One property of sulfated cellulose nanocrystals (CNCs) is their ability to self-assemble from a concentrated suspension under specific drying conditions into an iridescent film. Such colored films are very brittle, which makes them difficult to handle or integrate within an industrial process. The goal of this study is (i) to produce flexible films using neutral poly(ethylene glycol) (PEG) and (ii) to modulate their coloration using an anionic polyacrylate (PAAS). The first part is dedicated to studying the physicochemical interactions of the two polymers with CNCs using techniques such as zeta potential measurements, dynamic light scattering (DLS), quartz crystal microbalance (QCM), and atomic force microscopy (AFM). Iridescent solid films were then produced and characterized using scanning electron microscopy (SEM) and UV-visible spectroscopy. The mechanical and thermal properties of films incorporating CNC were measured to evaluate improvements in flexibility. The addition of 10 wt % of PEG makes these films much more flexible (with a doubling of the elongation), with the coloration being preserved and the temperature of degradation increasing by almost 35 °C. Up to 160 μmol/gCNC PAAS can be added to tune the coloration of the CNC films by producing a more narrow, stronger coloration in the visible spectrum (higher absorption) with a well-pronounced fingerprint texture.
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