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Dual stimuli-responsive polyurethane-based hydrogels as smart drug delivery carriers for the advanced treatment of chronic skin wounds

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Bioactive Materials 2021年第9期6卷 3013-3024页

作者： Rossella Laurano Monica Boffito Michela Abrami Mario Grassi alice zoso Valeria Chiono Gianluca Ciardelli Politecnico di Torino Mechanical and Aerospace Engineering DepartmentCorso Duca degli Abruzzi 2410129TorinoItaly Universitàdegli Studi di Trieste Department of Engineering and ArchitectureVia Alfonso Valerio 6/134127TriesteItaly

The design of multi-stimuli-responsive vehicles for the controlled and localized release of drugs is a challenging issue increasingly catching the attention of many research groups working on the advanced treatment of hard-to-close *** this work,a thermo-and pH-responsive hydrogel(P-CHP407)was prepared from an ad hoc synthesized amphiphilic poly(ether urethane)(CHP407)exposing a significant amount of-COOH groups(8.8±0.9 nmol/g_(polymer)).The exposure of acid moieties in P-CHP407 hydrogel led to slightly lower initial gelation temperature(12.1◦C vs.14.6◦C,respectively)and gelation rate than CHP407 hydrogel,as rheologically *** hydrogel characterization by Low Field NMR(LF-NMR)spectroscopy suggested that the presence of carboxylic groups in P-CHP407 caused the formation of bigger micelles with a thicker hydrated shell than CHP407 hydrogels,as further proved by Dynamic Light Scattering *** addition,P-CHP407 hydrogel showed improved capability to change its internal pH compared to CHP407 one when incubated with an alkaline buffer(pH 8)(e.g.,pH_(change_5min)=3.76 and 1.32,respectively).Moreover,LF-NMR characterization suggested a stronger alkaline-pH-induced interaction of water molecules with micelles exposing-COOH ***,the hydrogels were found biocompatible according to ISO 10993 and able to load and release Ibuprofen:delivery kinetics of Ibuprofen was enhanced by P-CHP407 hydrogels at alkaline pH,suggesting their potential use as smart delivery systems in the treatment of chronic infected wounds.

关键词： Stimuli-responsive hydrogel Drug delivery system pH-triggered release Advanced wound treatment Polyurethane hydrogel LF-NMR characterization

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Custom-design of intrinsically antimicrobial polyurethane hydrogels as multifunctional injectable delivery systems for mini-invasive wound treatment

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Engineered Regeneration 2021年第1期2卷 263-278页

作者： Rossella Laurano Valeria Chiono Chiara Ceresa Letizia Fracchia alice zoso Gianluca Ciardelli Monica Boffito Mechanical and Aerospace Engineering Department Politecnico di TorinoCorso Duca degli Abruzzi 24Torino 10129Italy Department of Pharmaceutical Sciences Universitadel Piemonte Orientale A.AvogadroLargo Guido Donegani 2Novara 28100Italy

Effective management of hard-to-close skin wounds is a challenging issue due to several co-morbidities in affected ***,infections represent a major obstacle in wound *** design of efficient wound treatments thus represents an urgent *** drug delivery hydrogels with intrinsic antimicrobial and antifungal properties were herein designed for perspective application in the mini-invasive treatment of hard-to-close ***,an amphiphilic polyurethane was synthesized from Poloxamer■407 macrodiol and N-Boc diethanolamine chain extender(DHP407,M_(w)=33 kDa).Chain-extension reaction step was optimized to maximize the formation of-NH groups along the polymer chains(4.5×10^(20)±1.8×10^(19)-NH groups/g polymer),after Boc-caging group removal(D-DHP407).DHP407 and D-DHP407 water-based solutions were thermosensitive with slightly different Critical Micellar Concentration(17.5μg/mL vs.19.7μg/mL)and cluster hydrodynamic diameter(235.6±19.9 nm vs.260.1±20.5 nm),and similar Critical Micellar Temperature(22.5℃ vs.23.1℃).A polyurethane solution concentration(15%w/V)was selected by tube-inverting test and rheological analysis showing injectability,as evidenced by sol-to-gel transition at 27.7±0.6℃ for DHP407 and 29.7±0.6℃ for D-DHP407,within few minutes,at similar gelation ***407 and D-DHP407 hydrogels showed controlled release of Bovine Serum Albumin(BSA)model protein(1 mg/mL),with no burst *** released from DHP407 and D-DHP407 hydrogels at 24 h was 33.7±5.0% and 24.6±1.2%,respectively.D-DHP407 hydrogel was biocompatible and able to support NIH-3T3 cell ***,D-DHP407 hydrogel showed intrinsic antifungal and antibacterial activity against *** and Gram-positive *** and Gram-negative *** bacteria,injectability and capability to retain shape post-injection,making it promising for future use in the management of hard-to-close skin wounds.

关键词： Antimicrobial poly(ether urethane)s Drug delivery systems Injectable formulations Antibiotic-free treatments Wound healing Thermosensitive hydrogels

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