Advancing Charge Density in Temperature‐Dependent Amphiphile Metal–Organic Polyhedra‐Based Triboelectric Nanogenerators

Abstract In this study, a mechanically flexible structure, a cuboctahedral metal‐organic polyhedra (MOP) Cu 24 5‐(octyloxy) isophthalic acid 24 Cu (II) paddlewheel clusters coordinated with (5‐(octyloxy) isophthalate), resulting in significantly enhanced hydrolytic stability are prepared. It should be noted that CuMOP‐1 exhibits evenly and symmetrically distributed non‐polar long alkyl chains and polar hydroxy groups, facilitating self‐assembly into higher‐order structures reminiscent of amphiphiles. Furthermore, the resultant CuMOP‐1 undergoes a phase change at 150–160 °C as confirmed temperature‐dependent Raman spectroscopy (RS), thermogravimetric analysis and Differential Scanning Calorimetry (TGA‐DSC). The possible use of Cu‐MOP‐1 for capturing mechanical energy is demonstrated by creating a flexible hybrid piezoelectric‐triboelectric nanogenerator (HP‐TENG). The resultant CuMOP‐1@ Polyvinylidene fluoride(PVDF) membrane‐based HP‐TENG demonstrates enhanced triboelectric output voltage of 547.5 V, current density of 15.16 µAcm −2 , and power density of 2.8 mWcm −2 due to its increased surface charge density and a substantial rise in the dielectric constant. Furthermore, the amphiphiles and phase change in CuMOP‐1 lead to ∽73% increase in voltage and 60% in current density of HP‐TENG in high‐temperature (140 °C) environments. HP‐TENG also exhibits exceptional temperature‐ and pressure‐sensing abilities, with sensitivities of 1.81 V°C −1 and 7.12 V°kPa −1 , respectively, showcasing its feasibility over a wide range of temperatures and pressures.