Tuning the Architecture of Cellulose Nanocrystal–Poly(allylamine hydrochloride) Multilayered Thin Films: Influence of Dipping Parameters

Abstract

Multilayered thin films consisting of alternating cationic polyelectrolyte, poly(allylamine hydrochloride) (PAH), and anionic cellulose nanocrystals (CNs) were constructed using the dipping procedure by screening different experimental parameters: the drying step between each layer adsorption, the dipping time, the ionic strength of the PAH solution, and the concentration of CNs dispersion. We showed that the drying process and the ionic strength of PAH solution were crucial parameters for the successful construction of 8-bilayer films. Film thickness is mainly influenced by dipping time and CN concentration when using the dipping procedure without drying. Two architectures of adsorbed CN layers-a single or a double layer of CNs-were revealed on the basis of the thickness increment per bilayer, depending on experimental conditions. The layer adsorption process was investigated in real-time using quartz crystal microbalance with dissipation (QCM-D) experiments in an aqueous environment or by incorporating a drying step. On the basis of in situ construction of PAH-CN films in wet media, QCM-D data were indicative of highly hydrated films for which the progressive layer stacking is disturbed or prevented. QCM-D monitoring of CNs and PAH layer adsorption was monitored by incorporating a drying process. The impact of experimental parameters on PAH-CN multilayered construction and on CN layer configuration is discussed. This study offers new opportunities for tailoring the architecture of CN-based multilayer films.