We studied the surface
and microstructure of cellulose acetate
(CA) films to tailor their barrier and mechanical properties for application
in electrochromic devices (ECDs). Cross-linking of CA was carried
out with pyromellitic dianhydride to enhance the properties relative
to unmodified CA: solvent resistance (by 43% in acetone and 37% in
DMSO), strength (by 91% for tensile at break), and barrier (by 65%
to oxygen and 92% to water vapor). Surface modification via tetraethyl
orthosilicate and octyltrichlorosilane endowed the films with hydrophobicity,
stiffness, and further enhanced solvent resistance. A detailed comparison
of structural, chemical, surface, and thermal properties was performed
by using X-ray diffraction, dynamic mechanical analyses, Fourier-transform
infrared spectroscopy, and atomic force microscopy. Coplanar ECDs
were synthesized by incorporating a hydrogel electrolyte comprising
TEMPO-oxidized cellulose nanofibrils and an ionic liquid. When applied
as the top layer in the ECDs, cross-linked and hydrophobized CA films
extended the functionality of the assembled displays. The results
indicate excellent prospects for CA films in achieving environmental-friendly
ECDs that can replace poly(ethylene terephthalate)-based counterparts.