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Controlling the surface structure and functionalization of a cellulose nanocrystal film modified by using glycidyloxypropylsilane in a coating process


We herein focused on the structural control and surface functionalization of a cellulose nanocrystal (CNC) film by modifying it with silane coupling reagents. Organosilanes containing a glycidyl group such as diethoxy(3-glycidyloxypropyl)(methyl)silane (GPMDES) and triethoxy(3-glycidyloxypropyl)silane (GPTES) in combination with tetraethoxysilane (TEOS) were selected as compounds for CNC surface modification with a spin coating process. Fourier transform infrared (FT-IR) and nuclear magnetic resonance (29Si-NMR) spectra indicated that the silane compounds were chemically bonded to the CNC surface, and both the glycidyl and methyl groups of GPMDES were detected. The surface of the CNC film observed by atomic force microscopy (AFM) retained the rod-shaped structure of the original CNCs. The surface roughnesses of the CNC films using GPMDES/TEOS and GPTES/TEOS as coprecursors were Sa = 4.9 nm and Sa = 3.7 nm, respectively. The water contact angle of the CNC films was 18° for GPMDES/TEOS and 36° for GPTES/TEOS. These results imply that the surface roughness of the silane-modified CNC film contributed to its hydrophilicity despite the existence of the hydrophobic methyl group. The adhesion strength of the silane-modified CNC film with the chitosan cast film was found to be 23 mN/mm for the 180° peel test, suggesting the reaction of glycidyl groups with amino groups.

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Correspondence to Koji Takagi.

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Taniyama, H., Takagi, K. Controlling the surface structure and functionalization of a cellulose nanocrystal film modified by using glycidyloxypropylsilane in a coating process. Polym J 55, 675–682 (2023).

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