Oblikovanje pametnih tekstilij z uporabo temperaturno in pH odzivnega hidrogela kot nosilca protimikrobnih učinkovin

Štular, Danaja (author), Tomšič, Brigita (mentor), Jerman, Ivan (comentor)

Namen raziskave je bil razvoj novih temperaturno in pH-odzivnih pametnih tekstilij s sočasno nadzorovano poroznostjo in uravnavanjem vlage ter proaktivno protimikrobno zaščito, zagotovljeno preko nadzorovanega sproščanja protimikrobnih učinkovin in oblikovanja biobariere. Z uporabo disperzijske polimerizacije je bil sintetiziran hidrogel na podlagi poli(N-izopropilakrilamida) in hitozana (PNCS) v mikro (PNCS_M) in nano velikostnem (PNCS_N) razredu. Velikost delcev hidrogela PNCS je vplivala na njegove odzivne lastnosti. Hidrogel PNCS_M je izkazal boljšo proaktivno poroznost in uravnavanje vlage ter večjo občutljivost na spremembe temperature, hidrogel PNCS_N pa je ob superiornem izločanju vlage izkazal intenzivnejšo odzivnost na spremembo pH. Obdelava vlaken s 30-sekundno kisikovo plazmo je izboljšala navzemanje in razporeditev hidrogela PNCS_N na vlaknih ter s tem izboljšanje želenih temperaturno in pH-odzivnih lastnosti funkcionaliziranih vzorcev. Za dosego proaktivnega protimikrobnega delovanja so bila v delce hidrogela PNCS_M vstavljena različna protimikrobna sredstva, tj. AgCl, koloidno srebro in eterično olje (EO) šetraja (Satureja montana), ki delujejo po principu nadzorovanega sproščanja, ter 3-(trimetoksisilil) propildimetiloktadecil amonijev klorid (Si-QAC) in (3-aminopropil)trietoksisilan (APTES), ki delujeta po principu oblikovanja biobariere. Pri tem je bilo doseženo odlično protimikrobno delovanje ter temperaturno pogojeno nadzorovano sproščanje srebra, čeprav je slednje nekoliko poslabšalo sposobnost proaktivnega uravnavanja vlage vzorcev ob spremembah temperature in pH. Za vstavitev hidrofobnega EO šetraja v delce hidrogela na vlaknih je bil sintetiziran hidrogel PNCS z vključenim β-ciklodekstrinom (PNCS/CD). Slednji je izboljšal temperaturno odzivnost hidrogela ter s tem omogočil povišanje koncentracije hitozana v strukturi hidrogela. To je zagotovilo sinergistično protimikrobno delovanje med biobariero hitozana in proaktivnim sproščanjem EO šetraja. V primeru kombinacije hidrogela PNCS_M ter Si-QAC in APTES so postopek nanosa, koncentracija in kemijska struktura polisiloksanskih matric pomembno vplivali na odzivne in zaščitne lastnosti ter citotoksičnost funkcionaliziranih vzorcev. Dvostopenjski postopek nanosa, ki je vključeval najprej nanos hidrogela PNCS_M z naknadnim nanosom 0,5-odstotnega Si-QAC, je zagotovil odlično protimikrobno aktivnost funkcionaliziranega vzorca, a je ta izkazal močno citotoksičnost. Ob zamenjavi Si-QAC s 4-odstotno koncentracijo APTES je bila dosežena odlična protimikrobnost, necitotoksičnost in ohranjene odzivne lastnosti. Med postopkom elektropredenja je bil hidrogel PNCS_M vstavljen v vlakna PLA, kar je zagotovilo izdelavo vlaknatih kompozitov z odzivnimi lastnostmi in proaktivnim sproščanjem ultravijoličnega (UV) barvila.

• Language: Slovenian
• Keywords: pametne tekstilije, kemijska modifikacija, odzivni hidrogel poli(N-izopropilakrilamid)/hitozan, uravnavanje vlage, nadzorovana poroznost, protimikrobna aktivnost, biobariera, nadzorovano sproščanje
• Work type: Doctoral dissertation
• Organization: NTF - Faculty of Natural Sciences and Engineering
• Year: 2019
• PID: 20.500.12556/RUL-111497
• Publication date in RUL: 02.10.2019

Secondary language

• Language: English
• Title: Tailoring of smart textiles using temparature and pH responsive hydrogel as a carrier of antimicrobial substances

Abstract

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.

• Keywords: smart textiles, chemical modification, poly(N-isopropylacrylamide)/chitosan stimuli responsive hydrogel, moisture management, controlled porosity, antimicrobial activity, bio-barrier, controlled release