Fabrication of Zwitterionized Nanocellulose/Polyvinyl Alcohol Composite Hydrogels Derived from Camellia Oleifera Shells for High-Performance Flexible Sensing.

To address the growing demand for environmentally friendly flexible sensors, here, a composite hydrogel of nanocellulose (NC) and polyvinyl alcohol (PVA) was designed and fabricated using shells as a sustainable alternative to petroleum-based raw materials. Firstly, NC was extracted from shells and modified with 2-chloropropyl chloride to obtain a nanocellulose-based initiator (Init-NC) for atomic transfer radical polymerization (ATRP). Subsequently, sulfonyl betaine methacrylate (SBMA) was polymerized by Init-NC initiating to yield zwitterion-functionalized nanocellulose (NC-PSBMA). Finally, the NC-PSBMA/PVA hydrogel was fabricated by blending NC-PSBMA with PVA. A Fourier transform infrared spectrometer (FT-IR), proton nuclear magnetic resonance spectrometer (NMR), X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), universal mechanical testing machine, and digital source-meter were used to characterize the chemical structure, surface microstructure, and sensing performance. The results indicated that: (1) FT-IR and NMR confirmed the successful synthesis of NC-PSBMA; (2) SEM, TEM, and alternating current (AC) impedance spectroscopy verified that the NC-PSBMA/PVA hydrogel exhibits a uniform porous structure (pore diameter was 1.1737 μm), resulting in significantly better porosity (15.75%) and ionic conductivity (2.652 S·m) compared to the pure PVA hydrogel; and (3) mechanical testing combined with source meter testing showed that the tensile strength of the composite hydrogel increased by 6.4 times compared to the pure PVA hydrogel; meanwhile, it showed a high sensitivity (GF = 1.40, strain range 0-5%; GF = 1.67, strain range 5-20%) and rapid response time (<0.05 s). This study presents a novel approach to developing bio-based, flexible sensing materials.