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Bi-axially oriented electroactive PVDF thin films were prepared by a 3D printing process during which multiple parameters play a critical role in enhancing β-phase and crystallinity of the thin films. The PVDF molecular chains were rotated and stretched to form orderly arrangement by the pulling of in situ strong auxiliary electric potential (voltage) and the mechanical pulling force, and the aligned PVDF molecular chains improved the crystallinity of the thin films. Doping very small amount of multi-walled carbon nanotubes (MWCNTs) or graphene (GR) as a nucleating agent significantly increased the content of the β-phase in the films. Adding GR behaved is better than the MWCNTs in improving the β-phase due to the lamellar structure of graphene can generate a large number of micro electric fields stimulating the transformation of molecular chain from trans-gauche-trans-gauche(TG + TG − ) to all-trans (TTTT). The content of β-phase in the PVDF/GR(0.03 wt%) composite thin film researched at 61.52%. Under the special environment of 3D printing, the printed PVDF thin films became very dense with high βphase after depositing layer-by-layer. It exhibited good piezoelectric properties without postpoling treatment and mechanical stretching.

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