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Facile preparation of optically transparent film of acetylated cellulose nanofiber-reinforced poly(methyl methacrylate) utilizing cosolvency in aqueous ethanol

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Abstract

Composite films of cellulose nanofibers (CNFs) and poly(methyl methacrylate) (PMMA) are fabricated typically by solution-casting using an organic solvent (e.g., chloroform) that can dissolve PMMA. However, the preparation of the casting dope using the previously reported method requires multistep procedures for the solvent exchange of the CNF suspension from water to the organic solvent. Here we developed a facile method utilizing the cosolvency of PMMA in aqueous ethanol (EtOH aq.) to fabricate an optically transparent CNF-reinforced PMMA film. In this study, an acetylated-CNF (Ac-CNF) was used as a hydrophobic filler for compatibility with a hydrophobic PMMA matrix. First, an appropriate amount of EtOH was added dropwise to Ac-CNF aq. suspension to adjust the EtOH concentration to 80 vol%. PMMA was then added to the solution and dissolved under heating above the upper critical solution temperature to yield a clear casting dope. The dope is cast at 65 °C and then dried at 45 °C for 24 h in a closed oven to obtain an Ac-CNF/PMMA composite film. The composite film with 1% Ac-CNFs exhibited high total-light transmittance (93%) and low haze (4.4%), while 1.3-times higher tensile strength and Young’s modulus than the neat PMMA film, indicating the effective reinforcement of PMMA by the well-dispersed Ac-CNFs. Thus, this method enables the facile preparation of an Ac-CNF/PMMA composite film with excellent transparency and enhanced mechanical performance.

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Acknowledgments

The authors thank Dr. Masanori Yasui and Mr. Toshiaki Ito (Electron Microscope Laboratory, Research Faculty of Agriculture, Hokkaido University) for supporting our microscopic observations.

Funding

This work was financially supported by a Promotion for Young Research Talent and Network from the Northern Advancement Center for Science and Technology (NOASTEC) Foundation to S.S.

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ST planed the study conception, and SS and YU supervised the work. IT performed film preparation, tensile tests, UV-vis measurements, and data analysis. ST did TG measurements. SS carried out SEM observations and haze measurements, kindly supported by TI. ST wrote the first draft of the manuscript, and SS and YU revised the manuscript. All authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Correspondence to Shiori Suzuki.

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The authors declare no competing interest.

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Taira, S., Tanouchi, I., Suzuki, S. et al. Facile preparation of optically transparent film of acetylated cellulose nanofiber-reinforced poly(methyl methacrylate) utilizing cosolvency in aqueous ethanol. Cellulose 31, 1559–1568 (2024). https://doi.org/10.1007/s10570-023-05625-7

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  • DOI: https://doi.org/10.1007/s10570-023-05625-7

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