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In general, various kinds of surface modifications are utilized to enhance the power output performance of triboelectric nanogenerators (TENGs), but they typically have limited stability. Here, a new strategy of adding electrolytes with asymmetric ion pairing to polymer friction layers of TENGs is introduced in order to enhance their triboelectric property. Indeed, Kelvin probe force microscopy (KPFM) measurements show that an addition of phosphoric acid (H3PO4 ), an electrolyte with more cations than anions, to polyvinyl alcohol (PVA) can make it one of the most negative triboelectric materials; whereas, an addition of calcium chloride (CaCl2 ), an electrolyte with more anions than cations, to PVA can make it one of the most positive triboelectric materials. Furthermore, the TENGs based on such solid polymer electrolytes (SPEs) produce significantly higher power output than typical metal‐polymer TENGs. Due to these unique features, SPEs are a promising triboelectric material for realizing high‐performance TENGs for self‐powered small electronics.  相似文献   
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