All‐Printed Wearable Triboelectric Nanogenerator with Ultra‐Charged Electron Accumulation Polymers Based on MXene Nanoflakes

Abstract The multilayer triboelectric nanogenerators (TENGs) are widely developed to enhance the output performance of device. However, these TENGs consisting of electron transfer, transport, trap layers toward a large volumetric charge density should be wearable and mass‐produced for commercialization. Thus, appropriate material selection in respective layers and fabrication method are crucial for the commercialization of multilayer TENG. This study presents all‐printed, sustainable wearable TENGs based on electron accumulation polymers (EAPs) with superior charge retention capability. The EAPs consisting of polytetrafluoroethylene (PTFE), carboxyl functionalized single‐walled carbon nanotubes (SWCNTs:COOH), and Ti 3 C 2 T x (MXene) in a fluorinated polymer matrix, are used. Compared to the reference, the EAPs not only lead to approximately six times higher output performance (300 V and 40 µA) but also four times more sustainable charge retention capability (92%) for an hour. These are attributed to the three‐step electron‐trapping mechanism with electron transfer/transport from PTFE/SWCNT and electron trapping in MXene. In addition, TENGs with EAPs exhibit excellent mechanical stability and reliability with fascinating single‐electrode demonstrations. Finally, the TENG with EAPs can efficiently operate various portable electronics and pH monitoring systems with a pH sensor and a seven‐segment display in realistic scenarios.