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Conformational changes of the thermal transitions of chitosan- graft-poly( N-vinylcaprolactam) copolymers in aqueous solution were studied by varying of the length of the grafted poly( N-vinylcaprolactam) (PVCL) chains, as well as the ionic strength and the pH of the solution. The conformational properties of the copolymer were monitored by means of dynamic light scattering and ζ-potential measurements. A series of copolymers with defined molecular architecture were synthesized. Obtained results point out that hydrophobic hydration plays a crucial role on the solubility of this copolymer at neutral and slightly alkaline solutions. The evolution of the size of macromolecular aggregates indicates that, in the coil state, there is a monomodal distribution, passing through a bimodal distribution in the pre-transition region, just before the phase separation. The role of the charge of the copolymers on the cooperative transition is also analyzed. The phase transition of these amphiphilic copolymers shows a strong dependence on the ionic strength of the solution. [ABSTRACT FROM AUTHOR]

A series of thermoresponsive copolymers based on chitosan- g -poly( N -vinylcaprolactam) were synthesized by amidation reaction using 4-(4,6-dimethoxy-1,3,5-triazin-2-yl)-4-methylmorpholinium chloride as coupling reagent. The effect of molecular architecture on the thermoresponsive properties of the graft copolymers solutions was studied by varying the chain length of the grafted poly( N -vinylcaprolactam), PVCL, (in the range from 4 to 26 kDa) and the spacing between grafted chains onto the chitosan backbone. The most interesting characteristic of these copolymers is their solubility in water at temperatures below their lower critical solution temperature (LCST). These solutions presented a LCST between 36 and 44 °C, which decreases with the spacing and length of grafted PVCL chains onto the chitosan backbone, in contrast with the limited decrease of the LCST of PVCL above a critical M ¯ n value around 18 kDa. This behavior offers tangible possibilities for the preparation and application of sensitive bioactive formulations and “smart” drug delivery systems. [ABSTRACT FROM AUTHOR]