Summary: | The oxidation of metal microparticles (MPs) in a polymer film yields a mesoporous highly-deformable composite polymer for enhancing performance and creating a gapless structure of triboelectric nanogenerators (TENGs). This is a one-step scalable synthesis for developing large-scale, cost-effective, and light-weight mesoporous polymer composites. We demonstrate mesoporous aluminum oxide (Al<sub>2</sub>O<sub>3</sub>) polydimethylsiloxane (PDMS) composites with a nano-flake structure on the surface of Al<sub>2</sub>O<sub>3</sub> MPs in pores. The porosity of mesoporous Al<sub>2</sub>O<sub>3</sub>-PDMS films reaches 71.35% as the concentration of Al MPs increases to 15%. As a result, the film capacitance is enhanced 1.8 times, and TENG output performance is 6.67-times greater at 33.3 kPa and 4 Hz. The pressure sensitivity of 6.71 V/kPa and 0.18 μA/kPa is determined under the pressure range of 5.5–33.3 kPa. Based on these structures, we apply mesoporous Al<sub>2</sub>O<sub>3</sub>-PDMS film to a gapless TENG structure and obtain a linear pressure sensitivity of 1.00 V/kPa and 0.02 μA/kPa, respectively. Finally, we demonstrate self-powered safety cushion sensors for monitoring human sitting position by using gapless TENGs, which are developed with a large-scale and highly-deformable mesoporous Al<sub>2</sub>O<sub>3</sub>-PDMS film with dimensions of 6 × 5 pixels (33 × 27 cm<sup>2</sup>).
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