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<p>This study investigates the application of cellulose nanofibrils extracted from spent coffee grounds (SCGNF) as sustainable reinforcing fillers for natural rubber (NR) composites. While nanocellulose from sources such as bagasse and rice husk has been extensively studied, SCGNF remains underexplored, particularly under peroxide curing systems, despite its potential for waste valorization and green elastomer development. SCGNF was isolated via alkali treatment, bleaching, and sulfuric acid hydrolysis, then functionalized with triethoxyvinylsilane (TEVS) to improve compatibility with the hydrophobic NR matrix. The fillers were characterized by FTIR, TGA, XPS, and TEM before incorporation. NR composites were prepared via latex compounding and peroxide vulcanization using dicumyl peroxide. Mechanical testing showed that both SCGNF and V-SCGNF enhanced stiffness and strength. NR/V-SCGNF at 5 phr achieved the highest tensile strength of 23.0 ± 0.7&#xa0;MPa, a 25% improvement over unfilled NR (18.4 ± 0.8&#xa0;MPa). At 10 phr, hardness increased from 30.4 to 35.2 Shore A, and M<sub>100</sub> more than doubled from 0.9&#xa0;MPa to 2.0&#xa0;MPa. Swelling degree decreased after silane treatment, likely due to stronger rubber-filler interaction. SEM confirmed better dispersion and interfacial adhesion in V-SCGNF, whereas SCGNF-filled samples showed agglomeration and voids. These improvements were statistically significant (<i>p</i> &lt; 0.05). Overall, surface-modified SCGNF demonstrates effective bio-based reinforcement, highlighting the value of upcycling spent coffee grounds into functional nanofillers for sustainable elastomer applications.</p> Graphical abstract <p></p>

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Valorization of spent coffee grounds into functional nanofibrils for sustainable reinforcement of peroxide-cured natural rubber composites

  • 期刊论文

  • 发表日期：

    2025年12月6日

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  • Panjalak Meetam,
  • Peerayut Tapangnoi,
  • Pongdhorn Sae-Oui,
  • Chomsri Siriwong

摘要

This study investigates the application of cellulose nanofibrils extracted from spent coffee grounds (SCGNF) as sustainable reinforcing fillers for natural rubber (NR) composites. While nanocellulose from sources such as bagasse and rice husk has been extensively studied, SCGNF remains underexplored, particularly under peroxide curing systems, despite its potential for waste valorization and green elastomer development. SCGNF was isolated via alkali treatment, bleaching, and sulfuric acid hydrolysis, then functionalized with triethoxyvinylsilane (TEVS) to improve compatibility with the hydrophobic NR matrix. The fillers were characterized by FTIR, TGA, XPS, and TEM before incorporation. NR composites were prepared via latex compounding and peroxide vulcanization using dicumyl peroxide. Mechanical testing showed that both SCGNF and V-SCGNF enhanced stiffness and strength. NR/V-SCGNF at 5 phr achieved the highest tensile strength of 23.0 ± 0.7 MPa, a 25% improvement over unfilled NR (18.4 ± 0.8 MPa). At 10 phr, hardness increased from 30.4 to 35.2 Shore A, and M100 more than doubled from 0.9 MPa to 2.0 MPa. Swelling degree decreased after silane treatment, likely due to stronger rubber-filler interaction. SEM confirmed better dispersion and interfacial adhesion in V-SCGNF, whereas SCGNF-filled samples showed agglomeration and voids. These improvements were statistically significant (p < 0.05). Overall, surface-modified SCGNF demonstrates effective bio-based reinforcement, highlighting the value of upcycling spent coffee grounds into functional nanofillers for sustainable elastomer applications.

Graphical abstract