Synthesis of Silver Nanoparticles - Chemical, Physical and Biological Methods

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Synthesisofsilvernanoparticles:chemical,physicalandbiologicalmethods
ResPharmSci.2014NovDec9(6):385406.
PMCID:PMC4326978
S.Iravani, 1,*H.Korbekandi, 2S.V.Mirmohammadi, 3andB.Zolfaghari1
1
DepartmentofPharmacognosyandIsfahanPharmaceuticalSciencesResearchCenter,SchoolofPharmacyandPharmaceuticalSciences,
IsfahanUniversityofMedicalSciences,Isfahan,I.R.Iran
2
DepartmentofGenetics&MolecularBiology,SchoolofMedicine,IsfahanUniversityofMedicalSciences,Isfahan,I.R.Iran
3
SchoolofPharmacyandPharmaceuticalSciences,IsfahanUniversityofMedicalSciences,Isfahan,I.R.Iran
*
Correspondingauthor:S.IravaniTel.00989132651091,Fax.00983116251011Email:siavashira@gmail.com
Received2013AugAccepted2013Oct.
Copyright:ResearchinPharmaceuticalSciences
ThisisanopenaccessarticledistributedunderthetermsoftheCreativeCommonsAttributionNoncommercialShareAlike3.0Unported,which
permitsunrestricteduse,distribution,andreproductioninanymedium,providedtheoriginalworkisproperlycited.
Abstract
Silvernanoparticles(NPs)havebeenthesubjectsofresearchersbecauseoftheiruniqueproperties(e.g.,size
andshapedependingoptical,antimicrobial,andelectricalproperties).Avarietyofpreparationtechniques
havebeenreportedforthesynthesisofsilverNPsnotableexamplesinclude,laserablation,gamma
irradiation,electronirradiation,chemicalreduction,photochemicalmethods,microwaveprocessing,and
biologicalsyntheticmethods.Thisreviewpresentsanoverviewofsilvernanoparticlepreparationby
physical,chemical,andbiologicalsynthesis.Theaimofthisreviewarticleis,therefore,toreflectonthe
currentstateandfutureprospects,especiallythepotentialsandlimitationsoftheabovementionedtechniques
forindustries.
Keywords:Nanoparticlesynthesis,Silvernanoparticles,Physicalsynthesis,Chemicalsynthesis,Biological
synthesis
INTRODUCTION
Nanotechnologyisanimportantfieldofmodernresearchdealingwithdesign,synthesis,andmanipulationof
particlestructuresrangingfromapproximately1100nm.Nanoparticles(NPs)havewiderangeof
applicationsinareassuchashealthcare,cosmetics,foodandfeed,environmentalhealth,mechanics,optics,
biomedicalsciences,chemicalindustries,electronics,spaceindustries,druggenedelivery,energyscience,
optoelectronics,catalysis,singleelectrontransistors,lightemitters,nonlinearopticaldevices,andphoto
electrochemicalapplications(1,2,3,4,5,6).
Nanobiotechnologyisarapidlygrowingscientificfieldofproducingandconstructingdevices.Animportant
areaofresearchinnanobiotechnologyisthesynthesisofNPswithdifferentchemicalcompositions,sizes
andmorphologies,andcontrolleddispersities.Nanobiotechnologyhasturnedupasanelementarydivisionof
contemporarynanotechnologyanduntiednovelepochinthefieldsofmaterialsciencereceivingglobal
attentionduetoitsampleapplications.Itisamultidisciplinaryapproachresultingfromtheinvestigationaluse
ofNPsinbiologicalsystemsincludingthedisciplinesofbiology,biochemistry,chemistry,engineering,
physicsandmedicine.Moreover,thenanobiotechnologyalsoservesasanimperativetechniqueinthe
developmentofclean,nontoxic,andecofriendlyproceduresforthesynthesisandcongregationofmetal
NPshavingtheintrinsicabilitytoreducemetalsbyspecificmetabolicpathways(1,2,3,4,5,6).
Nowadays,thereisagrowingneedtodevelopecofriendlyprocesses,whichdonotusetoxicchemicalsin
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4326978/?report=printable
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thesynthesisprotocols.Greensynthesisapproachesincludemixedvalencepolyoxometalates,
polysaccharides,Tollens,biological,andirradiationmethodwhichhaveadvantagesoverconventional
methodsinvolvingchemicalagentsassociatedwithenvironmentaltoxicity.Selectionofsolventmediumand
selectionofecofriendlynontoxicreducingandstabilizingagentsarethemostimportantissueswhichmust
beconsideredingreensynthesisofNPs.
SilverNPsareofinterestbecauseoftheuniquepropertieswhichcanbeincorporatedintoantimicrobial
applications,biosensormaterials,compositefibers,cryogenicsuperconductingmaterials,cosmeticproducts,
andelectroniccomponents.SomeimportantapplicationsofsilverNPsinpharmaceutics,medicine,and
dentistryareshowninTable1.Severalphysicalandchemicalmethodshavebeenusedforsynthesizingand
stabilizingsilverNPs(Table2)(7,8).
Themostpopularchemicalapproaches,includingchemicalreductionusingavarietyoforganicand
inorganicreducingagents,electrochemicaltechniques,physicochemicalreduction,andradiolysisarewidely
usedforthesynthesisofsilverNPs.Mostofthesemethodsarestillindevelopmentstageandthe
experiencedproblemsarethestabilityandaggregationofNPs,controlofcrystalgrowth,morphology,size
andsizedistribution.Furthermore,extractionandpurificationofproducedNPsforfurtherapplicationsare
stillimportantissues(9,10,11).
Thisreviewarticlepresentsanoverviewofsilvernanoparticlepreparationbyphysical,chemical,andgreen
synthesisapproaches.
SynthesisofsilverNPs
Physicalmethods Evaporationcondensationandlaserablationarethemostimportantphysicalapproaches.
TheabsenceofsolventcontaminationinthepreparedthinfilmsandtheuniformityofNPsdistributionare
theadvantagesofphysicalsynthesismethodsincomparisonwithchemicalprocesses.Physicalsynthesisof
silverNPsusingatubefurnaceatatmosphericpressurehassomedisadvantages,forexample,tubefurnace
occupiesalargespace,consumesagreatamountofenergywhileraisingtheenvironmentaltemperature
aroundthesourcematerial,andrequiresalotoftimetoachievethermalstability.Moreover,atypicaltube
furnacerequirespowerconsumptionofmorethanseveralkilowattsandapreheatingtimeofseveraltensof
minutestoreachastableoperatingtemperature(12,13).ItwasdemonstratedthatsilverNPscouldbe
synthesizedviaasmallceramicheaterwithalocalheatingarea(14).Thesmallceramicheaterwasusedto
evaporatesourcematerials.Theevaporatedvaporcancoolatasuitablerapidrate,becausethetemperature
gradientinthevicinityoftheheatersurfaceisverysteepincomparisonwiththatofatubefurnace.
ThismakespossibletheformationofsmallNPsinhighconcentration.Theparticlegenerationisverystable,
becausethetemperatureoftheheatersurfacedoesnotfluctuatewithtime.Thisphysicalmethodcanbe
usefulasananoparticlegeneratorforlongtermexperimentsforinhalationtoxicitystudies,andasa
calibrationdevicefornanoparticlemeasurementequipment(14).Theresultsshowedthatthegeometricmean
diameter,thegeometricstandarddeviationandthetotalnumberconcentrationofNPsincreasewithheater
surfacetemperature.SphericalNPswithoutagglomerationwereobserved,evenathighconcentrationwith
highheatersurfacetemperature.Thegeometricmeandiameterandthegeometricstandarddeviationofsilver
NPswereintherangeof6.221.5nmand1.231.88nm,respectively.
SilverNPscouldbesynthesizedbylaserablationofmetallicbulkmaterialsinsolution(15,16,17,18,19).The
ablationefficiencyandthecharacteristicsofproducednanosilverparticlesdependuponmanyparameters,
includingthewavelengthofthelaserimpingingthemetallictarget,thedurationofthelaserpulses(inthe
femto,picoandnanosecondregime),thelaserfluence,theablationtimedurationandtheeffectiveliquid
medium,withorwithoutthepresenceofsurfactants(20,21,22,23).
Oneimportantadvantageoflaserablationtechniquecomparedtoothermethodsforproductionofmetal
colloidsistheabsenceofchemicalreagentsinsolutions.Therefore,pureanduncontaminatedmetalcolloids
forfurtherapplicationscanbepreparedbythistechnique(24).Silvernanospheroids(2050nm)were
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preparedbylaserablationinwaterwithfemtosecondlaserpulsesat800nm(25).Theformationefficiency
andthesizeofcolloidalparticleswerecomparedwiththoseofcolloidalparticlespreparedbynanosecond
laserpulses.Asaresult,theformationefficiencyforfemtosecondpulseswassignificantlylowerthanthatfor
nanosecondpulses.Thesizeofcolloidspreparedbyfemtosecondpulseswerelessdispersedthanthatof
colloidspreparedbynanosecondpulses.Furthermore,itwasfoundthattheablationefficiencyfor
femtosecondablationinwaterwaslowerthanthatinair,whileinthecaseofnanosecondpulses,theablation
efficiencywassimilarinbothwaterandair.
Tienandcoworkers(26)usedthearcdischargemethodtofabricatesilverNPssuspensionindeionizedwater
withnoaddedsurfactants.Inthissynthesis,silverwires(Gredmann,99.99%,1mmindiameter)were
submergedindeionizedwaterandusedaselectrodes.Withasilverrodconsumptionrateof100mg/min,
yieldingmetallicsilverNPsof10nminsize,andionicsilverobtainedatconcentrationsofapproximately11
ppmand19ppm,respectively.Siegelandcolleagues(27)demonstratedthesynthesisofsilverNPsbydirect
metalsputteringintotheliquidmedium.Themethod,combiningphysicaldepositionofmetalintopropane
1,2,3triol(glycerol),providesaninterestingalternativetotimeconsuming,wetbasedchemicalsynthesis
techniques.SilverNPspossessroundshapewithaveragediameterofabout3.5nmwithstandarddeviation
2.4nm.ItwasobservedthattheNPssizedistributionanduniformparticledispersionremainsunchangedfor
dilutedaqueoussolutionsuptoglyceroltowaterratio1:20.
Chemicalmethods Chemicalreduction
ThemostcommonapproachforsynthesisofsilverNPsischemicalreductionbyorganicandinorganic
reducingagents.Ingeneral,differentreducingagentssuchassodiumcitrate,ascorbate,sodiumborohydride
(NaBH4),elementalhydrogen,polyolprocess,Tollensreagent,N,Ndimethylformamide(DMF),andpoly
(ethyleneglycol)blockcopolymersareusedforreductionofsilverions(Ag+)inaqueousornonaqueous
solutions.ThesereducingagentsreduceAg+andleadtotheformationofmetallicsilver(Ag0),whichis
followedbyagglomerationintooligomericclusters.Theseclusterseventuallyleadtotheformationof
metalliccolloidalsilverparticles(28,29,30).ItisimportanttouseprotectiveagentstostabilizedispersiveNPs
duringthecourseofmetalnanoparticlepreparation,andprotecttheNPsthatcanbeabsorbedonorbindonto
nanoparticlesurfaces,avoidingtheiragglomeration(31).Thepresenceofsurfactantscomprising
functionalities(e.g.,thiols,amines,acids,andalcohols)forinteractionswithparticlesurfacescanstabilize
particlegrowth,andprotectparticlesfromsedimentation,agglomeration,orlosingtheirsurfaceproperties.
Polymericcompoundssuchaspoly(vinylalcohol),poly(vinylpyrrolidone),poly(ethyleneglycol),poly
(methacrylicacid),andpolymethylmethacrylatehavebeenreportedtobetheeffectiveprotectiveagentsto
stabilizeNPs.Inonestudy,Oliveiraandcoworkers(31)prepareddodecanethiolcappedsilverNPs,
accordingtoBrustprocedure(32)basedonaphasetransferofanAu3+complexfromaqueoustoorganic
phaseinatwophaseliquidliquidsystem,whichwasfollowedbyareductionwithsodiumborohydridein
thepresenceofdodecanethiolasstabilizingagent,bindingontotheNPssurfaces,avoidingtheiraggregation
andmakingthemsolubleincertainsolvents.Theyreportedthatsmallchangesinsyntheticfactorsleadto
dramaticmodificationsinnanoparticlestructure,averagesize,sizedistributionwidth,stabilityandself
assemblypatterns.Kimandcolleagues(33)reportedsynthesisofsphericalsilverNPswithacontrollablesize
andhighmonodispersityusingthepolyolprocessandamodifiedprecursorinjectiontechnique.Inthe
precursorinjectionmethod,theinjectionrateandreactiontemperaturewereimportantfactorsforproducing
uniformsizedsilverNPswithareducedsize.
SilverNPswithasizeof172nmwereobtainedataninjectionrateof2.5ml/sandareactiontemperature
of100C.Theinjectionoftheprecursorsolutionintoahotsolutionisaneffectivemeanstoinducerapid
nucleationinashortperiodoftime,ensuringthefabricationofsilverNPswithasmallersizeandanarrower
sizedistribution.Zhangandcoworkers(34)usedahyperbranchedpoly(methylenebisacrylamide
aminoethylpiperazine)withterminaldimethylaminegroups(HPAMAMN(CH3)2)toproducecolloidsof
silver.Theamidemoieties,piperazinerings,tertiaryaminegroupsandthehyperbranchedstructurein
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HPAMAMN(CH3)2areimportanttoitseffectivestabilizingandreducingabilities.Chenandcolleagues
(35)haveshowntheformationofmonodispersedsilverNPsusingsimpleoleylamineliquidparaffinsystem.
ItwasreportedthattheformationprocessoftheseNPscouldbedividedintothreestages:growth,incubation
andOatwaldripeningstages.Thehigherboilingpointof300Cofparaffinaffordsabroaderrangeof
reactiontemperatureandmakesitpossibletoeffectivelycontrolthesizeofsilverNPsbyvaryingtheheating
temperaturealonewithoutchangingthesolvent.Moreover,thesizeofthecolloidalsilverNPscouldbe
regulatednotonlybychangingtheheatingtemperature,ortheripeningtime,butalsobyadjustingtheratio
ofoleylaminetothesilverprecursor.
SilverNPscanbepreparedatroomtemperature,bysimplemixingofthecorrespondingmetalionswith
reducedpolyoxometalateswhichservesasreducingandstabilizingagents.Polyoxometalatesaresolublein
waterandhavethecapabilityofundergoingstepwise,multielectronredoxreactionswithoutdisturbingtheir
structure.ItwasdemonstratedthatsilverNPswereproducedbyilluminatingadeaeratedsolutionof
polyoxometalate/S/Ag+(36).Furthermore,greenchemistrytypeonestepsynthesisandstabilizationofsilver
nanostructureswithMoVMoVI mixedvalencepolyoxometalatesinwateratroomtemperaturehasbeen
reported(37).
Microemulsiontechniques
UniformandsizecontrollablesilverNPscanbesynthesizedusingmicroemulsiontechniques.TheNPs
preparationintwophaseaqueousorganicsystemsisbasedontheinitialspatialseparationofreactants(metal
precursorandreducingagent)intwoimmisciblephases.Theinterfacebetweenthetwoliquidsandthe
intensityofinterphasetransportbetweentwophases,whichismediatedbyaquaternaryalkylammonium
salt,affecttherateofinteractionsbetweenmetalprecursorsandreducingagents.Metalclustersformedatthe
interfacearestabilized,duetotheirsurfacebeingcoatedwithstabilizermoleculesoccurringinthenonpolar
aqueousmedium,andtransferredtotheorganicmediumbytheinterphasetransporter(38).Oneofthemajor
disadvantagesistheuseofhighlydeleteriousorganicsolvents.
Thuslargeamountsofsurfactantandorganicsolventmustbeseparatedandremovedfromthefinalproduct.
Forinstance,Zhangandcoworkers(39)useddodecaneasoilyphase(alowdeleteriousandevennontoxic
solvent),buttherewasnoneedtoseparatethepreparedsilversolutionfromthereactionmixture.Onthe
otherhand,colloidalNPspreparedinnonaqueousmediaforconductiveinksarewelldispersedinalow
vaporpressureorganicsolvent,toreadilywetthesurfaceofpolymericsubstratewithoutanyaggregation.
TheadvantagescanalsobefoundintheapplicationsofmetalNPsascatalyststocatalyzemostorganic
reactions,whichhavebeenconductedinnonpolarsolvents.ItisveryimportanttotransfermetalNPsto
differentphysicochemicalenvironmentsinpracticalapplications(40).
UVinitiatedphotoreduction
Asimpleandeffectivemethod,UVinitiatedphotoreduction,hasbeenreportedforsynthesisofsilverNPsin
thepresenceofcitrate,polyvinylpyrrolidone,poly(acrylicacid),andcollagen.Forinstance,Huangand
YangproducedsilverNPsviaphotoreductionofsilvernitrateinlayeredinorganiclaponiteclaysuspensions
whichservedasstabilizingagentforpreventionofNPsaggregation.ThepropertiesofproducedNPswere
studiedasafunctionofUVirradiationtime.BimodalsizedistributionandrelativelylargesilverNPswere
obtainedwhenirradiatedunderUVfor3h.FurtherirradiationdisintegratedthesilverNPsintosmallersizes
withasingledistributionmodeuntilarelativelystablesizeandsizedistributionwasobtained(41).Silver
NPs(nanosphere,nanowire,anddendrite)havebeenpreparedbyUVirradiationphotoreductiontechnique
atroomtemperatureusingpoly(vinylalcohol)(asprotectingandstabilizingagent).Concentrationofboth
poly(vinylalcohol)andsilvernitrateplayedsignificantroleinthegrowthofthenanorodsanddendrites(42).
Sonoelectrochemistrytechniqueutilizestheultrasonicpowerprimarilytomanipulatethematerial
mechanically.Pulsedsonoelectrochemicalsyntheticmethodinvolvesalternatingsonicandelectricpulses,
andelectrolytecompositionplaysacrucialroleinshapeformation(43).Itwasreportedthatsilver
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nanospherescouldbepreparedbysonoelectrochemicalreductionusingacomplexingagent,nitrilotriacetate
toavoidaggregation(43).
Photoinducedreduction
SilverNPscanbesynthesizedbyusingavarietyofphotoinducedorphotocatalyticreductionmethods.
Photochemicalsynthesisisacleanprocesswhichhashighspatialresolution,convenienceofuse,andgreat
versatility.Moreover,photochemicalsynthesisenablesonetofabricatetheNPsinvariousmediumsincluding
cells,emulsion,polymerfilms,surfactantmicelles,glasses,etc.Nanosizedsilverparticleswithanaverage
sizeof8nmwerepreparedbyphotoinducedreductionusingpoly(styrenesulfonate)/poly(allylamine
hydrochloride)polyelectrolytecapsulesasmicroreactors(44).Moreover,itwasdemonstratedthat
photoinducedmethodcouldbeusedforconvertingsilvernanospheresintotriangularsilvernanocrystals
(nanoprisms)withdesirededgelengthsin30120nmrange(45).Particlegrowthprocesswascontrolled
usingdualbeamilluminationofNPs.Citrateandpoly(styrenesulfonate)wereusedasstabilizingagents.In
anotherstudy,silverNPswerepreparedthroughaveryfastreductionofAg+byaminoalkylradicals
generatedfromhydrogenabstractiontowardanaliphaticaminebytheexcitedtripletstateof2substituted
thioxanthoneseries(TXOCH2COOandTXSCH2COO).Quantumyieldofthispriorreactionwas
tunedbysubstituenteffectonthioxanthones,andledtoakineticcontrolofconversionofsilverion(Ag+)to
silvermetal(Ag0)(46).
ThedirectphotoreductionprocessofAgNO3inthepresenceofsodiumcitrate(NaCit)wascarriedoutwith
differentlightsources(UV,white,blue,cyan,greenandorange)atroomtemperature.SatoBerrand
coworkers(47)haveshownthatthislightmodificationprocessresultsinacolloidwithdistinctiveoptical
propertieswhichcanberelatedtothesizeandshapeoftheparticles.Moreover,Ghoshandcolleagues(48)
reportedasimpleandreproducibleUVphotoactivationmethodforthepreparationofstablesilverNPsin
aqueousTritonX100(TX100).TheTX100moleculesactasreducingagentandalsoasNPsstabilizer
throughtemplate/cappingaction.
Furthermore,surfactantsolutionhelpstocarryouttheprocessofNPsgrowthinthediffusioncontrolledway
bydecreasingthediffusionormasstransfercoefficientofthesystem.ItalsohelpstoimprovetheNPssize
distributionsbyincreasingthesurfacetensionatthesolventNPsinterface.Huangandcoworkers(49)
reportedthesynthesisofsilverNPsinanalkalineaqueoussolutionofAgNO3/carboxymethylatedchitosan
(CMCTS)usingUVlightirradiation.CMCTS,awatersolubleandbiocompatiblechitosanderivative,
servedsimultaneouslyasareducingagentforsilvercationandastabilizingagentforthesilverNPs.The
diameterrangeofproducedsilverNPswas28nm,andtheycanbedispersedstablyinthealkalineCMCTS
solutionformorethan6months.
Electrochemicalsyntheticmethod
ElectrochemicalsyntheticmethodcanbeusedtosynthesizesilverNPs.Itispossibletocontrolparticlesize
byadjustingelectrolysisparametersandtoimprovehomogeneityofsilverNPsbychangingthecomposition
ofelectrolyticsolutions.Polyphenylpyrrolecoatedsilvernanospheroids(320nm)weresynthesizedby
electrochemicalreductionattheliquid/liquidinterface.Thisnanocompoundwaspreparedbytransferring
thesilvermetalionfromaqueousphasetoorganicphase,whereitreactedwithpyrrolemonomer(50).In
anotherstudy,monodispersesilvernanospheroids(118nm)weresynthesizedbyelectrochemicalreduction
insideoroutsidezeolitecrystalsaccordingtosilverexchangedegreeofcompactzeolitefilmmodified
electrodes(51).Furthermore,sphericalsilverNPs(1020nm)withnarrowsizedistributionswere
convenientlysynthesizedinaqueoussolutionbyanelectrochemicalmethod(52).PolyNvinylpyrrolidone
waschosenasthestabilizerforthesilverclustersinthisstudy.PolyNvinylpyrrolidoneprotectsNPsfrom
agglomeration,significantlyreducessilverdepositionrate,andpromotessilvernucleationandsilverparticle
formationrate.Applicationofrotatingplatinumcathodeeffectivelysolvesthetechnologicaldifficultyof
rapidlytransferringmetallicNPsfromcathodevicinitytobulksolution,avoidingtheoccurrenceof
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flocculatesinvicinityofcathode,andensuresmonodispersityofparticles.Additionofsodiumdodecyl
benzenesulfonatetotheelectrolyteimprovedparticlesizeandparticlesizedistributionofsilverNPs(52).
Irradiationmethods
SilverNPscanbesynthesizedbyusingavarietyofirradiationmethods.Laserirradiationofanaqueous
solutionofsilversaltandsurfactantcanproducesilverNPswithawelldefinedshapeandsizedistribution
(53).Furthermore,laserwasusedinaphotosensitizationsyntheticmethodofmakingsilverNPsusing
benzophenone.Atshortirradiationtimes,lowlaserpowersproducedsilverNPsofabout20nm,whilean
increasedirradiationpowerproducedNPsofabout5nm.Laserandmercurylampcanbeusedaslight
sourcesforproductionofsilverNPs(54).Invisiblelightirradiationstudies,photosensitizedgrowthofsilver
NPsusingthiophene(sensitizingdye)andsilvernanoparticleformationbyilluminationofAg(NH3)+in
ethanolhasbeendone(55,56).
Microwaveassistedsynthesis
MicrowaveassistedsynthesisisapromisingmethodforsynthesisofsilverNPs.Microwaveheatingisbetter
thanaconventionaloilbathwhenitcomestoconsistentlyyieldingnanostructureswithsmallersizes,
narrowersizedistributions,andahigherdegreeofcrystallization(57).Microwaveheatinghasshorter
reactiontimes,reducedenergyconsumption,andbetterproductyieldswhichpreventstheagglomerationof
theparticlesformed(57).Moreover,otherthantheeliminationoftheoilbath,microwaveassistedsynthesis,
inconjunctionwithbenignreactionmedia,canalsodrasticallyreducechemicalwastesandreactiontimesin
severalorganicsynthesesandchemicaltransformations(58).
ItwasreportedthatsilverNPscouldbesynthesizedbymicrowaveassistedsynthesismethodemploying
carboxymethylcellulosesodiumasreducingandstabilizingagent.Thesizewasdependedonconcentration
ofsodiumcarboxymethylcelluloseandsilvernitrate.TheproducedNPswereuniformandstable,andwere
stableatroomtemperaturefor2monthswithoutanyvisiblechanges(59).ProductionofsilverNPsinthe
presenceofPtseeds,polyvinylpyrrolidineandethyleneglycolwasalsoreported(60).
Furthermore,starchhasbeenemployedasatemplateandreducingagentforsynthesisofsilverNPswithan
averagesizeof12nm,usingmicrowaveassistedsyntheticmethod.Starchfunctionsasatemplate,
preventingtheaggregationofproducedsilverNPs(61).Microwavesincombinationwithpolyolprocess
wereappliedforsynthesisofsilvernanospheroidsusingethyleneglycolandpolyNvinylpyrrolidoneas
reducingandstabilizingagents,respectively(62).Inatypicalpolyolprocessinorganicsaltisreducedbythe
polyol(e.g.,ethyleneglycolwhichservesasbothsolventandreducingagent)atahightemperature.Yinand
coworkers(63)reportedthatlargescaleandsizecontrolledsilverNPscouldberapidlysynthesizedunder
microwaveirradiationfromanaqueoussolutionofsilvernitrateandtrisodiumcitrateinthepresenceof
formaldehydeasareducingagent.SizeandsizedistributionofproducedsilverNPsarestronglydependent
onthestatesofsilvercationsintheinitialreactionsolution.SilverNPswithdifferentshapescanbe
synthesizedbymicrowaveirradiationofasilvernitrateethyleneglycolH2[PtCl6]poly(vinylpyrrolidone)
solutionwithin3min(64).Moreover,theuseofmicrowaveirradiationtoproducemonodispersedsilverNPs
usingbasicaminoacids(asreducingagents)andsolublestarch(protectingagent)hasbeenreported(65).
Radiolysisofsilverionsinethyleneglycol,inordertosynthesizesilverNPs,wasalsoreported(66).
Moreover,silverNPssupportedonsilicaaerogelwereproducedusinggammaradiolysis.Theproduced
silverclusterswerestablein29pHrangeandstartedagglomerationatpH>9(67).Oligochitosanasa
stabilizercanbeusedinpreparationofsilverNPsbygammaradiation.ItwasreportedthatstablesilverNPs
(515nm)weresynthesizedina1.89.0pHrangebythismethod(68).SilverNPs(45nm)werealso
synthesizedbyrayirradiationofaceticwatersolutionscontainingsilvernitrateandchitosan(69).
Silvernanospheroids(14nm)havebeenproducedbyrayirradiationofsilversolutioninoptically
transparentinorganicmesoporoussilica.Reductionofsilverionswithinthematrixisbroughtaboutby
hydratedelectronsandhydroalkylradicalsgeneratedduringradiolysisof2propanolsolution.Theproduced
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NPswithinthesilicamatrixwerestableinthepresenceofoxygenforatleastseveralmonths(70).Moreover,
silverNPshavebeenproducedbyirradiatingasolution,preparedbymixingsilvernitrateandpolyvinyl
alcohol,with6MeVelectrons(71).Pulseradiolysistechniquehasbeenappliedtostudyreactionsof
inorganicandorganicspeciesinsilvernanoparticlesynthesis,tounderstandthefactorscontrollingtheshape
andsizeoftheNPssynthesizedbyacommonreductionmethodusingcitrateions(asreducingand
stabilizingagents)(72),andtodemonstratetheroleofphenolderivativesinformationofsilverNPsbythe
reductionofsilverionswithdihydroxybenzene(73).Dihydroxybenzenecouldbeusedtoreducesilverions
tosynthesizestablesilverNPs(withanaveragesizeof30nm)inairsaturatedaqueoussolutions(73).
Silver,gold,platinum,andgoldpalladiumnanostructureshavebeenpreparedusingmicrowaveassisted
syntheticapproach.MorphologiesandsizesofNPscanbecontrolledbyalteringsomeexperimental
parameterssuchastheconcentrationofmetallicprecursors,surfactantpolymers,solvents,andtemperature.
Moreover,monodispersesilverNPscanbesynthesizedinlargequantitiesusingmicrowaveassisted
chemistrymethodinanaqueoussystem.Inthismethod,aminoacidsactasreducingagentsandsoluble
starchactsasaprotectingagent.
Notonlysilver,butsilverdopedlanthanumchromitescanalsobesynthesizedwithmicrowaveenergy(74).
MicrowaveenergyandthermalreductioncanbecoupledtosynthesizesilverNPsthatcanbedepositedon
oxidizedcarbonpaperelectrodes.ThesilverNPsthataresynthesizedthroughthismethodmaintaina
uniformsizebetweenparticlesandarewelldispersedoverthecarbonpapersubstrate.Themicrowave
assistedsynthesisofsilverNPsismadepossiblebydepositingthesilvercatalystsoncarbonpaperelectrodes.
Thismethodcanpotentiallybeusedinalkalinefuelcellsbecausethesynthesisoccursquickly,thereishigh
activity,andtheprocessisverysimple(75).
Nanosizedcalciumdeficienthydroxyapatitescanbeusedtogeneratenanosizedcalciumdeficient
hydroxyapatitewithasilversubstitutioninthreedifferentconcentrationsbymicrowaveassistedsynthesis.
Thisstudyshowedthatcontrollingtheparametersofthemicrowaveprocesscouldinfluencethesizeofthe
crystalsproduced.Itwasshownthatthemicrowavepowerhadmoreofanimpactonthesizeoftheparticles
thanthelengthoftimeofthetreatment.Theensuingpowderproductcouldbeusedinthefieldofmedicine
andbiomedicalengineeringtomakegraftsandcoatingmetalimplantsinadditiontoworkagainstbacterial
infectionswithouttheuseofantibiotics.Thismethodcanreducemedicinalcostsandtimeofhospitalization
(76).
Polymerbasedsilvercompositeswereproducedusingmicrowaveenergyonthebasisofinterfacial
polymerization.Awater/chloroforminterfacewasusedundermicrowaveirradiationwithnooxidizingagent.
TheproducedsilverNPs(about20nminsize)weresphericalandwelldispersed(77).Silvernitrate
providedsilverionsforthethermalpolymerizationofpyrrole.Theionswereconvertedtosilver/polypyyrole
nanocomposites.Transmissionelectronmicroscopy(TEM)imagesprovedthattheparticleswereabout
510nminsize.Thesilver/polypyyrolehadathickfilm,whichcouldsenseammonia,hydrogensulfide,and
carbondioxideat100,250,and350C,respectively(78).
Microwaveradiationandethyleneglycolcanbeusedtosynthesizesilverpowdersfromsilvernitrateat
temperaturesof100200C.Itwasreportedthatwhenpolyvinylpyrrolidonewasusedinthemixtureof
silvernitrate,theNPsrangedfrom62to78nmindiameter(79).Moreover,FeAgbimetallicNPscouldbe
synthesizedbyusingmicrowaveheatingandanoilsolublesilversalt(80).TheproducedsilverNPswere
characterizedthroughfreezeetchingreplicationTEMwhichrevealedthenanoparticlediameterand
distribution.TheproducedsilverNPs(30nm)weresphericalinshape(81).
Hydrolysisofalkoxysilanesalongwiththesilversalt,inthepresenceofmicrowaveirradiation,canproduce
silver/SiO2compositesols,whichdisplayedantimicrobialproperties(82).Mengandcoworkers(83)
discussedtheutilizationofvariouswaterbasedsynthesisroutestowardtheshapecontrolledsynthesisof
silverNPsandmicrostructures.Severalonepotmethodsemployingcommercialmicrowaveovens,
inexpensive/lowpowerultrasoundcleaners,ortwoelectrodeelectrochemistryweredescribed.Synthesisof
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silvernanostructureswithvariousshapesinsolutionandtheirdopingonunmodifiedsilicaandon/inside
carbonsphereswereinvestigated.
Microwaveassistedsynthesiswasusedtopreparedifferentkindsofnanosilvercolloids.Silvernitratewas
mixedwithsodiumcitrateandthensplitintofivegroups.Eachgroupwasheatedforvaryingdurationsof
timeatdifferenttemperatures.Itwasdeterminedthatthenanosilvercolloidshadanegativelychargedsurface
whenheatedforalongperiodoftimeandapositivelychargedsurfacewhenheatedforashortperiodof
time(84).Moreover,silicaaluminacanbeusedtosynthesizesilverNPswithprecursorslikeAg2Oor
AgNO3.Theparticleswereassmallas3nmindiameterorasbigas50nm.Theywerenotoxidized,and
theparticleswerewellspreadout(85).Inanotherstudy,nanosilver/polyvinylpyrrolidonecomposite
materialsweresynthesizedusingthemicrowaveapproach.TheproducedNPsrangedfrom1525nmand
wereevenlyspreadoutinthepolyvinylpyrrolidonematrix(86).
Polymersandpolysaccharides
SilverNPswerepreparedusingwaterasanenvironmentallyfriendlysolventandpolysaccharidesas
capping/reducingagents.Forinstance,synthesisofstarchsilverNPswascarriedoutwithstarch(capping
agent)andDglucose(reducingagent)inagentlyheatedsystem(87).
ThebindinginteractionsbetweenstarchandproducedsilverNPswereweakandcouldbereversibleat
highertemperatures,allowingseparationofthesynthesizedNPs.Indualpolysaccharidefunction,silverNPs
weresynthesizedbyreductionofsilverionsinsideofnanoscopicstarchtemplates(87,88).Theextensive
networkofhydrogenbandsintemplatesprovidedsurfacepassivationorprotectionagainstnanoparticle
aggregation.GreensynthesisofsilverNPsusingnegativelychargedheparin(reducing/stabilizingagentand
nucleationcontroller)wasalsoreportedbyheatingasolutionofsilvernitrateandheparinto70Cforabout
8h(89).TEMmicrographsdemonstratedanincreaseinparticlesizeofsilverNPswithincreased
concentrationsofsilvernitrate(substrate)andheparin.Moreover,changesinheparinconcentrationvariedthe
morphologyandsizeofsilverNPs.ThesynthesizedsilverNPswerehighlystable,andshowednosignsof
aggregationaftertwomonths(89).Inanotherstudy,stablesilverNPs(1034nm)weresynthesizedby
autoclavingasolutionofsilvernitrate(substrate)andstarch(capping/reducingagent)at15psiand121C
for5min(90).TheseNPswerestableinsolutionforthreemonthsatabout25C.SmallersilverNPs(10
nm)weresynthesizedbymixingtwosolutionsofsilvernitratecontainingstarch(cappingagent),andNaOH
solutionscontainingglucose(reducingagent)inaspinningdiskreactorwithareactiontimeoflessthan10
min(91).
Silvernitrate,glucose,sodiumhydroxide,andstarchcanbeused,respectively,toserveasprecursor,
reducingagent,accelerator,andstabilizerforthereductionsynthesisofsilvernitrate.Polyethyleneglycol
(reducingagentandstabilizingagent)wasusedtopreparestablemonodispersesilvercolloids(~10nm)(92).
BiodegradablestarchworkedasastabilizingagenttosynthesizesilverNPs(520nm).Theanalysesshowed
thattheNPswerecoatedwithalayerofstarch(93).
SilverNPs(~133nm)canbesynthesizedusingsulfatedpolysaccharidewhichcanbeobtainedfrom
marineredalgaePorphyravietnamensis.Itwasreportedthatsulfatemoietyfromthepolysaccharideswas
involvedinsilvernitratereduction.Zetapotentialmeasurementsof35.05mVshowedthattheanionic
polysaccharidehadindeedcappedthenanoparticlessurfacesandcontributedtotheelectrostaticstability.
TheNPswerestableataverybroadpHrange,from2to10,andelectrolyteconcentrationof102M(94).
Polymersthathaveionexchangeablecapacitycanbeusedinmanyfieldsofscience.Thepolymeroften
usedcontainedphosphonicacidgroupsandhadalowmolecularweight.Forinstance,silverNPswere
stabilizedinthepresenceofanionexchangepolymer.Thesurfacemorphologyindicatedthatcubesand
rectangularprismstructureswereformed(95).Copolymerslikecyclodextrin,graftedwithpolyacrylicacid,
canbeusedtoproducesilverNPswherepotassiumpersulfatewasusedastheinitiator.Thecopolymer
reducesandstabilizesthesilverionsthatyieldedsilverNPs.Theconcentrationofthealkali,silvernitrate,the
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copolymer,andthemethodofheatingallplayedanimportantroleindeterminingthesizeoftheproduced
NPs(96).
Poly(methylvinylethercomaleicanhydride)couldbeusedasareducingandstabilizingagentaswell.The
producedNPswerestableatroomtemperatureforuptoamonthandhada58nmcoatofpoly(methyl
vinylethercomaleicanhydride)surroundingthem(97).ItwasreportedthattheNPs(10.213.7nm)were
facecenteredcubic(FCC)structures,notaggregating,andverysphericalinshape(98).Sarkarand
colleagues(99)examinedthesynthesisofsilvernanowiresandNPs.Throughapolypolprocess,withthe
helpofapolymer,silvernanowiresandNPswereformed.ItwasreportedthattheNPswere60200nmin
sizeandheldprismaticandhexagonalshapeswhilethenanowireshaddiametersfrom50to190nmand
lengthsbetween40and1000m.Thereactionoccurredat210Cwhenethyleneglycolwasusedasthe
solvent.Thedifferentphotoluminescenceemissionfromthenanoclustersspreadoutthroughthemethanol
andtheethyleneglycolatroomtemperature.Theexcitationwavelengthsweremeasuredbetween300and
414nm(99).BychangingthereducingandcappingagentsthatareusedtosynthesizesilverNPs,onecan
changethemorphologiesoftheNPs,aswell.ThesynthesisyieldedNPswhichweresphericalinshapeand
around1543nminsizeafterbeingheatedat70Cfor30minwhileatroomtemperature,theparticleswere
only824nm.Sodiumhydroxidereducedsaltinethyleneglycolandcubeswereformeduponsome
aggregation.Byadding5wt%polyvinylpyrrolidoneto1wt%ofstarchsolution(aq),mixturesofspherical
andanisotropicstructureswereproduced.Thereactiontookplaceat70Cfor1h(100).
Tollensmethod
Asimpleonestepprocess,Tollensmethod,hasbeenusedforsynthesisofsilverNPswithacontrolledsize.
ThisgreensynthesistechniqueinvolvesreductionofAg(NH3)2+(asTollensreagent)byanaldehyde(101).
InthemodifiedTollensprocedure,silverionsarereducedbysaccharidesinthepresenceofammonia,
yieldingsilvernanoparticlefilms(50200nm),silverhydrosols(2050nm)andsilverNPsofdifferent
shapes.Inthismethod,ammoniaconcentrationandnatureofthereducingagentplayanimportantrolein
controllingsizeandmorphologyofsilverNPs.Itwasrevealedthatthesmallestparticleswereformedatthe
lowestammoniaconcentration.Glucoseandthelowestammoniaconcentration(5mM)resultedinthe
smallestaverageparticlesizeof57nmwithanintensemaximumofsurfaceplasmonabsorbanceat420nm.
Moreover,increaseinNH3from0.005Mto0.2Mresultedinasimultaneousincreaseinparticlesizeand
polydispersity(102).SilverNPswithcontrollablesizesweresynthesizedbyreductionof[Ag(NH3)2]+with
glucose,galactose,maltose,andlactose(103).
Thenanoparticlesynthesiswascarriedoutatvariousammoniaconcentrations(0.0050.20M)andpH
conditionsof11.513.0resultinginaverageparticlesizesof25450nm.Theparticlesizewasincreasedby
increasing(NH3),andthedifferenceinstructureofreducingagent(monosaccharidesanddisaccharides)and
pH(particlesobtainedatpH11.5weresmallerthanthoseatpH12.5)influencedtheparticlesize.
PolydispersityalsodecreasedbyloweringthepH.ProducedsilverNPswerestabilizedandprotectedby
sodiumdodecylsulfate(SDS),polyoxyethylenesorbitanemonooleate(Tween80),andpolyvinylpyrrolidone
(PVP360)(104,105).
Biobasedmethods Anumberofreportsprevailedintheliteraturesindicatethatsynthesisofnanoparticlesby
chemicalapproachesareecounfriendlyandexpensive.Thus,thereisagrowingneedtodevelop
environmentallyandeconomicallyfriendlyprocesses,whichdonotusetoxicchemicalsinthesynthesis
protocols.Thishasconductedresearcherstolookattheorganisms.Thepotentialoforganismsin
nanoparticlesynthesisrangesfromsimpleprokaryoticbacterialcellstoeukaryoticfungiandplants(106).
Someexamplesofnanoparticleproductionincludeusingbacteriaforgold,silver,cadmium,zinc,magnetite,
andironNPsyeastsforsilver,leadandcadmiumNPsfungiforgold,silverandcadmiumNPsalgaefor
silverandgoldNPsplantsforsilver,gold,palladium,zincoxide,platinum,andmagnetiteNPs(7,107).
BiobasedprotocolscouldbeusedforsynthesisofhighlystableandwellcharacterizedNPswhencritical
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aspects,suchastypesoforganisms,inheritableandgeneticalpropertiesoforganisms,optimalconditionsfor
cellgrowthandenzymeactivity,optimalreactionconditions,andselectionofthebiocatalyststatehavebeen
considered.SizesandmorphologiesoftheNPscanbecontrolledbyalteringsomecriticalconditions,
includingsubstrateconcentration,pH,light,temperature,bufferstrength,electrondonor(e.g.,glucoseor
fructose),biomassandsubstrateconcentration,mixingspeed,andexposuretime.Inthefollowingsection,
wediscussedthesynthesisofNPsusingmicroorganismsandbiologicalsystems(Fig.1andTable3).
Bacteria
BacteriahavebeenexploredinthesynthesisofsilverNPs.ItwasreportedthathighlystablesilverNPs(40
nm)couldbesynthesizedbybioreductionofaqueoussilverionswithaculturesupernatantofnonpathogenic
bacterium,Bacilluslicheniformis(108).Moreover,welldispersedsilvernanocrystals(50nm)were
synthesizedusingthebacteriumB.licheniformis(109).Saifuddinandcoworkers(110)havedescribeda
novelcombinationalsynthesisapproachfortheformationofsilverNPsbyusingacombinationofculture
supernatantofB.subtilisandmicrowaveirradiationinwater.Theyreportedtheextracellularbiosynthesisof
monodispersedAgNPs(550nm)usingsupernatantsofB.subtilis,butinordertoincreasetherateof
reactionandreducetheaggregationoftheproducedNPs,theyusedmicrowaveradiationwhichmight
provideuniformheatingaroundtheNPsandcouldassistthedigestiveripeningofparticleswithno
aggregation.
SilvernanocrystalsofdifferentcompositionsweresuccessfullysynthesizedbyPseudomonasstutzeriAG259
(111).Thesilverresistantbacterialstrain,P.stutzeriAG259,isolatedfromasilvermine,accumulatedsilver
NPsintracellularly,alongwithsomesilversulfide,ranginginsizefrom35to46nm(112).Largerparticles
wereformedwhenP.stutzeriAG259challengedwithhighconcentrationsofsilverionsduringculturing,
resultedintracellularformationofsilverNPs,ranginginsizefromafewnmto200nm(8,111).P.stutzeri
AG259detoxificatedsilverthroughitsprecipitationintheperiplasmicspaceanditsreductiontoelemental
silverwithavarietyofcrystaltypologies,suchashexagonsandequilateraltriangles,aswellasthree
differenttypesofparticles:elementalcrystallinesilver,monoclinicsilversulfideacanthite(Ag2S),anda
furtherundeterminedstructure(111).Theperiplasmicspacelimitedthethicknessofthecrystals,butnottheir
width,whichcouldberatherlarge(100200nm)(8).
Inanotherstudy,rapidbiosynthesisofmetallicNPsofsilverusingthereductionofaqueousAg+ionsby
culturesupernatantsofKlebsiellapneumonia,Escherichiacoli,andEnterobactercloacaewasreported
(113).ThesyntheticprocesswasquitefastandsilverNPswereformedwithin5minofsilverionscomingin
contactwiththecellfiltrate.Itseemsthatnitroreductaseenzymesmightberesponsibleforbioreductionof
silverions.
ItwasalsoreportedthatvisiblelightemissioncouldsignificantlyincreasesynthesisofsilverNPs(16nm)
byculturesupernatantsofK.pneumoniae(114).MonodispersedandstablesilverNPswerealsosuccessfully
synthesizedwithbioreductionof[Ag(NH3)2]+usingAeromonassp.SH10andCorynebacteriumsp.SH09
(115).Itwasspeculatedthat[Ag(NH3)2]+firstreactedwithOHtoformAg2O,whichwasthen
metabolizedindependentlyandreducedtosilverNPsbythebiomass.
Lactobacillusstrains,whenexposedtosilverions,resultedinbiosynthesisofNPswithinthebacterialcells
(116,117).Ithasbeenreportedthatexposureoflacticacidbacteriapresentinthewheyofbuttermilkto
mixturesofsilverionscouldbeusedtogrowNPsofsilver.ThenucleationofsilverNPsoccurredonthecell
surfacethroughsugarsandenzymesinthecellwall,andthenthemetalnucleiweretransportedintothecell
wheretheyaggregatedandgrewtolargersizedparticles.Korbekandiandcolleagues(117)demonstratedthe
bioreductivesynthesisofsilverNPsusingL.caseisubsp.caseiatroomtemperature.Researchershave
reportedqualitativeproductionofsilverNPsbyLactobacillussp.,buttheydidnotoptimizethereaction
mixture.BiosynthesizedsilverNPswerealmostspherical,single(2550nm)orinaggregates(100nm),
attachedtothesurfaceofbiomassorwereinsideandoutsideofthecells.Thereductionofmetalionsand
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stabilizationofthesilverNPswasconfirmedtooccurbyanenzymaticprocess.Electronmicroscopyanalysis
indicatedthatthesilverNPswereformedonthesurfaceofthecytoplasmiccellmembrane,insidethe
cytoplasmandoutsideofthecells,possiblyduetothebioreductionofthemetalionsbyenzymespresenton
thecytoplasmicmembraneandwithinthecytoplasm(117).
Fungi
SilverNPs(550nm)couldbesynthesizedextracellularlyusingFusariumoxysporum,withnoevidenceof
flocculationoftheparticlesevenamonthafterthereaction(118).Thelongtermstabilityofthenanoparticle
solutionmightbeduetothestabilizationofthesilverparticlesbyproteins.ThemorphologyofNPswas
highlyvariable,withgenerallysphericalandoccasionallytriangularshapesobservedinthemicrographs.
SilverNPshavebeenreportedtointeractstronglywithproteinsincludingcytochromec(Cc).Thisprotein
couldbeselfassembledoncitratereducedsilvercolloidsurface(119).Interestingly,adsorptionof(Cc)
coatedcolloidalgoldNPsontoaggregatedcolloidalAgresultedAg:Cc:Aunanoparticleconjugate(120).In
UVvisspectrafromthereactionmixtureafter72h,thepresenceofanabsorptionbandatca.270nmmight
beduetoelectronicexcitationsintryptophanandtyrosineresiduesintheproteins.InF.oxysporum,the
bioreductionofsilverionswasattributedtoanenzymaticprocessinvolvingNADHdependentreductase
(121).TheexposureofsilverionstoF.oxysporum,resultedinthereleaseofnitratereductaseand
subsequentformationofhighlystablesilverNPsinsolution(122).Thesecretedenzymewasfoundtobe
dependentonNADHcofactor.TheymentionedhighstabilityofNPsinsolutionwasduetocappingof
particlesbyreleaseofcappingproteinsbyF.oxysporum.StabilityofthecappingproteinwasfoundtobepH
dependent.AthigherpHvalues(>12),theNPsinsolutionremainedstable,whiletheyaggregatedatlower
pHvalues(<2)astheproteinwasdenatured.Kumarandcoworkers(122)havedemonstratedenzymatic
synthesisofsilverNPswithdifferentchemicalcompositions,sizesandmorphologies,usingNADPH
dependentnitratereductasepurifiedfromF.oxysporumandphytochelatin,invitro.Silverionswerereduced
inthepresenceofnitratereductase,leadingtoformationofastablesilverhydrosol1025nmindiameterand
stabilizedbythecappingpeptide.UseofaspecificenzymeinvitrosynthesisofNPsshowedinteresting
advantages.ThiswouldeliminatethedownstreamprocessingrequiredfortheuseoftheseNPsin
homogeneouscatalysisandotherapplicationssuchasnonlinearoptics.Thebiggestadvantageofthis
protocolbasedonpurifiedenzymewasthedevelopmentofanewapproachforgreensynthesisof
nanomaterialsoverarangeofchemicalcompositionsandshapeswithoutpossibleaggregation.Korbekandi
andcolleagues(123)demonstratedthebioreductivesynthesisofsilverNPsusingF.oxysporum.Previous
researchersreportedqualitativeproductionofsilverNPsbyF.oxysporum,buttheydidnotoptimizethe
reactionmixture.InSEMmicrographs,silverNPswerealmostspherical,single(2550nm)orinaggregates
(100nm),attachedtothesurfaceofbiomass.ThereductionofmetalionsandstabilizationofthesilverNPs
wasconfirmedtooccurbyanenzymaticprocess.ItseemsthatthefirststepinvolvestrappingoftheAg+
ionsbyF.oxysporumcells.MoredetailsofthelocationofNPsproductionbythisfunguswererevealed,and
theprevioustheorieswerecorrected.Incontrastwiththepreviousstudies,itisclaimedthatthenanoparticle
productioninF.oxysporumisintracellularbyengulfingtheNPsinvesicles,transporting,andexcretingof
themthroughexocytosisoutsideofthecells(123).Ingleandcoworkers(124)demonstratedthepotential
abilityofFusariumacuminatumEll.andEv.(USM3793)cellextractsinbiosynthesisofsilverNPs.The
NPsproducedwithin1520minandweresphericalwithabroadsizedistributionintherangeof540nm
withtheaveragediameterof13nm.Anitratedependentreductaseenzymemightactasthereducingagent.
Thewhiterotfungus,Phanerochaetechrysosporium,alsoreducedsilverionstoformnanosilverparticles
(125).Themostdominantmorphologywaspyramidalshape,indifferentsizes,buthexagonalstructures
werealsoobserved.
StablesilverNPscouldbeachievedbyusingAspergillusflavus(126).TheseNPswerefoundtobestablein
waterformorethan3monthswithnosignificantaggregationbecauseofsurfacebindingofstabilizing
materialssecretedbythefungus(126).ExtracellularbiosynthesisofsilverNPs(525nm)usingAspergillus
fumigatushasalsobeeninvestigated(127).MostoftheNPsweresphericalinnaturewithsomeothers
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havingoccasionallytriangularshapes(127).
TheextracellularfiltrateofCladosporiumcladosporioidesbiomasswasusedtosynthesizesilverNPs(128).
Itwassuggestedthatproteins,organicacidsandpolysaccharidesreleasedbyC.cladosporioideswere
responsibleforformationofsphericalcrystallinesilverNPs.Kathiresanandcoworkers(129)haveshown
thatwhentheculturefiltrateofPenicilliumfellutanumwasincubatedwithsilverionsandmaintainedunder
darkconditions,sphericalsilverNPscouldbeproduced.Penicilliumgenuswereusedforgreensynthesisof
silverNPs(130).Penicilliumsp.J3isolatedfromsoilwasabletoproducesilverNPs(131).The
bioreductionofthesilverionsoccurredonthesurfaceofthecellsandproteinsmighthavecriticalroleinthe
formationandstabilizationofthesynthesizedNPs.
Sanghiandcolleagues(132)haveinvestigatedtheabilityofCoriolusversicolorinformationof
monodispersesphericalsilverNPs.thetimetakenforproductionofsilverNPswasreducedfrom72hto1h
underalkalineconditions(pH10).Itwasindicatedthatalkalineconditionsmightbeinvolvedinbioreduction
ofsilverions,waterhydrolysisandinteractionwithproteinfunctionalities.Findingsofthisstudyhaveshown
thatglucosewasnecessaryforthereductionofsilverNPs,andSHoftheproteinplayedanimportantrolein
thebioreduction.
Algae
Afewreportsareavailableregardinggoldaccumulationusingalgalgeneraincludingcyanobacteriaas
biologicalreagent.CyanobacteriaandeukaryoticalgagenerasuchasLyngbyamajuscule,Spirulina
subsalsa,Rhizocloniumheiroglyphicum,Chlorellavulgaris,Cladophoraprolifera,Padinapavonica,
Spirulinaplatensis,andSargassumfluitanscanbeusedascosteffectivemeansforbiorecoveryofgoldout
oftheaqueoussolutions,aswellastheformationofgoldNPs(133,134,135,136).Marinealgaelike
Chaetoceroscalcitrans,Chlorellasalina,IsochrysisgalbanaandTetraselmisgraciliscanalsobeusedfor
reductionofsilverionsandtherebysynthesisofAgNPs(113).Marinecyanobacterium,Oscillatoriawillei
NTDM01hasbeenusedforsynthesisofsilverNPs(100200nm).Silvernitratesolutionincubatedwith
washedmarinecyanobacteriachangedtoayellowcolorfrom72honwards,indicatingtheformationof
silverNPs.WhenSpirulinaplatensisbiomasswasexposedto103MaqueousAgNO3,extracellular
formationofsphericalsilverNPs(716nm)hasbeenresultedin120hat37CatpH5.6(137).Proteins
mightberesponsibleforreductionandstabilizationoftheNPs.InthecaseofC.vulgaris,theproteinsinthe
extracthavedualfunctionofAg+ionreduction,andshapecontrolledsynthesisofNPs.TheAgnanoplates
areobtainedatroomtemperature.ReductionofAg+ionsisdonebythehydroxylgroupsinTyrresiduesand
carboxylgroupsinAsp/Gluresidues.ThisisresponsiblefortheanisotropicgrowthofAgnanoplateswhich
yieldsrodlikeparticleswithameanlengthof44nmandwidthof1624nm.
Plants
SynthesisofNPsusingplantsisverycosteffective,andthuscanbeusedasaneconomicandvaluable
alternativeforthelargescaleproductionofNPs(10).Camelliasinensis(greentea)extracthasbeenusedas
areducingandstabilizingagentforthebiosynthesisofsilverNPs(138).Phenolicacidtypebiomolecules
(e.g.,caffeineandtheophylline)presentintheC.sinensisextractseemedtoberesponsiblefortheformation
andstabilizationofsilverNPs.BlacktealeafextractswerealsousedintheproductionofsilverNPs(139).
TheNPswerestableandhaddifferentshapes,suchasspheres,trapezoids,prisms,androds.Polyphenols
andflavonoidsseemedtoberesponsibleforthebiosynthesisoftheseNPs.
Plantextractsfromalfalfa(Medicagosativa),lemongrass(Cymbopogonflexuosus),andgeranium
(Pelargoniumgraveolens)haveservedasgreenreactantsinsilvernanoparticlesynthesis.Moreover,ahigh
densityofextremelystablesilverNPs(1640nm)wasrapidlysynthesizedbychallengingsilverionswith
Daturametelleafextract(140).Theleafextractsofthisplantcontainsbiomolecules,includingalkaloids,
proteins/enzymes,aminoacids,alcoholiccompounds,andpolysaccharideswhichcouldbeusedas
reductanttoreactwithsilverions,andthereforeusedasscaffoldstodirecttheformationofsilverNPsinthe
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solution.
SongandcolleagueselucidatedthefactthatPinusdesiflora,Diospyroskaki,Ginkobiloba,Magnoliakobus
andPlatanusorientalisleafbrothssynthesizedstablesilverNPswithaverageparticlesizerangingfrom15
to500nm,extracellularly.InthecaseofM.kobusandD.kakileafbroths,thesynthesisrateandfinal
conversiontosilverNPswasfaster,whenthereactiontemperaturewasincreased.Buttheaverageparticle
sizesproducedbyD.kakileafbrothdecreasedfrom50nmto16nm,whentemperaturewasincreasedfrom
25Cto95C(141).Theresearchersalsoillustratedthatonly11minwasrequiredformorethan90%
conversionatthereactiontemperatureof95CusingM.kobusleafbroth(141).Itwasfurtherdemonstrated
thatleafextractsfromtheaquaticmedicinalplant,Nelumbonucifera,wasabletoreducesilverionsand
producesilverNPs(45nm)indifferentshapes(142).
CapsicumannuumcanbeusedforgreensynthesizingsilverNPs(143).Proteinswithaminegroupsreduced
thesilverionsandactedasacontrolduringsynthesis.Afterinteractingwiththesilverions,theprotein's
secondarystructurewasfoundtobealtered.ThecrystallinephaseoftheNPschangedfrompolycrystalline
tosinglecrystallineandincreasedinsizewithincreasingreactiontime.Arecognitionreductionlimited
nucleationandgrowthmodelwassuggestedtoexplainthepossibleformationmechanismofsilverNPsin
CapsicumannuumL.extract(143).
SphericalsilverNPs(4050nm)wereproducedusingleafextractofEuphorbiahirta(144).TheseNPshad
potentialandeffectiveantibacterialpropertyagainstBacilluscereusandStaphylococcusaureus.
Acalyphaindica(Euphorbiaceae)leafextractshaveproducedsilverNPs(2030nm)within30min(145).
TheseNPshadexcellentantimicrobialactivityagainstwaterbornepathogens,E.coliandV.cholera
(minimuminhibitoryconcentration(MIC)=10g/ml).
Moreover,silverNPs(57nm)wereproducedwhen10mlofMoringaoleiferaleafextractwasmixedto90
mlof1mMaqueousofAgNO3andwasheatedat6080Cfor20min.TheseNPshadconsiderable
antimicrobialactivityagainstpathogenicmicroorganisms,includingStaphylococcusaureus,Candida
tropicalis,Klebsiellapneumoniae,andCandidakrusei(146).
IthasbeenreportedthatcottonfibersloadedwithbiosynthesizedsilverNPs(~20nm)usingnaturalextracts
ofEucalyptuscitriodoraandFicusbengalensishadexcellentantibacterialactivityagainstE.coli.These
fibershadpotentialforutilizationinburn/wounddressingsaswellasinthefabricationofantibacterial
textilesandfinishings(147).Garciniamangostanaleafextractcouldbeusedasreducingagentinorderto
biosynthesizesilverNPs(35nm).
TheseNPshadhigheffectiveantimicrobialactivityagainstE.coliandS.aureus(148).Itwasreportedthat
OcimumsanctumleafextractcouldreducesilverionsintocrystallinesilverNPs(430nm)within8minof
reactiontime.TheseNPswerestableduetothepresenceofproteinswhichmayactascappingagents.O.
sanctumleavescontainascorbicacidwhichmayplayanimportantroleinreductionofsilverionsinto
metallicsilverNPs.TheseNPshaveshownstrongantimicrobialactivityagainstE.coliandS.aureus(149).
GreensynthesisofsilverNPsusingCacumenplatycladiextractwasinvestigated.Reducingsugarsand
flavonoidsintheextractseemedtobemainlyresponsibleforreductionofsilverions,andtheirreductive
capabilitypromotedat90C,leadingtoformationofsilverNPs(18.44.6nm)withnarrowsize
distribution.TheproducedNPshadsignificantantibacterialactivityagainstbothgramnegativeandgram
positivebacteria(E.coliandS.aureus)(150).IncaseofCinnamonzeylanicum,thebarkextractcouldbe
usedinbiosynthesisofcubicandhexagonalsilvernanocrystals(3140nm)(151).
TheparticlesizedistributionvariedwithvariationintheamountofC.zeylanicumbarkextract.Thenumber
ofparticlesincreasedwithincreasingdosageduetothevariationintheamountofreductivebiomolecules.
SmallNPswereformedathighpH.TheshapeofsilverNPsathighpHwasmoresphericalinnaturerather
thanellipsoidal.BactericidaleffectofproducednanocrystallinesilverparticleswastestedagainstE.coli
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strain.Asaresult,thevarioustestedconcentrationsof2,5,10,25,and50mg/Lproducedinhibitionof10.9,
32.4,55.8,82,and98.8%,respectively.TheMICwasfoundtobe50mgL1.Inanotherstudy,silverNPs
weresuccessfullyproducedusingP.eldaricabarkextract.CharacterizationbyUVvisibleandTEM
techniquesconfirmedthereductionofsilverionstosilverNPs.Thepreparationofnanostructuredsilver
particlesusingP.eldaricabarkextractprovidesanenvironmentallyfriendlyoption,ascomparedtocurrently
availablechemicaland/orphysicalmethods(152).
StudyingsynthesisofsilverNPswithisolated/purifiedbioorganicsmaygivebetterinsightintothesystem
mechanism.Glutathione(GluCysGly)asareducing/cappingagentcansynthesizewatersolubleandsize
tunablesilverNPswhicheasilybindtoamodelprotein(bovineserumalbumin)(153).Tryptophanresidues
ofsyntheticoligopeptidesattheCterminuswereidentifiedasreducingagentsproducingsilverNPs(154).
Moreover,silverNPsweresynthesizedbyvitaminEinLangmuirBlodgetttechnique,bybiosurfactants
(sophorolipids)andbyLvalinebasedoligopeptideswithchemicalstructures,Z(LVal)3OMeandZ(L
Val)2LCys(SBzl)OMe(155,156).ThesulfurcontentintheZ(LVal)2LCys(SBzl)OMecontrolsthe
shapeandsizeofsilverNPs,whichsuggestsinteractionbetweensilverionsandthioethermoietyofthe
peptide(156).
PurenaturalconstituentscouldbeusedtobioreduceandstabilizesilverNPs.Kasthuriandcoworkers(157)
haveshowntheabilityofapiinextractedfromhennaleavestoproduceanisotropicgoldandquasispherical
silverNPs.Secondaryhydroxylandcarbonylgroupsofapiinwereresponsibleforthebioreductionofmetal
salts.InordertocontrolsizeandshapeofNPs,theyuseddifferentamountsofapiin(asthereducingagent).
TheNPswerestableinwaterfor3months,whichcouldbeattributedtosurfacebindingofapiintoNPs.
Furthermore,geraniolasavolatilecompoundobtainedfromP.graveolenswasusedforbiosynthesisof
silverNPs(110nm).TheyalsoevaluatedinvitrocytotoxicityofsilverNPsagainstFibrosarcomaWehi164
atdifferentconcentrations(15g/ml).Thepresenceof5g/mlofsilverNPssignificantlyinhibitedthecell
line'sgrowth(upto60%)(158).Thevarioussyntheticandnaturalpolymerssuchaspoly(ethyleneglycol),
poly(Nvinyl2pyrrolidone),starch,heparin,polycationicchitosan(14linked2amino2deoxyD
glucose),sodiumalginate,andgumacaciahavebeenreportedasreducingandstabilizingagentsfor
biosynthesisofsilverNPs.Forinstance,itwasreportedthatmonodispersesphericalsilverNPs(~3nm)
couldbesynthesizedusinggumkondagogu(nontoxicpolysaccharidederivedasanexudatefromthebark
ofCochlospermumgossypium)(159).Itwassuggestedthatcarboxylateandhydroxylgroupswereinvolved
incomplexationandbioreductionofsilverionsintoNPs.Thismethodwascompatiblewithgreenchemistry
principlesasthegumservesamatrixforbothbioreductionandstabilizationofthesynthesizedNPs.Dueto
availabilityoflowcostplantderivedbiopolymer,thismethodcouldbeimplementedforlargescalesynthesis
ofhighlystablemonodispersedNPs.
CONCLUSION
SilverNPshavegainedconsiderableinterestbecauseoftheiruniqueproperties,andprovenapplicabilityin
diverseareassuchasmedicine,catalysis,textileengineering,biotechnology,nanobiotechnology,bio
engineeringsciences,electronics,optics,andwatertreatment.TheseNPshavesignificantinhibitoryeffects
againstmicrobialpathogens,andarewidelyusedasantimicrobialagentsinadiverserangeofproducts.
TheflexibilityofsilvernanoparticlesyntheticmethodsandfacileincorporationofsilverNPsintodifferent
mediahaveencouragedresearcherstofurtherinvestigatethemechanisticaspectsofantimicrobial,antiviral
andantiinflammatoryeffectsoftheseNPs.Shape,sizeandsizedistributionofsilverNPscanbecontrolled
byadjustingthereactionconditionssuchasreducingagent,stabilizeroremployingdifferentsynthetic
methods.Therefore,itisimportanttoelucidatetheeffectsofreactionconditionsonmorphologyandsizeof
NPs.
DifferentmethodshavebeendevelopedtoobtainsilverNPsofvariousshapesandsizes,includinglaser
ablation,gammairradiation,electronirradiation,chemicalreduction,photochemicalmethods,microwave
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processing,andthermaldecompositionofsilveroxalateinwaterandinethyleneglycol,andbiological
syntheticmethods.BiosyntheticmethodsofNPsprovideanewpossibilityofconvenientlysynthesizingNPs
usingnaturalreducingandstabilizingagents.Aspossibleenvironmentallyandeconomicallyfriendly
alternativestochemicalandphysicalapproaches,biosynthesisofmetalandsemiconductorNPsusing
organismshasbeensuggested.Monodispersityandparticlesizeandshapeareveryimportantparametersin
theevaluationofNPssynthesis.Therefore,theefficientcontrolonthemorphologyandmonodispersityof
NPsmustbeexplored.Thereactionconditionsshouldbeoptimized.Byusingscreenedorganismswithhigh
productioncapabilityandcontrollingthereactionconditions,wellcharacterizedNPscanbeobtainedby
synthesisratesfasterorcompatibletothoseofchemicalandphysicalapproaches.Thisecofriendlymethod
canpotentiallybeusedinvariousareas,includingpharmaceuticals,cosmetics,foods,andmedical
applications.
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FiguresandTables
Table1
Importantapplicationsofsilvernanoparticles.
Table2
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Someimportantphysical,chemicalandphotochemicalmethodsforsynthesizingandstabilizingsilverNPs.
Fig.1
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BiosynthesisofsilverNPsWedemonstratedthebioreductivesynthesisofsilvernanoparticlesusingF.oxysporum(an
unpublishedscanningelectronmicroscopymicrographrecordedfromsilverNPsproducedbyreactionofsilvernitrate
solution(1mM)withF.oxysporum).
Table3
Someimportantexamplesoforganismsusedforsynthesizingsilvernanoparticles.
ArticlesfromResearchinPharmaceuticalSciencesareprovidedherecourtesyofMedknowPublications
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