Bioinspired Architecture of Ultra-strong Yet Tough Polyvinyl Alcohol Nanocomposites via Orientational Reinforcement with Cellulose Nanocrystals

Abstract

Porous films with high strength and toughness are in high demand for energy storage, flexible electronics, and biomedical applications. However, balancing mechanical performance with controlled pore architecture remains challenging. In this study, a bioinspired strategy was employed to fabricate strong and tough cellulose nanocrystals (CNC)-reinforced polyvinyl alcohol (PVA) composite nanofibers using a modified electrospinning technique. This approach yields a well-ordered soft–hard intercalated structure inspired by natural spider silk. By tuning CNC content and nanofiber orientation, the resulting CNC/PVA composite nanofiber-based films exhibit excellent specific strength (156.8 MPa g⁻¹ cm⁻³), high toughness (27.3 MJ m⁻²), and tunable porosity (68–90%). Additionally, these films exhibit excellent thermal stability, enhanced electrolyte wettability, and a well-controlled pore architecture, rendering them highly effective as lithium-ion battery separators that effectively suppress lithium dendrite growth. Compared to conventional plastic films (e.g., Polypropylene, Polyethylene), the aligned CNC/PVA nanofiber film has a lower carbon footprint and inherent biodegradability. This work presents a sustainable pathway for developing high-performance porous materials with promising applications in renewable energy systems, flexible electronics, and related fields.

Keywords

Nanocomposites / Cellulose nanocrystals / Oriented reinforcement / Sustainable application / Life cycle assessment

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Funding

National Natural Science Foundation of China(32271792)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China

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