Flexible cellulose-based piezoelectric composite membrane involving PVDF and BaTiO3 synthesized with the assistance of TEMPO-oxidized cellulose nanofibrils

Meilin Li; Bei Jiang; Shuoang Cao; Xinyi Song; Yuanqiao Zhang; Lijun Huang; Quanping Yuan

doi:10.1039/d3ra00604b

Flexible cellulose-based piezoelectric composite membrane involving PVDF and BaTiO₃ synthesized with the assistance of TEMPO-oxidized cellulose nanofibrils

RSC Adv. 2023 Mar 31;13(15):10204-10214. doi: 10.1039/d3ra00604b. eCollection 2023 Mar 27.

Authors

Meilin Li^{1

2}, Bei Jiang^{1

2}, Shuoang Cao^{1

2}, Xinyi Song^{1

2}, Yuanqiao Zhang^{1

2}, Lijun Huang^{1

2}, Quanping Yuan^{1

2}

Affiliations

¹ School of Resources, Environment and Materials, Guangxi University Nanning 530004 China yuanquanping@gxu.edu.cn.
² State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, Guangxi University Nanning 530004 China.

Abstract

High-performance flexible barium titanate (BaTiO₃)-based piezoelectric devices have gained much attention. However, it is still a challenge to prepare flexible polymer/BaTiO₃-based composite materials with uniform distribution and high performance due to the high viscosity of polymers. In this study, novel hybrid BaTiO₃ particles were synthesized with assistance of TEMPO-oxidized cellulose nanofibrils (CNFs) via a low-temperature hydrothermal method and explored for their application in piezoelectric composites. Specifically, Ba²⁺ was adsorbed on uniformly dispersed CNFs with a large amount of negative charge on their surface, which nucleated, resulting in the synthesis of evenly dispersed CNF-BaTiO₃. The obtained CNF-BaTiO₃ possessed a uniform particle size, few impurities, high crystallinity and dispersity, high compatibility with the polymer substrate and surface activity due to the existence of CNFs. Subsequently, both polyvinylidene fluoride (PVDF) and TEMPO-oxidized CNFs were employed as piezoelectric substrates for the fabrication of a CNF/PVDF/CNF-BaTiO₃ composite membrane with a compact structure, displaying the tensile strength of 18.61 ± 3.75 MPa and elongation at break of 3.06 ± 1.33%. Finally, a thin piezoelectric generator (PEG) was assembled, which output a considerable open-circuit voltage (4.4 V) and short-circuit current (200 nA), and could also power a light-emitting diode and charge a 1 μF capacitor to 3.66 V in 500 s. Its longitudinal piezoelectric constant (d ₃₃) was 5.25 ± 1.04 pC N^-1 even with a small thickness. It also exhibited high sensitivity to human movement, outputting a voltage of about 9 V and current of 739 nA for only a footstep. Thus, it exhibited good sensing property and energy harvesting property, presenting practical application prospects. This work provides a new idea for the preparation of hybrid BaTiO₃ and cellulose-based piezoelectric composite materials.