Gold Nanoparticle-Based Colorimetric and

Anal.Chem.2008,80,9021–9028

GoldNanoparticle-BasedColorimetricand

“Turn-On”FluorescentProbeforMercury(II)IonsinAqueousSolution

HaoWang,YongxiangWang,JianyuJin,andRonghuaYang*

BeijingNationalLaboratoryforMolecularSciences,CollegeofChemistryandMolecularEngineering,PekingUniversity,Beijing100871,China

Anapproachforvisualand uorescentsensingofHg2+inaqueoussolutionispresented.ThismethodisbasedontheHg2+-inducedconformationalchangeofathymine(T)-richsingle-strandedDNA(ssDNA)andthedifferenceinelectrostaticaf nitybetweenssDNAanddouble-stranded(dsDNA)withgoldnanoparticles.Thedye-taggedssDNAcontainingT-Tmismatchedsequenceswascho-senasHg2+acceptor.Athighionicstrength,introductionofthessDNAtoacolloidalsolutionoftheaggregatesofgoldnanoparticlesresultsincolorchange,fromblue-graytoredofthesolution,andthe uorescencequenchingofthedye.BindingofHg2+withthessDNAformsthedouble-strandedstructure.ThisformationofdsDNAreducesthecapabilitytostabilizebarenanoparticlesagainstsalt-inducedaggregation,remainingablue-grayinthecolorofthesolution,but uorescencesignalenhancementcomparedwiththatwithoutHg2+.Withtheoptimumconditionsdescribed,thesystemexhibitsadynamicresponserangeforHg2+from9.6×10-8to6.4×10-6Mwithadetectionlimitof4.0×10-8M.Boththecolorand uorescencechangesofthesystemareextremelyspeci cforHg2+eveninthepresenceofhighconcentrationsofotherheavyandtransitionmetalions,whichmeettheselectiverequirementsforbiomedicalandenvironmentalapplication.Thecombineddatafromtrans-missionelectronmicroscopy, uorescenceanisotropymeasurements,anddialysisexperimentsindicatethatboththecolorandthe uorescenceemissionchangesoftheDNA-functionedgoldnanoparticlesgeneratedbyHg2+aretheresultsofthemetal-inducedformationofdsDNAandsubsequentformationofnanoparticleaggregates.

Heavymetalionpollutionposessevererisksinhumanhealthandtheenvironment.Mercury(II)(Hg2+),widelydistributedintheair,water,andsoil,1isconsideredtobeahighlytoxicheavymetalionandisknownasahazardouspollutantwithrecognizedaccumulativecharacterintheenvironmentandbiota.2-4Mercuryvaporsandorganicmercuryderivatives,suchasmethylmercury,

*Towhomcorrespondenceshouldbeaddressed.E-mail:Yangrh@http://doc.guandang.net.Fax:+86-10-62751708.

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AnalyticalChemistry,Vol.80,No.23,December1,20089021

havebeendeveloped.Inaddition,nanosensorsbasedonmetalnanoparticles,27,28,32,33,36-40semiconductorquantumdots,41,42single-walledcarbonnanotubes,43andnanoscalemembrane44orchip45haveattractedinterestinrecentyears.AlthoughtheseapproacheshavemadegreatcontributionstowardaHg2+assay,limitations,suchasinsuf cientresolutioninwater,irreversibleHg2+complex,interferencewithotherheavymetalions,andsophisticatedsynthesisoftheprobematerials,stillexisted.Therefore,itshouldbedesirabletodevelopanewmethodtosolvetheseprobl …… 此处隐藏：37846字，全部文档内容请下载后查看。喜欢就下载吧 ……