We present a simple yet efficient method for orienting cellulose nanofibrils in layer-by-layer assembled films through spray-assisted alignment. While spraying at 90° against a receiving surface produces films with homogeneous in-plane orientation, spraying at smaller angles causes a macroscopic directional surface flow of liquid on the receiving surface and leads to films with substantial in-plane anisotropy when nanoscale objects with anisotropic shapes are used as components. First results with cellulose nanofibrils demonstrate that such fibrils are easily aligned by grazing incidence spraying to yield optically birefringent films over large surface areas. We show that the cellulosic nanofibrils are oriented parallel to the spraying direction and that the orientational order depends for example on the distance of the receiving surface from the spray nozzle. The alignment of the nanofibrils and the in-plane anisotropy of the films were independently confirmed by atomic force microscopy, optical microscopy between crossed polarizers, and the ellipsometric determination of the apparent refractive index of the film as a function of the in-plane rotation of the sample with respect to the plane of incidence of the ellipsometer.
Abstract. An extensive investigation of three different series of isotactic ethylene/propylene (EP) random copolymers was performed to understand the factors influencing the change in optical properties in the steam sterilization of extrusion cast films from such materials. Different analytical methods (differential scanning calorimetry (DSC), X-ray diffraction and electron microscopy) were employed to elucidate structural changes determining film optics, and in addition to the polymer structure parameters also nucleation and processing effects were studied. The findings clearly show that a combination of homogeneously randomized comonomer distribution and nucleation can partly inhibit lamellar thickening in sterilization, thus preserving high transparency even after a heat treatment. In detail, attention has to be paid to the combined effects of primary and secondary post-crystallization, which both are affected by the chain regularity.
The functionalization of chitosan with carboxymethyl groups allows zwitterionic or anionic chitosan derivatives to be obtained as a function of the degree of substitution. Here, we show that polyelectrolyte multilayers of chitosan and carboxymethylchitosan can be assembled by “dipping” or “spraying” to form strongly hydrated films in which both the polyanion and polycation possess the same polymer backbone (“matched chemistries”). Such films grow rapidly to fairly large thickness in very few assembly steps, especially in the case of “matched” charge densities, and atomic force microscopy reveals the formation of surface patterns that are dependent on the deposition conditions and on the number of layers. Interestingly, the influence of the molar masses of the polyelectrolyte pairs on the complex formation is somewhat counterintuitive, the stronger complexation occurring between polyanions and polycations of different (“non-matching”) lengths.
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