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Open AccessDOI: pub_80__articleID_239Original Research

Enhanced Mechanical Properties and Thermal Stability of Poly(Lactic Acid) Composites Reinforced with Modified Cellulose Nanofibers

ZHANG Wei¹,LI Ming¹,WANG Fang¹

Institute of Polymer Science and Engineering, Tsinghua University

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Enhanced Mechanical Properties and Thermal Stability of Poly(Lactic Acid) Composites Reinforced with Modified Cellulose Nanofibers
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Published In
Chinese Journal of New Drugs
Published:January 15, 2025Edition:Vol 34, Issue 15 • pp. 100-112Citation:ZHANG Wei et al. (2025), Chinese Journal of New Drugs
Impact FactorPremier Chinese Biomedical Journal indexed in SinoBioData: Chinese Journal of New Drugs (中国新药杂志).
Source Journal中国新药杂志

Key Takeaways & Executive Findings

  • • • Tensile strength of PLA increased from 58.2 MPa to 72.4 MPa (24.4% improvement) at 3 wt% modified CNF loading, enabling use in structural applications where neat PLA fails. • • Young's modulus rose from 2.1 GPa to 3.0 GPa (42.9% increase) at 3 wt% CNF, providing greater stiffness for load-bearing components. • • Thermal stability improved: T5% (temperature at 5% weight loss) increased from 315°C to 338°C at 3 wt% CNF, extending the processing window and service temperature range. • • Glass transition temperature (Tg) shifted from 58°C to 63°C at 3 wt% CNF, indicating enhanced dimensional stability under elevated temperatures, critical for automotive under-hood applications.

Abstract

Poly(lactic acid) (PLA) composites reinforced with cellulose nanofibers (CNFs) were prepared via melt blending followed by injection molding. CNFs were surface-modified with a silane coupling agent to improve interfacial adhesion. The effects of CNF content (0–5 wt%) on mechanical properties, thermal stability, and dynamic mechanical behavior were systematically investigated. Tensile strength increased from 58.2 MPa (neat PLA) to 72.4 MPa at 3 wt% CNF, a 24.4% improvement, while Young's modulus rose from 2.1 GPa to 3.0 GPa (42.9% increase). Flexural strength and modulus also improved significantly. Thermal stability, assessed by TGA, showed that the temperature at 5% weight loss (T5%) increased from 315°C to 338°C at 3 wt% CNF, indicating enhanced thermal resistance. DMA revealed a notable increase in storage modulus and a shift in glass transition temperature (Tg) from 58°C to 63°C, suggesting restricted polymer chain mobility due to strong CNF-PLA interactions. SEM micrographs confirmed uniform dispersion of CNFs at low loadings, with agglomeration observed at 5 wt%. The optimal CNF content was determined to be 3 wt%, providing a balance between mechanical reinforcement and processability. These findings demonstrate that surface-modified CNFs are effective bio-based reinforcing agents for PLA, offering a sustainable route to high-performance biodegradable composites for packaging and automotive applications.

1. Introduction

Poly(lactic acid) (PLA) is a promising bio-based polymer for reducing dependence on petroleum-derived plastics, yet its widespread adoption is hindered by inherent brittleness, low heat deflection temperature, and poor thermal stability. Conventional reinforcements such as glass fibers improve mechanical properties but compromise biodegradability and increase density. Cellulose nanofibers (CNFs) offer an eco-friendly alternative due to their high specific strength, low density, and renewable nature. However, the hydrophilic nature of CNFs leads to poor dispersion in hydrophobic PLA matrices and weak interfacial adhesion, resulting in limited reinforcement. Prior attempts using unmodified CNFs have yielded modest improvements, with tensile strength gains typically below 10% and often accompanied by decreased elongation at break.

This study addresses the interfacial incompatibility by surface-modifying CNFs with a silane coupling agent, which introduces hydrophobic moieties that enhance compatibility with PLA. The modified CNFs were incorporated into PLA via melt blending, a scalable industrial process. The experimental protocol systematically varied CNF content from 0 to 5 wt% and evaluated mechanical, thermal, and dynamic mechanical properties. The results demonstrate that at an optimal loading of 3 wt%, tensile strength and modulus are significantly enhanced without sacrificing processability, while thermal stability is markedly improved. This work provides a practical pathway to producing high-performance PLA composites suitable for packaging, automotive, and consumer goods, where both mechanical integrity and thermal resistance are critical.

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Cite This Research Paper
ZHANG Wei, LI Ming, WANG Fang (2025). Enhanced Mechanical Properties and Thermal Stability of Poly(Lactic Acid) Composites Reinforced with Modified Cellulose Nanofibers. Chinese Journal of New Drugs. https://doi.org/pub_80__articleID_239
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Frequently Asked Questions

What is the optimal CNF loading to balance mechanical reinforcement and processability, and what are the trade-offs at higher loadings?

The optimal CNF content is 3 wt%, yielding a 24.4% increase in tensile strength (to 72.4 MPa) and a 42.9% increase in Young's modulus (to 3.0 GPa). At 5 wt% CNF, agglomeration occurs, leading to a decrease in tensile strength to 68.5 MPa and a reduction in elongation at break, indicating a trade-off between reinforcement and ductility.

How does the silane surface modification of CNFs improve interfacial adhesion, and what evidence supports enhanced compatibility?

Silane coupling agents react with hydroxyl groups on CNF surfaces, introducing organic moieties that increase hydrophobicity and compatibility with PLA. Evidence includes improved dispersion observed in SEM micrographs, increased Tg (from 58°C to 63°C) indicating restricted chain mobility, and enhanced tensile strength without sacrificing elongation at low loadings, all pointing to stronger interfacial bonding.

What is the impact of CNF addition on the thermal stability of PLA, and does it affect the processing window?

The temperature at 5% weight loss (T5%) increased from 315°C for neat PLA to 338°C at 3 wt% CNF, indicating a 23°C improvement in thermal stability. This broadens the processing window and allows for higher service temperatures, which is critical for applications such as hot-fill packaging or automotive components.

Are the mechanical property improvements consistent across different testing modes (tensile, flexural, dynamic mechanical)?

Yes, improvements were observed across all testing modes. Flexural strength increased from 82.3 MPa to 96.7 MPa (17.5% increase) at 3 wt% CNF, and flexural modulus rose from 3.2 GPa to 4.1 GPa (28.1% increase). DMA showed a significant increase in storage modulus across a wide temperature range, confirming enhanced stiffness under dynamic loading.

What are the scalability prospects of this melt blending approach for industrial production?

Melt blending is a standard industrial technique, and the CNF loadings used (up to 5 wt%) are compatible with conventional twin-screw extruders. The silane modification can be performed in a batch process prior to compounding. The observed improvements at 3 wt% CNF suggest that cost-effective production is feasible, though the cost of modified CNFs must be weighed against performance gains.

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