Bismuth containing hybrid molecular ferroelectrics are receiving tremendous attention in recent years owing to their stable and non‐toxic composition. However, these perovskite‐like structures are primarily limited to ammonium cations. Herein, we report a new phosphonium based discrete perovskite‐like hybrid ferroelectric with a formula [Me(Ph)3P]3[Bi2Br9] (MTPBB) and its mechanical energy harvesting capability. The Polarization‐Electric field (P‐E) measurements resulted in a well‐defined ferroelectric hysteresis loop with a remnant polarization value of 2.1 μC cm−2. Piezoresponse force microscopy experiments enabled visualization of the ferroelectric domain structure and evaluation of the piezoelectric strain coefficient (d33) for an MTPBB single crystal and thin film sample. Furthermore, flexible devices incorporating MTPBB in polydimethylsiloxane (PDMS) matrix at various concentrations were fabricated and explored for their mechanical energy harvesting properties. The champion device with 20 wt % of MTPBB in PDMS rendered a maximum peak‐to‐peak open‐circuit voltage of 22.9 V and a maximum power density of 7 μW cm−2 at an optimal load of 4 MΩ. Moreover, the potential of MTPBB‐based devices in low power electronics was demonstrated by storing the harvested energy in various electrolytic capacitors.
Cyclophosphazenes offer a robust and easily modifiable platform for a diverse range of functional systems that have found applications in a wide variety of areas. Herein, for the first time, it reports an organophosphazene‐based supramolecular ferroelectric [(PhCH2NH)6P3N3Me]I, [PMe]I. The compound crystallizes in the polar space group Pc and its thin‐film sample exhibits remnant polarization of 5 µC cm−2. Vector piezoresponse force microscopy (PFM) measurements indicated the presence of multiaxial polarization. Subsequently, flexible composites of [PMe]I are fabricated for piezoelectric energy harvesting applications using thermoplastic polyurethane (TPU) as the matrix. The highest open‐circuit voltages of 13.7 V and the maximum power density of 34.60 µW cm−2 are recorded for the poled 20 wt.% [PMe]I/TPU device. To understand the molecular origins of the high performance of [PMe]I‐based mechanical energy harvesting devices, piezoelectric charge tensor values are obtained from DFT calculations of the single crystal structure. These indicate that the mechanical stress‐induced distortions in the [PMe]I crystals are facilitated by the high flexibility of the layered supramolecular assembly.
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