资源描述：
《Supramolecular regulation of bioorthogonal catalysis in cells》由会员上传分享，免费在线阅读，更多相关内容在学术论文-天天文库。
1、ARTICLESPUBLISHEDONLINE:23JUNE2015
2、DOI:10.1038/NCHEM.2284Supramolecularregulationofbioorthogonalcatalysisincellsusingnanoparticle-embeddedtransitionmetalcatalystsGulenYesilbagTonga†,YoungdoJeong†,BradleyDuncan,TsukasaMizuhara,RubulMout,RiddhaDas,SungTaeKim,Yi-CheunYeh,BoYan,Singy
3、ukHouandVincentM.Rotello*Bioorthogonalcatalysisbroadensthefunctionalpossibilitiesofintracellularchemistry.Effectivedeliveryandregulationofsyntheticcatalyticsystemsincellsarechallengingduetothecomplexintracellularenvironmentandcatalystinstability.Here,wereportthefabricationofprote
4、in-sizedbioorthogonalnanozymesthroughtheencapsulationofhydrophobictransitionmetalcatalystsintothemonolayerofwater-solublegoldnanoparticles.Theactivityofthesecatalystscanbereversiblycontrolledbybindingasupramolecularcucurbit[7]uril‘gate-keeper’ontothemonolayersurface,providingabio
5、mimeticcontrolmechanismthatmimicstheallostericregulationofenzymes.Thepotentialofthisgatednanozymeforuseinimagingandtherapeuticapplicationswasdemonstratedthroughtriggeredcleavageofallylcarbamatesforpro-fluorophoreactivationandpropargylgroupsforprodrugactivationinsidelivingcells.ioo
6、rthogonalchemistry1–3isapromisingstrategyfortheintra-usingcompetitiveguests38,restoringcatalyticactivity(Fig.1).Thecellulargenerationofmoleculesfortherapeutic4andimagingefficacyofthissystemwasdemonstratedinsolutionandincellsBapplications5,6unattainablethroughnaturallyoccurringbio-
7、throughtwoapplications:(1)thegatedgenerationofafluorophoreprocesses7,8.Transitionmetalcatalysts(TMCs)areexcellentcandi-throughdeallylationofanon-fluorescentprecursorand(2)thedatesforuseinbioorthogonalprocesses9–11,rapidlycatalysinggatedactivationofaprodrugbycleavingthepropargylfunc
8、tionalitytransformationsthatcannotbeperformedviaenzymaticpro-thathasbeenintroducedtoblocktheactivesideoftheoriginaldrug.cesses12–15.However,theapplicationofTMC-mediatedreactionsSuchgatedcontrolofcatalysishasnotbeendemonstratedincellstoinlivingcellsischallengingduetoissuesofbiocom
9、patibility,dateandisimportantbecauseital
