with micro/nanostructured surface as the triboelectric layer, the charge density generated is significantly improved, more superior to that of TENG with metals as the triboelectric layer. As this polymer‐based TENG is further integrated with PPy‐based supercapacitors, an all‐plastic‐materials based self‐charging power system is built to provide sustainable power with excellent long cycling life. Since the environmental friendly materials are adopted and the facile electrochemical deposition technique is applied, the new self‐charging power system can be a practical and low cost power solution for many applications.

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In this work, polypyrrole/graphene doped by p-toluenesulfonic is prepared as an active material for supercapacitors, and its capacitance performance is investigated in various aqueous electrolytes including HCl, LiCl, NaCl, and KCl with a concentration of 3 M, respectively. A rising trend of capacitance is observed according to the cationic mobility (Li(+) < Na(+) < K(+) < H(+)), which is due to its effect on the ionic conductivity, efficient ion/charge diffusion/exchange and relaxation time. On the other hand, long-term cycling stability is in the following order: KCl < NaCl < LiCl < HCl, corresponding to the decreasing tendency of cation size (K(+) > Na(+) > Li(+) > H(+)). The reason can be attributed to the fact that the insertion/de-insertion of large size cation brings a significant doping level decrease and an over-oxidation increase during the charging-discharging cycles. Hence, we not only obtain good capacitance performance (280.3 F g(-1) at 5 mV s(-1)), superior rate capability (225.8 F g(-1) at 500 mV s(-1)) and high cycling stability (92.0% capacitance retention after 10,000 cycles at 1 A g(-1)) by employing 3 M HCl as an electrolyte, but also reveal that the electrolyte cations have a significant effect on the supercapacitors' electrochemical performance.