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<p>Hydrophilic cellulose nanocrystals (CNC) receive much attention as bio-based fillers, but their inherent hydrophilicity restricts utility in hydrophobic matrices. In this study, we focus on a tailored esterification strategy for the hydrophobic functionalization of CNC using palmitoyl chloride (C16). By varying the molar equivalents of the fatty acid chloride, this work expands upon existing protocols to precisely control surface substitution. CNC were produced under controlled conditions from <i>Leucaena leucocephala</i>, an invasive plant species with high cellulose content (58.05 ± 1.55%). Extraction involved sodium chlorite pretreatment followed by mild sulfuric acid hydrolysis with a protic co-solvent, yielding CNC with uniform rod-like morphology (416.5 ± 67.6&#xa0;nm) at ~ 50% yield. The resulting CNC palmitate exhibited increasing hydrophobicity with degree of substitution (DS), confirmed via FTIR and XRD. Microscopy revealed aggregation due to hydrophobic interactions. Surface modification improved compatibility with hydrophobic matrices: CNC palmitate increased the water contact angle of polyhydroxyalkanoate (PHA) films to 97.3 ± 0.7° and enhanced thermal stability. While current research emphasizes sustainable CNC production, this study highlights a scalable approach to surface engineering for improved dispersion and performance in hydrophobic polymer systems.</p>

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Hydrophobic modification of cellulose nanocrystals refined via non-fuming process from Leucaena leucocephala

  • 期刊论文

  • 发表日期：

    2025年6月16日

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  • Carine Shu Shien Lim,
  • Eric Wei Chiang Chan,
  • Hoong Chern Lee,
  • Chen Wai Wong

摘要

Hydrophilic cellulose nanocrystals (CNC) receive much attention as bio-based fillers, but their inherent hydrophilicity restricts utility in hydrophobic matrices. In this study, we focus on a tailored esterification strategy for the hydrophobic functionalization of CNC using palmitoyl chloride (C16). By varying the molar equivalents of the fatty acid chloride, this work expands upon existing protocols to precisely control surface substitution. CNC were produced under controlled conditions from Leucaena leucocephala, an invasive plant species with high cellulose content (58.05 ± 1.55%). Extraction involved sodium chlorite pretreatment followed by mild sulfuric acid hydrolysis with a protic co-solvent, yielding CNC with uniform rod-like morphology (416.5 ± 67.6 nm) at ~ 50% yield. The resulting CNC palmitate exhibited increasing hydrophobicity with degree of substitution (DS), confirmed via FTIR and XRD. Microscopy revealed aggregation due to hydrophobic interactions. Surface modification improved compatibility with hydrophobic matrices: CNC palmitate increased the water contact angle of polyhydroxyalkanoate (PHA) films to 97.3 ± 0.7° and enhanced thermal stability. While current research emphasizes sustainable CNC production, this study highlights a scalable approach to surface engineering for improved dispersion and performance in hydrophobic polymer systems.