Title Sustainable fabrication of piezoceramic-rich and graphene-based composites for fully 3D-printed flexible sensors
Authors Daukševičius, Rolanas ; Kompelli, Gopi ; Svirskas, Šarūnas ; Jasiūnienė, Elena ; Cicėnas, Vaidotas ; Turczyn, Roman
DOI 10.1088/1361-665X/ae8cc8
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Is Part of Smart materials and structures.. Bristol : Institute of Physics. 2026, vol. 35, iss. 7, art. no. 075049, p. 1-24.. ISSN 0964-1726. eISSN 1361-665X
Keywords [eng] FDM ; thermoplastic ; nanocomposite ; percolation ; piezoelectricity ; polarization ; hysteresis
Abstract [eng] Progress in additively manufactured piezoelectrics is impeded by environmental, regulatory and scalability concerns related to solvent processing. Hazardous solvents dominate the preparation of polyvinylidene fluoride (PVDF)-based piezocomposites for fused filament fabrication (FFF), which remains underdeveloped compared to solvent-assisted additive electronics technologies. The piezoelectric performance of existing FFF-printed PVDF composites is limited due to moderate ferroelectric ceramic content (≲35 vol%). Solvent-free processing and multi-material FFF of highly ceramic-filled (≳50 vol%) piezoelectric devices are largely underexplored. Herein, we report the fully melt-based fabrication of a flexible lead-free piezocomposite filament, highly filled with barium titanate (BTO) particles at the upper printability threshold (~55 vol%), enabling FFF of piezoelectric sensors with co-printed graphene-doped electrodes. X-ray microtomography and tensile testing indicate that re-extrusion provides uniform filler dispersion in a soft PVDF copolymer (PVDF-HFP) matrix. The multi-material FFF process is fine-tuned to deliver consistent 3D printing of well-fused ceramic-rich and graphene-doped sheets as indicated by strain-rate strengthening behavior. Adding 8 wt% graphene nanoplatelets (GNPs) yields 1.6 S/cm conductivity and <100 Ω/sq sheet resistance, sufficient for effective strong-field poling (≳20 kV/mm). The achieved maximum values of d 33 (35.4 pC/N) and dielectric constant (108 at 1 kHz) are comparable to or exceed solvent-processed counterparts, aligning with predictions of effective medium models. The 3D-printed vibration sensors exhibit practically usable d 31 -mode sensitivity with high linearity and repeatability, confirming FFF reproducibility. This study establishes a scalable and cost-effective solvent-free process for environmentally responsible material extrusion (MEX) additive manufacturing of flexible piezoelectric devices, addressing current limitations in composite filling level and processing sustainability.
Published Bristol : Institute of Physics
Type Journal article
Language English
Publication date 2026
CC license CC license description