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<p>Against the backdrop of global carbon neutrality goals, the development of high-performance polylactic acid (PLA) materials is of increasing importance. However, the inherent brittleness, hydrophobicity, and limited toughness of PLA restrict its broader applications. This study proposes an interfacial regulation strategy, using self-synthesized poly(butylene adipate)-based polyurethane prepolymer (PBAPU) as a compatibilizer and bio-based cellulose nanofibrils (CNFs) as a reinforcing phase, to prepare a series of CNF/PLA composites via melt blending. Fourier transform infrared spectroscopy indicates the consumption of reactive isocyanate (–NCO) groups during processing, suggesting the occurrence of extensive interfacial reactions involving hydroxyl-containing species in the system. Combined with scanning electron microscopy observations, these results imply the formation of an interconnected interfacial interaction network that improves compatibility between CNF and the PLA matrix. When the CNF content was 5 wt%, the composite exhibited optimal comprehensive properties. The impact strength and elongation at break reached 8.0&#xa0;kJ·m<sup>−2</sup> and 18.1%, representing increases of 116.2% and 147.9%, respectively, compared with neat PLA, while the tensile strength was maintained at 50.3&#xa0;MPa. Moreover, the composites retained good thermal stability, and their surface wettability was significantly enhanced, as evidenced by a marked decrease in water contact angle. This work suggests that effective interfacial regulation through polyurethane prepolymers and nanocellulose enables the simultaneous toughening, strengthening, and hydrophilization of PLA, providing a feasible strategy for the design of high-performance bio-based composites.</p> Graphical Abstract <p></p>

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Polyurethane prepolymers compatibilized cellulose nanofibrils/polylactic acid composites: Interfacial regulation, structure, and properties

  • 期刊论文

  • 发表日期：

    2026年5月24日

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  • Fangqing Weng,
  • Chengyue Wu,
  • Duyu Guo,
  • Qing Huang,
  • Yu Zhang,
  • Qiangxian Wu,
  • Lanlan Cui,
  • Jiamin Deng

摘要

Against the backdrop of global carbon neutrality goals, the development of high-performance polylactic acid (PLA) materials is of increasing importance. However, the inherent brittleness, hydrophobicity, and limited toughness of PLA restrict its broader applications. This study proposes an interfacial regulation strategy, using self-synthesized poly(butylene adipate)-based polyurethane prepolymer (PBAPU) as a compatibilizer and bio-based cellulose nanofibrils (CNFs) as a reinforcing phase, to prepare a series of CNF/PLA composites via melt blending. Fourier transform infrared spectroscopy indicates the consumption of reactive isocyanate (–NCO) groups during processing, suggesting the occurrence of extensive interfacial reactions involving hydroxyl-containing species in the system. Combined with scanning electron microscopy observations, these results imply the formation of an interconnected interfacial interaction network that improves compatibility between CNF and the PLA matrix. When the CNF content was 5 wt%, the composite exhibited optimal comprehensive properties. The impact strength and elongation at break reached 8.0 kJ·m−2 and 18.1%, representing increases of 116.2% and 147.9%, respectively, compared with neat PLA, while the tensile strength was maintained at 50.3 MPa. Moreover, the composites retained good thermal stability, and their surface wettability was significantly enhanced, as evidenced by a marked decrease in water contact angle. This work suggests that effective interfacial regulation through polyurethane prepolymers and nanocellulose enables the simultaneous toughening, strengthening, and hydrophilization of PLA, providing a feasible strategy for the design of high-performance bio-based composites.

Graphical Abstract