The aim of the research was to develop new temperature and pH responsive smart textile materials with simultaneous controlled porosity, moisture management and pro-active antimicrobial protection, provided by controlled release of antimicrobial substances and bio-barrier formation. Hydrogels based on poly-N(isopropylacrylamide) and chitosan with micro- (PNCS_M) and nano-size (PNCS_N) particles were synthesized using dispersion polymerisation. The particle size of PNCS hydrogels influenced their responsive properties. On the fibre surface, PNCS_M hydrogel showed better pro-active porosity and moisture management properties and greater temperature sensitivity, while PNCS_N hydrogel showed superior moisture release and greater pH responsiveness. The 30-second oxygen plasma treatment of fibres improved adsorption and distribution of the PNCS_N hydrogel on fibre surface, which improved the desired temperature and pH responsive properties of functionalised samples. In order to achieve the proactive antimicrobial activity, different antimicrobials, i.e. AgCl, colloidal silver and savory (Satureja montana) essential oil (EO) with the working mechanism based on controlled release, or 3-(trimethoxysilyl) propyl-dimethyltetecyl ammonium chloride (Si-QAC) and (3-aminopropyl) triethoxysilane (APTES) with the working mechanism based on the formation of a bio-barrier, were incorporated into the PNCS hydrogel particles. An excellent antimicrobial activity and temperature related controlled release of silver was achieved, although the presence of silver compounds repressed the temperature and pH-related moisture management of samples. For the embedment of the hydrophobic savory EO into hydrogel particles, PNCS hydrogel with incorporated β-cyclodextrins (PNCS/CD) was synthesized. The latter improved the temperature responsive properties of the hydrogel and allowed an increase in the chitosan concentration, which resulted in the synergistic antimicrobial activity provided by the bio-barrier formed by chitosan and a pro-active release of the savory EO. When combining PNCS hydrogel and Si-QAC or APTES, the application procedure, concentration and the chemical composition of polysyloxane matrix greatly influenced the responsive and protective properties, as well as the cytotoxicity of functionalised samples. The two-step application procedure, including the application of first PNCS_M hydrogel and then 0.5 % Si-QAC, ensured an excellent antimicrobial activity, although the sample showed high cytotoxicity. When Si-QAC was replaced with a 4% concentration of APTES, an excellent antimicrobial activity, noncytotoxicity and preserved responsiveness were obtained. The electrospinning procedure was used for the formation of composite PNCS_M hydrogel and PLA fibres with stimuli responsive properties and pro-active release of the ultraviolet (UV) dye.
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