Dispersions of nanofillers into aqueous and solid biopolymeric matrices were studied from the physicochemical viewpoint. This work was carried out based on the idea that the combination of biopolymers, derived from renewable resources, and nanofiller, environmentally friendly, may form a new generation of nanomaterials with excellent and unique properties at low cost. To this purpose, two pectins with different degrees of methyl esterification and nanoclays like halloysite and laponite RD were selected. The thermodynamic and structural studies on the aqueous mixtures of pectin and nanoclay were able to discriminate the interactions, which control the adsorption of pectin onto the filler and the aggregation of both pectin and clay particles. The gained insights were useful to interpret the mesoscopic structure of the nanocomposites (prepared from the aqueous mixtures by means of the casting method) evidenced by SEM, thermal stability, tensile properties, and transparency investigations. The attained knowledge represents a basic point for designing new hybrid nanostructures in both the aqueous and the solid phase for specific purposes.

Halloysite clay nanotubes are functionalized by exploiting the different charges between the inner positive and the outer negative surfaces; accordingly, a selective adsorption\ud is pursued by employing anionic and cationic surfactants. The obtained hybrid materials dispersed in aqueous phase are studied from the physicochemical viewpoint to investigate the colloidal stability that is a crucial parameter for applications. It is demonstrated that the adsorption of anionic surfactant into the HNTs lumen increases the net negative charge of the nanotubes enhancing the electrostatic repulsions and consequently the dispersion stability. The solubilization capability of these functionalized nanotubes toward hydrophobic\ud compounds is demonstrated. This paper puts forward an easy strategy to prepare hybrid materials, like inorganic micelles, that can be used in water for solubilization and delivery of a hydrophobic compound by taking advantage of the sustainable and biocompatible properties

Pectin bionanocomposite films filled with various concentrations of two different types of halloysite nanotubes were prepared and characterized in this study as potential films for food packaging applications. The two types of halloysite nanotubes were long and thin (patch) (200-30 000 nm length) and short and stubby (Matauri Bay) (50-3000 nm length) with different morphological, physical, and dispersibility properties. Both matrix (pectin) and reinforcer (halloysite nanotubes) used in this study are considered as biocompatible, natural, and low-cost materials. Various characterization tests including Fourier transform infrared spectroscopy, field emission scanning electron microscopy, release kinetics, contact angle, and dynamic mechanical analysis were performed to evaluate the performance of the pectin films. Exceptional thermal, tensile, and contact angle properties have been achieved for films reinforced by patch halloysite nanotubes due to the patchy and lengthy nature of these tubes, which form a bird nest structure in the pectin matrix. Matauri Bay halloysite nanotubes were dispersed uniformly and individually in the matrix in low and even high halloysite nanotube concentrations. Furthermore, salicylic acid as a biocidal agent was encapsulated in the halloysite nanotubes lumen to control its release kinetics. On this basis, halloysite nanotubes/salicylic acid hybrids were dispersed into the pectin matrix to develop functional biofilms with antimicrobial properties that can be extended over time. Results revealed that shorter nanotubes (Matauri Bay) had better ability for the encapsulation of salicylic acid into their lumen, while patchy structure and longer tubes of patch halloysite nanotubes made the encapsulation process more difficult, as they might need more time and energy to be fully loaded by salicylic acid. Moreover, antimicrobial activity of the films against four different strains of Gram-positive and Gram-negative bacteria indicated the effective antimicrobial properties of pectin/halloysite functionalized films and their potential to be used for food packaging applications.

We prepared hybrid halloysite nanotubes (HNT/sodium alkanoates) in which the inner cavity of the nanoclay was selectively modified. Physicochemical studies evidenced the interactions between HNT and sodium alkanoates, ruled out clay exfoliation, quantified the amount of the loaded substance, and showed an increase of the total net negative charge, allowing us to obtain rather stable aqueous nanoclay dispersions. These dispersions were exploited as inorganic micelles to capture hydrocarbon and aromatic oils in the vapor and liquid states and were revealed to be nonfoaming but very efficient in encapsulating oils. Here, we have fabricated biocompatibile and low-cost inorganic micelles that can be exploited for industrial applications on a large scale.

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During drying, an aqueous suspension of strongly charged halloysite clay nanotubes concentrates at the edge of the droplet ("coffee-ring" effect) which provides alignment of the tubes along the liquid-substrate contact line. First, the surface charge of the nanotubes was enhanced by polyanion adsorption inside of the lumen to compensate for the internal positive charges. This increased the magnitude of the ξ-potential of the tubes from -36 to -81 mV and stabilized the colloids. Then, colloidal halloysite was dropped onto the substrate, dried at 65 °C and after a concentration of ∼0.05 mg mL(-1) was reached, the alignment of nanotubes occurred starting from the droplet edges. The process was described with Onsager's theory, in which longer nanorods, which have higher surface charge, give better ordering after a critical concentration is reached. This study indicates a new application of halloysite clay nanotubes in polymeric composites with anisotropic properties, microchannel orientation, and production of coatings with aligned nanotubes.

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