The piezoelectric properties of poly(vinylidene fluoride) (PVDF) are largely determined by the interplay among β-phase content, crystallite size, and domain polarization. However, conventional melt processing methods generally yield limited efficiency in inducing and stabilizing the β-phase, thus constraining the achievable piezoelectric output of PVDF films. Here, we introduce a cyclic shear–compression (CSC) approach that enables the formation of PVDF films consisting predominantly of ultrafine β-phase crystallites. When processed above the melting temperature (T > Tm), the CSC method facilitates rapid film formation, yielding thicknesses as low as 16 μm while enhancing the crystallinity by 50%. In the solid state (T < Tm), CSC processing further refines the piezoelectric microstructure, increasing the β-phase fraction to 76% and reducing the crystallite size to 5.4 nm, alongside promoting domain polarization. As a result, the CSC-processed PVDF films exhibit a remarkable open-circuit voltage of 26.1 V. This work establishes CSC processing as an efficient and eco-friendly route for precise phase engineering in PVDF, opening a promising avenue for developing high-performance piezoelectric polymer films.
Wang et al. (Sat,) studied this question.
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