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1、Articlepubs.acs.org/JACSCellProtective,ABCTriblockPolymer-BasedThermoresponsiveHydrogelswithROS-TriggeredDegradationandDrugRelease††††‡MukeshK.Gupta,JohnR.Martin,ThomasA.Werfel,TianweiShen,JonathanM.Page,,†andCraigL.Duvall*†BiomedicalEngineering,VanderbiltUniversity
2、,Nashville,Tennessee37235,UnitedStates‡ChemicalandBiomolecularEngineering,VanderbiltUniversity,Nashville,Tennessee37235,UnitedStates*SSupportingInformationABSTRACT:AcombinationofanionicandRAFTpolymerizationwasusedtosynthesizeanABCtriblockpolymerpoly-[(propylenesulfid
3、e)-block-(N,N-dimethylacrylamide)-block-(N-iso-propylacrylamide)](PPS-b-PDMA-b-PNIPAAM)thatformsphysi-callycross-linkedhydrogelswhentransitionedfromambienttophysiologictemperatureandthatincorporatesmechanismsforreactiveoxygenspecies(ROS)triggereddegradationanddrugre
4、lease.Atambienttemperature(25°C),PPS-b-PDMA-b-PNIPAAMassembledinto66±32nmmicellescomprisingahydrophobicPPScoreandPNIPAAMontheoutercorona.Uponheatingtophysiologictemperature(37°C),whichexceedsthelowercriticalsolutiontemperature(LCST)ofPNIPAAM,micellesolutions(at≥2.5w
5、t%)sharplytransitionedintostable,hydratedgels.Temperature-dependentrheologyindicatedthattheequilibriumstoragemoduli(G′)ofhydrogelsat2.5,5.0,and7.5wt%were20,380,and850Pa,respectively.ThePPS-b-PDMA-b-PNIPAAMmicelleswerepreloadedwiththemodeldrugNilered,andtheresultingh
6、ydrogelsdemonstratedROS-dependentdrugrelease.Likewise,exposuretotheperoxynitritegeneratorSIN-1degradedthemechanicalpropertiesofthehydrogels.Thehydrogelswerecytocompatibleinvitroandweredemonstratedtohaveutilityforcellencapsulationanddelivery.Thesehydrogelsalsopossess
7、edinherentcell-protectivepropertiesandreducedROS-mediatedcellulardeathinvitro.SubcutaneouslyinjectedPPS-b-PDMA-b-PNIPAAMpolymersolutionsformedstablehydrogelsthatsustainedlocalreleaseofthemodeldrugNileredfor14daysinvivo.Thesecollectivedatademonstratethepotentialuseof
8、PPS-b-PDMA-b-PNIPAAMasaninjectable,cyto-protectivehydrogelthatovercomesconventionalPNIPAAMhydrogellimitationssuchassyneresis,lackofdegrada
