Muhammad Syaiful Fadly, Kusmono, Muhammad Waziz Wildan, Dody Ariawan, Teguh Dwi Widodo, Bakri Bakri, Rushdan Ahmad Ilyas, Yogi Angga Swasono
The growing demand for sustainable high-performance reinforcement materials has intensified research on nanocellulose derived from agricultural residues. However, the intrinsic hydrophilicity of cellulose nanofibers (CNF) remains a major limitation, as strong intermolecular hydrogen bonding promotes aggregation and restricts interfacial compatibility with hydrophobic polymer matrices. Addressing this challenge requires effective surface engineering strategies capable of modifying the polarity of nanocellulose while preserving its crystalline structure and thermal stability. Therefore, this study aims to comparatively investigate the effects of citric acid, amino-silane, and butyric anhydride surface modifications on the structural, morphological, thermal, dispersion, and wettability properties of cellulose nanofibers extracted from pineapple leaf fiber (PALF). In this study, cellulose nanofibers were successfully extracted from PALF, an abundant agro-industrial waste, through sequential alkalization, peroxide bleaching, and mechanical nanofibrillation using a conventional high-speed blender. To tailor the surface chemistry of CNF, three different modification approaches, namely citric acid esterification, amino-silane functionalization using 3-aminopropyltriethoxysilane (APTES), and butyric anhydride esterification, were comparatively investigated. The resulting cellulose nanofibers exhibited diameters of approximately 10.75 nm, confirming successful nanoscale fibrillation. Surface functionalization improved the physicochemical properties of CNF, increasing the crystallinity from 65.48% to 70.19% and enhancing the maximum thermal degradation temperature from 357.61 °C to 365.27 °C for butyric anhydride-modified CNF (BACNF). In addition, the water contact angle increased from 0° to 78.39° after butyric anhydride treatment, indicating enhanced hydrophobicity. These findings highlight the potential of pineapple leaf biomass as a sustainable precursor for high-quality nanocellulose with tunable surface properties for advanced polymer nanocomposite applications. © 2026 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Department of Mechanical and Industrial Engineering, Faculty of Engineering, Universitas Gadjah Mada, Jalan Grafika No. 2, Yogyakarta, 55281, Indonesia; Department of Mechanical Engineering, Faculty of Engineering, Universitas Tadulako, Jalan Soekarno Hatta Km. 9, Palu, 94148, Indonesia; Department of Mechanical Engineering, Faculty of Engineering, Universitas Sebelas Maret, Surakarta, 57126, Indonesia; Department of Mechanical Engineering, Faculty of Engineering, Brawijaya University, Malang, 65145, Indonesia; Department of Chemical Engineering, Faculty of Chemical and Energy Engineering, Universiti Teknologi Malaysia, UTM, Skudai, Johor, 81310, Malaysia; Research Center for Food Technology and Processing, National Research and Innovation Agency (BRIN), Gading, Playen, Gunungkidul, Yogyakarta, 55861, Indonesia
