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首页 放射化学系列-氟、氯、溴、碘的放射化学(英文)

放射化学系列-氟、氯、溴、碘的放射化学(英文).pdf

放射化学系列-氟、氯、溴、碘的放射化学(英文)

冰夜
2014-01-10 0人阅读 举报 0 0 0 暂无简介

简介:本文档为《放射化学系列-氟、氯、溴、碘的放射化学(英文)pdf》,可适用于工程科技领域

Jl((~C*INationalAcademyvofSciencesNationalResearchCouncilII,NUCLEARSCIENCESERIESTheRadiochemistryofFluorine,chlorine,BromineandIodineCOMMITTEEONNUCLEARSCIENCELFCIJRTItiCkrzfnnmtNationalBureauofStamlamlsROBLgYDEVANS,ViceChdmurnMaeeaohuaertsInetltuteofTeohnol~J~~iiStq“lWethtcgEIFgcCnrporatlon”HJC~TIS‘G(iMANovBrockhavenNationalLaboratoryT~erlab,IhoSAMUELEPSTHNWWAYNEMEINKECaliforniaInetituteofTeohnolmUnlversltyofMichiganHERBERTGCkDSTEINAHSNELLNuolearweloprgentCorporationofOakRidgeNgtionalLaboratorymrkaEAUEHZHGHJGOMBERGUmlveieltyofWiehlngtOnUniversiwofMichiganDMVANPATTER“EILKLEMABartolReseamihlundattonNorthwesternUnlversltyROBERTLPLATZMANArgonnehIatbtalLaboratoryLIAISON*EMBERS”PAULCAEBERSOLDAtomicEnergyCotmglusionJHOWARDMcMILLENNattondSoknceFounthttlonwDImRYUSAirForoeWILLIAMEWRICiRTOiceofNavalReaeamhSUBCOMMITTEEONRADOCHEMISTRYWWAYNEMEINKE,CkahwtanE~”LRYDEUnkershyofMichig~UnlverdwofCalifornia(Berkeley)NATHANiLLOUHAROLDYNWYRdlologlcdDmmLaboratoryMoundLahoiatoryGREGORYRCHOPPLNGEORGEiEDDICOTTEFlorCdaSfmUritvertggOakRidgeNationalLabormoryGEORGEACOWANELLISPSTEINBERGLos~JlSfWieIltifiChhOWOryArgonueNationalLaboratoryARTHURWFAIRHALLPETERCSTEVENSONUniversityof“WadtonUnlverfiitydCalifomkLivermore)HARMONFINSTONLEOYAFFEBrookhmenNatlomilLaboratoryMcGfllUniversityTheRadiochemistryofFluorine,Chlorine,BromineandlodineByJACOBKLEINBERGandGACOWANUniversityofCaliforniaLosAlamosSm”entifcLaboratoryLosAlamos,NewMexicoJanuarySEPPRWERTYESubcommitteeonRadiochemietryNationalAcademyofSciencesNationalResearchCouncilPrintedinUSAPrice$AveifeblefromtheOfficeofTeclmlceLIServices,IWputmentofCommerce,WMMncm,DCFOREWORDTheSubcommitteeonRadiochemistryisoneofanumtirofsubcommitteesworkingundertheCommitteeonNuclearSciencewithintheNationalAcdeqyofSciencesNationalResearchcouncilItsmembersrepresmtgovernment,industrial,anduniversityklmratotiesintheareaaofnuclearchemistryandandyticdchemistry‘TheSubcommitteehasconcerneditseMwiththoseareasofnucleexsciencewhichinvolvethechemist,suchasthecollectionanddistributionofradiochemicalprocedures,theestabMshmentofspecificationsforraikLochemlcalJypurereagents,theproblemsofstockpilinguncontaminatedmaterials,theavailabilityofcyclotrontimeforserviceirradiations,theplsceofradiochemistryhtheundergraduatecollegeprogram,etcThisseriesofmonographshasgxownoutoftheneedforuptodatecompilationsofradlochemicalinfomnationaudproceduresTheSubcommitteehaserdeavrmedtopresentaseriesWhichwillbeofmaxhmmusetotheworkscientistandwhichcontainsthelatestavailableIDformatlonEachmonographcollectshonevolumetheperttientinforstionrequiredforradlochemicalworkwithanindividualelmentoragroupofcloselyrelatedelementsAuexpertintheradiochemistryoftheparticularelementhaswrittenthemcno~aph,followingastandardfomatdevelopedbytheSubcommitteeTheAtomicEnergyCommissionhasaponsoredtheprtitingoftheseriesTheSubcommitteeiscoflidentthesepublicationswillbeusefulnot”onlytotheradiochemistbutalEototheresearchworkerinotherfieldssuchasphysics,biochemistryor”medictiewhowishestouseradiochemicaltechniquestosolveaspecificyroblemWWayneMeinke,ChairmanSubcommitteeonRadiochemistryiiiCONTENTSGeulefralReferencetamnlorgmlcEndAnaLytlaidClMstryoftbeIlogeneIvWJecthmofRadiocbmlcalRocedumsforntie,~jErcadne,andIodinev’INTRODUCTIONThisvolumewhichdealswiththeradiochemistryoffluorine,chlorine,bromineandiodineoneofaseriemofmonographsonradiochemiatryoftheelementsThereisincludedareviewofthenuclearandchemicalfeatureaofparticularinteresttotheradiochemist,adiscussionofproblemBofdissolutionofasampleandcountingtechniques,andfinally,aCollectionofradiochemicalproceduresfortheele~nteasfoundintheliteratureTheseriesofmxmgraptitillcoverallelemntsforwhichradiochemicalproceduresarepertinentPlansincluderevisionofthemonographperiodicallyasnewtechniqueandprocedureswarrsntThereaderisthereforeencouragedtocalltotheat~ntionoftheauthorenypublishedoronpubliehedmaterialontheradiochemistryoffluorine,chlorine,bromineandiodinewhichmightbeincludedinarevised~rsionofthrnnographviTheRadiochemistryofFluorine,Chlorine,BromineandIodineJMMBHIEIIEtEHGAKDGACOWMUniversityofCalMbrniaIcmAmmqMientiIoratoryusALmos,mewMexicoJ~$LGHWZMLREFHRlmcHsToTEEn’mRMNIcmAmUmmALmRasl!RYm’HALwmsWFHUetid,GEFLuudell,HABrightandJHoffhn,FyQpWd~cAnalySlEIJadHdition,JohnMOYandSone,hC,NewYark,,ChandhWMIatherandJHHildebmnd,laferaumBmkof~~Cchedstry,*dHditlon,TheMlJanCmipany,,ChxTMoeXLer,InorganicMmislzy,AnAdvancedTeAook,JWileyatldSons,hC,NewYak,,ChHRemy,TreatiseonInorganlcChenllstxy(translatedbyJSAlidtIWSOll),EIBtierPtiblluCcmFSW,Amaterdfnn,x,tiNVSidguick,TheChemicalFxamenteand!Iheti~*,HoldWversityPress,UaMlol,,pplo$nalFPTceadlandWTHaXL,AualytlcalChedslry,gtbWtiorl,VolI,Jn~by=dScms,~C,NewYork,,PP*CJRedden,AualytlcalChedalxyoftheManhattanProt,Chaand,MrawHiJlHookCo,WYork,SIITABLEOFIwItm*OFFImRllm,CmFmfE,~JUUUHECl==*~eBecPUomin{tiEc$stab(Cb’lmdence*”)secreecPa~necB,IAble(dnmdence“$)Xlflw{B*$EC(K)lofistable(ebundence)nlinWr#(ap)Om(d,n)e(P,)P(,U)ole(a,pi)O“(p,n)Fm(n,n)Fm(,n)~=”(a,a)endOthermEeidlrel*(d,P)~=(n~y)NP(n,cz)#(p,n)(d,n)~(p,n)c*(,n)clss(P,Pn)Malltarcl=#(qn)~(d,n)matiNatuBKLCl=(n,)Clge(d,p)HeialrelCls(d,p)C(n,)endsIITABIEm’~aFELummE,clmmmE,BRcMIXEMDI~IEE(Contld)IeotopeHalfIAfamofrlewMethodofPrquraumlpJselhrIuindnbr“br“brmin<minPB{PEC{BECBL=PPITP~astale(LnameXI*)BllrIT#rdnp{$(yez#Staue(dnlndlwloe)A‘(,P)~Fe,Co,Cu,AeA(n,p)mqc=,n)Cd=(c=,a)seqtl,n)se(P,)A=(u,)*n(PAAt(a,n)*(a,p)Sem(d,n)Ae=(a,n)S==(d,p)em(p,n)~(n)Brw(n,n)IkghtarBrNetuialS(d,ti)*n(a,p)Se=(p,n)m=(n,)endoers*m(pn)()*=(dsp)Rr,n)UBre(n,n)NUlwImtopeHalfLifeTypeofIkayMeaodof’R’epuatiml~‘hr#hr#uinlldn#BaecEIPBecIllslgnlln~br~hldnk’dayPPP{Pfnl($)PPPP‘mYQPQ’S,n)Se=(d,n)H,)andOti=(d,n)IaP(,a)W’y:im!H,m,Blssilmm,u,u,mF#(n,tZ)SEJflaaicmm,uRklsiaam,uDugh*SeIlssiwluEsionuFassionuRP(#gill)orPdylT,n)wmsb=(aJkrl)wSb=(a,n)Tel=(p,n)=*u~(a,n)mUl*X=*U(a,n)m=S(a,n)TeE(p,n)andotherspyEC~dayEc$*f~sle(abmdame)*pqpexlo~yearP~lso*hrP*bPpZlbrPpshrPm(a,a)Teu(tl,n)~flBEiOnMDsUItelrXel=Sb=(a,n)Te=(d,n)Tee(p,n)IL(n,n)andOBNdillralI=(n,y)Te=qtL,n)Tel=(p,n)~BSiOnUTe=O(d,n)El!#”(p,n)=(n,)Oe=g(n,~)T”(d,n)afissionm,umBSi~Th,U,~,PU~=SpaflBeionuF’lsslonm,u,u==Dlter!rd=wfissionR),uMssimu,Pu~=s~fiBSiOnUFISsimm,u,u=,Pu*~=nTNEiIEQFnmafwm~,~,BRQHEAl!U)ICent’d)IsotopeHalfLifeTypbofIbcayWuMdofPreparationpshrrSpallfleeimUFiEsicQm,u,PuDaugb*m=~aec{FFISslcmu,PuPn(~“*)peBecrFissionu,entarC=paecB~salonU,encehxBa=l(hlyaeIeotopamliatadwhichfaUincategmieaAmdBtiale~Iaotqea”,D~,JMHolJandaraud(ToEkklmrg,Rsviewof~Phyalce,~No,Partn,s$GeQaralPmPartieaofwmeEeloewe~,Cmorine,branina,Edbdine,Withwraepmtiveatmicrnmbera,,and,alongwith**,cqpkslmhalogcma!Qmaeelemeutepoaaesam:~svakmcashellcmflgwaticm~differsmmdlyinitschemistrytheoimrhelngem*ddfflerencecbaervedarelargelyattributablemlbyhighelectawmgativity,smallsize,andInebilityto~temarethlxleighteleclmmeintllmvalenceshelldiatmicnatureoftbselemntarymolecules,intherelativelyMimgeamountsofgyreqdmdtodissociate*semleculna(heatofdissociation,kcalble:F=**clIzTF~G),afiwe~valuesfortheelecmmaffinitiesoftieatma(F)*CLBF,~kceLgatcm)Wmeattendencyforthehalogenetoreacho*tcafigumtialaFeflectidintbeebundanceofhdldeaaltaandintllalarge~ofcmpkfi~~~tiahwaOovaleaoeofmmImI’hOrim,thiaitlleolllycovalenceFerndttedfmUleualrhalcgem,wheremtioesharedpedreAswuldbeexpectad,iodine,thelergestofthalogem,cenfolmthegreatestmnmerofmvlslsntbculdsmmticanpcamdswlthtalsthehalogemareneceessmilylnanegativemeoxldatimststeWithactiwsmwhichgiverisetohugecationsofWcharge,ig,dllml,Calcim,tblsoxldatlcmslateiElanionicWOutheotherhemd,withmetels,emnactiveCUESeucbasbarylMumandalumimm,whicharewtantlalsowrcesofionsofrelativelyMchargedsnsity,thebandsbetweenhalogen,particularlychlorim,braolnemlodMe,andmeware~tlyc~tin~tarwithameWexhibitingawarletyofoxidationabates,thecovalentactermfmyonehIsMdetypeImresaeswithimreaslngoSdatdonstateoftheIneltalThis*endisgenemUyao~edbyincreasingvolatilityaswellasincreeelngmlubilityinncmpolaxor~csolvents(eg,canpsreFSCISandFc)Dunionwithothernonme,fluorlqe,*meteleclmcmegatlvedamentknown,invariablymaybeqdedesbeingInanegativeoxidationstate!lheotherhaksusBRYbeC~idSr*sstibitingeitkekXbOnegativemelectropositivecharactmdependingupau~dectimegatlvltyofti~ttowblcbtheymeJoinedThemostc~SixuoneInwbicbIns,braulnendIodineexblbitpositiveofidatlonstesmItismtewWthatiodine,tieleastele~egativehalogen,isectuallycapableoffuingtiecationtcspcicles”~s~stAbleentitycsabeconsiderablyslizedbycodlnationwithsuchmcbasesasPYIUJNThusSudlcqguunds“ti“Py~andIPY~,emongothers,havekm~qe~nlamlchsCbangeeIncnlmattonsta*arefrequmltlyofBlmicmceInradlochmlcalproceduresfortheanelysisofchlorine,brmdneandiodine,tbe~~tlalrelationebi~wblchexistamcmgthemiousoxidationstatesoftieeeedmentsareshownonpageAcidicSolutiana:Basic*lutims:I,maervatimemEeciesof~canceintheAnalyticalQlemis*ofmlogens~viewofthefactthatthef~tiondel~~ybrmineendiodllleisoflmpmtameinanmiberofmthodefortheanalytical*terdnatimoftheseelements,spropertiesofthesesdbstanceearedesmibedAsisevident~thePtesJUaldatacitadave,btibramineendiodinearefWrlystrongoxhliz~agentsBrminesrathmmlubleinwater,gdissolvinghgofwaterat°themlubili~ofiodineisDnlchsmaller(Ogperliterofsolutimat°)Fmbothelszmnts,solutininwaterisaccompaniedbythemdnreactionH~=HXHXOForbrmdne,tieequKUhriumconstantforthisreactioniixaforIcddne,x=(Forchlmfne,theconstantisxThereactionISofnosignificanceftmfluorine,wblchvigmouslyliberatesOXYWI=dOSaefimUqtidwaterwiththefurmationofhydrofluorlcacid)Incoldtitsalbllnesolutionshypdmlltesaltsaefamedinwemconcenixatedalkanesolutionsthehypobalitiicmdis~matestohalati(X)andhalideionswisccqletdymisciblewithccmionorganicsolventsIodineIsgenertiyappreciablysolubleinorganicsolventsIhsolventsexblbitingnodcmorcharacteristics,eg,carbon~d,cblmfm,carbontetrachloride,thesolutionssrevioletinCInSummticsolventsSUChasbenzeneendtdllenethesoluticmeareredbsolventswhichmayberegsudedastypicalLewisbases(eg,etier,pyridine,iodineIsmostsolubleandgivesbrownsolutionsThereislittledmbtthatinboththeredendbrownsolutimssolvaticmoftieIdineoccursAn~tcharacteristicofelementaryicdineIsitsabiJStytocmitdnewithiodideIOUtoformFEyiodideticms,~,ofwhichthetriiodideion,~,istiemoststableotherpolyiodiaeionswhichhavebeenidentifiedare~,IandQ!lhemats~lepolyiodidesaltsareformedwithlargecatbns,eg,Cs,gpaternaryanmxmiumIons!lkibrauideeareknown,buttheymmuchlessslethantriiodides‘heexistenceofthetzichlorideiminsolutionhasbeendefinitelyetillshed,butnosbsblesolldsaltsofthisanionhavebeenisolated!lhe=flucmi*ionisunknownThetrendinstabilltyofthetlbaliaeloneb~“Bolutionisshownbythevaluesforeequilibriumconstantiforereactian,rwIodinetheconstitat°isfarbrmineandforcbbrine,=’MostoftheanalyticaldeterminationsforthehalogensinvolveprecipitationreactionsofthehalideionsFluoriaemaybeprecipitatedasthecalciumsalt(Ksp°:x~)orasleadchloroflwrideFbFa“PbC)Precipitationofthecalciumsaltisnotentirelysatisfactoryevenwhenthesolutiontobetestedcontainsappreciblesmountsoffluoride,lowresultsccmunonlybeingobtainedPrecipitationofleadchlorofluorideisusuallycarriedoutinthePHrangetheprecipitatecanbeweighedassuch,orthefluroinecontentcanbedeterminedindirectlyfromtitrationofthechlorideChloride,brcxuide,oriodidecanbedeterminedbyprecipitationwithsilverion(Ksp°:*cx’jrx=MI~xlolefilverfluorideexhibitsavolubilityofgpergofwateratabout)TheanalyticalproceduremaybeagravimetriconematitrationIodidemaybeprecipitatedauddetermhedasthe~di~(II)saltASamatteroffact,precipitationbymeansof~um(II)chloridefrcuuaslightlyacidicsolutionisasatisfactorymethodlfortheseparationofiodidefromchlorideandbromideAmorecannonwayofseparatingiodidefromsolutionwiththeotherhalidesisbytheadditionofnitrousacid,whichconvertsiodidetofreeiodineandiswithouteffectontheremaininghalidesSep~ationofbromidefromchloridecanbeaccomplishedbyoxidationofthefozmertoelementarybrcaninebypotassiumpermanganateinaceticacidsolutionItcanalsobeaffectedfromthesilversaltssilverbromideisessentiallyinsolubleinanaqueoussolutionofammoniumcarbonate,whereastie‘chlorideissolubleIonExchmgeSeparationsIonexchangehasbeenusedinfrequentlyforseparationofthehalogensfromeachother,probablybecausethewellknownconversiontothefreeelementfollowedbyextractionintoauorganicsolmtissowelLestablishedAnionexchangeseparationofthehalideionswasdemonstratedearlyinthehistoryofmodernexchmgematerialsA‘hemmnoniumsaltsoffluoride,chloride,brcmide,audiodidewereabsorbedonDowex(mesh)inthenitrateformElutionwasperformedatroomtemperaturewith~soditunnitrateataPHofFluoridecomesofffirs”tPeaktovalleyratiosoftobetweenF,Cl,Br,andwereobtainedindicatinggoodsepsxationAsimilaseparationhasbeenusedfordeterminingClandBrinmixturesofthetwobyabsorptiononastrongbaseanionresin,XEsuppliedbyRohmandkSnonionicwettingCompanyTheelutingagentwasONaNOScontainingaagentAfurtherapplicationofthismethodhasbeenloueedforthemalyticalegtiad~,Br,andIaIbwml~resin,theelu~agentONaNOShcdllarheJlmparatlonmaBlamllghaaereeinusedONaNDstoeluteCl‘lMeelumtcmcematlonw=thenticreaeedtogtoaccelezatetheelutlanofBrendA=thodforsg~Cl,~andmaknswaeofpmdpitatlm*cmaw*yACOIUmUlmImdeUfIlgtOSOrX)aendahmlnalnatoratioofmipltenttoflllurmeBlxreofloneispawed~~ColuumeandvedlneunMghtfortominutiBmeutofintificaticmisforIendMta‘y~mwendmhhalldeehavebaaisquatedm~~tedwitiASXwclmcmtography=aactivatluaanalyelshavebeanccabmfortileaetemillationofs,Br,endclInOrgmlcCcqx!undeF’horidehaebeenquantlktivdysqazatedfmmtasmuchmmrueonaDowexl~colmnninthehydroxideformmmeh,slz’cmgbaeeresinwaEcycledetheewiti~NaOHend~Ef,leftlnuhydroxldefonnelutionWeperformedwithO=NaOH~uorideheEbmstedfrcmdumlnumbyelgfrathealkBllneformofastrongbaseredng!lheelmlnmccmsmoffthecolumnflretRateeofuQmendenaffinitysemieeforseveralmlcmeIncludlngthehdeBhavebeaudetemninedforhydroueZtiCODiUUlOXIdemTheaffhltysesdeixmdnedwithOlLJEolutlaneis:Cl,N>Br,,m:>>soAsyntheticinorgmiclaexchangerwueedtoremovetigequentitleaofunwantedFeactivitythatfomdeeabyproductinacmkaalationUTheaolutimInconcentratedHClweaPsedthroughanA~COaudmorethem~ofIIMfluoridewae*sorbedsolventWtcactllnlse~ticmeExtractionofthefreeelmtformof*halogenintosolvant(C~,CE~)afterueeof*properoxldlzingagent,beenafavoradseparationmethodforCl,Br,endISevwral~leearevanintiesectiononproceduresanCmgmicwlcmgdetailedBecaueemanyorganiccaundedthehalogmscanbepewed,SzllErdchalmereexactionayehavebveryccmmunlywadtoticreeeethespeclflcactivityofahalogen!JherecoilenergyoftheIncidentnuclearparticlebreaketieHbetweenMhalogenendthecarbcmalxmExtractionof*orgenlcsolutionwithwaterthenyieldeahighepciflcactivityofthehalldeHeutionactivationfolluwedbyexb’acticmdBrandIaaddisILtilJJtialofclhasbeenusedaesmanalyticalmlmlodtoae~ueaxnlntsOfmimdhalldeeTWmauylstlbmlumsulfateWbeenusedtoertrectfluoridefrmaaolutlcmin~~eId”hmeUmdIsmoreusefulfmconcentratlcmpurposesIbnesahighlyspecificsepJustlcmAw~ofHzSmeaddedtothesolutloncmtddnguptomgtiFmillimoleoftetrtauylBtibOUi~sulfateladandte~broughttomlItisshakanuilhtheeSuccessivenil~CQSOfQendtheClayerLBevaporatedaudweidJxstiuatlalaemtlcmeDistillatitmoffluarineashydrofluoellicicacidforsepmtlngfluoridefrcmInfaringionsbeforeapltatlaaJChlorine,branlne,andIodinecsnbese~tedbyisctxmolyusedtitrationorpreSelectimoddationanddls~tionoftheeleamtIodineisaxidiztibyadditlaofHaNhdiluteH~MErminecaubemddlzedulthtelluricacid,XMQh~ticacid,mKH(I~)indilutetitiCacidCMorinecanbeoxldlsedbyadditionofancen~tedEUOSchangeRWWticmAprimerequisiteinradlochemiualanalyticalproceduresIsthecmeteexchsuwebetieentheradioactivespeciesbeingdeterminedaudcarrierObselrlmtionaonedlaugebetweenvarioushalngenentitiesbaqueousIlbedllmlare~edhlouExchangebetweeufreehalogenandhalddeIminsolutlaIsccaqpleteuithinm~timeofmhlngandse~tionThreeplausiblemechaulmsfarexcbmgehavebeenpostulated~!IheeeIn

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