in the hanford reach riverbed - radioactivist · 2009. 2. 27. · introduction wild fall chinook...
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Uranium-233 Hanford Reach
Riverbed
By: Norm Buske The RadioActivist Campaign [email protected]
Rev. 2
January 2006
in the
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Uranium-233 in the Hanford Reach Riverbed
Summary The 50-mile Hanford Reach of the Columbia River in Eastern Washington is recognized as
• a scenic recreation area and national monument.• crucial spawning habitat for wild chinook salmon.• part of the Columbia Basin irrigation project and the mid-Columbia hydro-
electric power generation system.• collecting radioactive and toxic wastes from old nuclear weapons production
at the Hanford Site.
ThepresentstudyconfirmsthatsomeofHanford’sworstradioactivewasteisstickingtoColumbiariverbed sediments.
Hanfordreactorsproduceduranium-233(U-233)fortacticalnuclearweaponsduringtheColdWar.TRAChassurveyedHanford’sradioactivityintheriverbedsince1999.BasedontheevidenceinTRAC’sstudies,theWashingtonStateEcologyDepartmentjointlysampledriverbedsedimentswithTRACon23 September 2004. Ecology then analyzed colloids from the sediment samples to test for U-233. The objectivewastoanswerthequestion:IsU-233ofHanfordoriginpresentorabsentinHanfordReachsediment?
TRACandEcologyagreedonsamplelocations.OnebackgroundsamplewascollectedatVernita,upstreamofHanfordandsonotinfluencedbyHanforddischargesintotheriver.Threesampleswerecollectedfromtheriverbed,neartheupstreamendofD-Island.ThosethreeD-Islandsamplesprovidedthetest data for this study. Unfortunately,thedetectionleveltoidentifyU-233wasnotclearlyspecifiedforEcology’sanalyses.Ecology’sICP-MSanalyseshadadetectionlevelahundredtimesabovethelevelrequiredfordetectionofU-233andsoprovidedonlynilresults.Ecology’salphaspectrometrydidnotreportU-233distinctfromnaturally occurring U-234.
EcologyprovideditsalphaspectrometrydatafilestoTRAC.TRACappliedanordinaryanalyticalprocedure to separate a U-233 peak from the U–234 peaks in the spectra. The three test samples from D-IslandyieldedU-233intherangeof0.010 to 0.024 pCi/g.Thebackground(VernitaBKG),blank,andspikeresultswereeach0.000pCi/g.These results confirm the presence of U-233 of Hanford origin, on sediments in the riverbed of the Hanford Reach. Thelevelofconfidenceinthisconfirmationdependsonpreviously held beliefs.
TheU-233wasteispresentincolloids that stick on sediments under the Hanford Reach. The colloidsinteractchemicallywithwaterintheriverbed,wheresalmonhatchlingslive.
Contents Summary...................................................................................................BelowBackground and Sampling Locations ........................................................ 2Introduction................................................................................................ 3Procedure:Chronology............................................................................. 4Analytical Results ...................................................................................... 7Confidence................................................................................................ 8Implications............................................................................................... 9References(hyperlinked)..........................................................................10ProducedandPublishedby......................................................................10
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Uranium-233 in the Hanford Reach Riverbed
Reactor areas are identified by letter. Major salmon spawning areas are identified by numbered black bars (Areas #1 - #10). The Vernita background sample was collected a half mile upstream of Hanford River Mile (HRM) zero at Vernita Bridge. The three test samples were collected from the upstream end of D-Island, about HRM 10.5.
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Uranium-233 in the Hanford Reach Riverbed
Introduction Wildfallchinooksalmonspawnintenareasthatunderliethe50-mileHanfordReachoftheColumbiaRiverinEasternWashington;seeLocationsonPage2.Theseareasarecrucialhabitatforthewildsalmonhatchlings(alevin) that are believed to maintain the strength of the salmon stock for a billion-dollar-a-year commerce.
BeginninginWorldWarII,Hanford’snuclearreactors,builtontheshoreoftheColumbia,usedriverwatertocooltheircores.Radioactiveandtoxicwastesfromthereactorsweredischargedbackintotheriver.
Hanford’sbestknownnuclearproductwasplutonium-239(Pu-239).Pu-239poweredtheTrinityTestatAlamogordo,NewMexico,on16July1945andthebombdroppedonNagasaki,Japanon9August1945,endingWorldWarII.PlutoniumfromHanford’sreactors provided much of the strength of the U.S. nuclear deterrent during the Cold War.
InadditiontoPu-239,Hanfordproducedawidevarietyofspecial nuclear materials, ranging from test specimens to full production.DuringtheColdWar,allHanford’s9reactorsproduceduranium-233(U-233)fortacticalnuclearweapons.
In2000,theU.S.DepartmentofEnergy,owneroftheHanfordSite, began to declassify information about its still semi-secret productionofU-233inHanford’sreactors.Followingarequest
undertheFreedomofInformationAct,TRAClookedovertensofthousandsofpagesofdocumentsrelatingtoU-233production,processing,andwastedisposalatHanford.SeeReferences4and5,forasummaryofTRAC’sdiscoveries.
Since1999,TRAChassurveyedartificialradioactivityinthesedimentsundertheHanfordReachoftheColumbiaRiver.SeeReferences3,4,and5.BasedonTRAC’saccumulatingevidenceofU-233wasteintheriverbed,theWashingtonStateEcologyDepartmentjointlysampledriverbedsedimentswithTRACon23September2004.Thesamplesweresplitthreewaysforqualitycontrolandassurance.
TRACextractedthecolloidalandfinefractionfromonesetofthesamplesplitsandreturnedthatfraction to Ecology. Ecology then analyzed those four sample fractions, as Stakeholder Columbia River Samples,totestforthepresenceorabsenceofU-233.Theobjectivewastoanswerthequestion:Is U-233 of Hanford origin present in Hanford Reach sediment?—Thiswasaconfirmationorrefutationtest,notan indication of the importance of any U-233 that might be present.
RepresentativesofEcology,ofthestateDepartmentofHealth(DivisionofRadiationProtection),ofthePacificNorthwestNationalLaboratory,andofTRACparticipatedinsamplecollectionon23September2004.Theseparticipantscollaboratedtoselecttheexactsamplinglocations.Thisassuredthatsamplelocationwasunobjectionablefromanyknownstandpoint.OnesamplewascollectednearVernita,upstreamofHanfordoperationsandsowasnotinfluencedbyHanforddischargesintotheriver.Thatsamplerepresentedbackground(BKG)forthisstudy.Threesampleswerecollectedfromtheriverbed,neartheupstreamendofD-Island.ThosethreeD-Islandsamplesprovidedthetestdataforthisstudy.
Therequireddetectionlevelwasdiscussed,butevidentlynotagreed.Ecologyunderstoodthattheircontractlaboratorieswould“runthesamplesatthelowestdetectionlimitforwhichtheyarequalityassured/qualitycontrolled[Reference1].”TRACunderstoodthatdetectionleveltobe1part/trillion(=0.1µg/kg)bymassor0.01pCi/gactivity,thelevelrequiredtodetectU-233.Ecology’sactualdetectionlevelwas100parts/trillion(=10µg/kg),byICP-MS.Ecology’sICP-MSanalyseshadadetectionlevelahundredtimesabovetherequiredlevelandsocouldnotprovideanymeaningfulresults.
D-Reactor is one of Hanford’s 9 nuclear reac-tors that produced U-233 for nuclear weap-ons during the Cold War.
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Uranium-233 in the Hanford Reach Riverbed
Ecology’salphaspectrometrydidnotreportU-233separatelyfromU-234intheirisotopicuraniumanalyses.
The alpha spectra of the samples and reference materials, for isotopic uranium, contain alpha energypeaksfornaturallyoccurringU-234,U-235,andU-238,aswellaspeaksforartificialU-233ifitispresentintheanalyzedmaterial.TheU-233alphapeaksarewithinthegeneralregionoftheU-234peaks.Therefore,Ecology’scontractlaboratorydidnotreportU-233andU-234separately,butinsteadreportedthesumofthosetwoisotopicactivitiesas“U-233/U-234”.
Nonetheless, the main alpha emission from U-233 has distinctively higher energy than the highest alpha energy from U-234 decay. Therefore, the activity of U-233 can be analytically separated from the activityofU-234,eventhoughEcology’scontractlaboratorydidnotmakethisdistinctionintheirreport.
TRAC has performed this ordinary, post-analysis separation of U-233 from U-234. This is the report of that analytical separation of the three test samples, the background sample, a tracer, and a blank.
Procedure: Chronology Onebackground(BKG)samplewascollectedahalfmileupstreamofVernita,whichisupstreamofHanfordSiteoperations.Thislocation(onWGS84datum)isausualreferencebackgroundforHanfordSite impact studies:
VernitaBKG: NorthLatitude: 46.63435° WestLongitude: 119.75458°
TheVernitasampleprovidedacheckforanon-HanfordsourceofU-233,suchasworldwidefalloutfromatmospherictestingofnuclearweaponsorafalsepositiveanalyticalresult.
Threesedimentsampleswerecollectedfromtheriverbed,ontheupstreamendofD-Island.
ThelocationsoftheseD-Islandsampleswereasfollows:
D-Island“1”: NorthLatitude: 46.70151° WestLongitude: 119.54201°D-Island“2”: “ 46.70153° “ 119.54167°D-Island“3”: “ 46.70175° “ 119.54136°
ThosethreesampleswerecollectedupstreamoftheD-/DR-Reactordischargepipestoeliminatethepossibility of sampling U-233 debris that might have been discharged into the river from failed target rods in D-orDR-Reactor.TheD-Reactordischargepipewasmarkedbyriserventslocatedbetween:
northriser: NorthLatitude: 46.70245° WestLongitude: 119.54135°southriser: “ 46.70224° “ 119.54117°
TheDR-Reactordischargepipewasfartherdownstream.
Ateachsamplinglocation,largegravelsandcobbleswereremovedbyhandandshovelfromthesediments.
Finersedimentswereshoveledintoa2-mmstandardstainlesssteelsieve,overacollectingpan(seephotosidebaronnextpage).Thecontentsofthecollectingpanwerepouredintoalargesamplebag.Theparticipantsrepeatedtheprocessuntilthesamplebagwasfilledforthree-waysplitting:toEcology,tothestateHealthDepartment’sDivisionofRadiationProtection,andtoTRAC.TRACpreparedandre-submitted the samples to Ecology.
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Uranium-233 in the Hanford Reach Riverbed
TRACextractedcolloidsfromthesurfacesofthesedimentsamples,asfollows:About750gofsedimentwereplacedintoroundedsquareplasticbottles(Cole-ParmerCat.No.A-62270-00)whichwerethenfilledwithdistilledwater.Thebottleswererotatedhorizontallyat6rpmforatleast5hours(Cole-ParmerRoto-TorqueRotator,Cat.No.A07637-00withatesttubebasketmodifiedtorotatetwo,quartbottlesatatime).
The rotated samples werethenflushedwithdistilledwaterthroughastandard0.475 mm stainless steel sieve. Theextractedcolloidsandtheveryfinesedimentsthatpassedthroughthesievewereovendriedat<90°Candweighed.On 7 October 2004, TRAC shipped each sample (one of 3 ounces and three of 4 ounces) to Ecology for analysis, along withaChainofCustodyletter.
On28October2004,Ecologyshippedsplitsofthefourpreparedsamples,alongwithaChainofCustodyandanAnalyticalRequesttoParagonAnalytics.Ecology’sanalyticalrequestincludeduraniumisotopes(“ISOUR”)witharemarkforuranium-233(“UR233”).
ParagonAnalyticsusedtheirstandardProcedurePASOP14R9forisotopicuraniumanalysis:“Inthisreport,anyuraniuminthisregionofinterest[inthealphaenergyspectrum]willbereportedasU-233/234[ParagonLaboratoriesCaseNarrative(7December2004)].”Thesampleanalyseswerecompletedon2December.Theresultsincludedaduplicate(“Dup.”)oftheD-Island“1”sampleanalysis,aMethodBlankanalysis,andaMethodTraceranalysis.
AlthoughProcedurePASOP14R9doesnotseparateU-233fromU-234,Paragon’salphaanalysisissharpenoughtoallowcompleteseparationofthe4825keValphaemissionofU-233decayfromthe4776keVemissionofU-234decay.InordertoseparateU-233fromU-234inEcology’salphaspectra,TRACrequestedthespectralfilesfromEcologyon30January2005.Ecologyprovidedthosedatafilesby23March.
Each alpha spectrum consists of a list of counts in each of 508energychannels.Eachspectrumisdocumentedwiththesampledescription;spectrumacquisitioninformation;andcalibrationinformationincluding(bychannel)energy,efficiency,andsharpness(FWHM).Thisinformationallowsareviewertoreplicateanyofthecomputer-generatedanalyticalreportsofradioactivity. Uranium-233hasadistinctalphaemissionpeakat4825keV,withanintensityof84.4%[D.R.Lide,ed.,“CRCHandbookofChemistryandPhysics,”84thed.,CRCPress,BocaRaton(2003)11-184].Thenearestnaturaluraniumpeakisat4776keV,arisingfromU-234decay.TRACselecteda50keVwide,spectralregionofinterest,justabove4800keV.TRACpickedtheparticularchannelsbasedontheenergycalibration information for each alpha spectrum. Then TRAC read the number of counts in each of those
Joint Sampling Process
Step 2: Shovel finer sediments into a 2-mm stainless steel sieve (on right).
Step 3: Empty sieved sediments from collec-tion pan into sample bag. The sample is then divid-ed among the sampling participants.
Rotating two bottles with sediment samples and distilled water to extract colloids from the sedi-ment surfaces.
Step 1: Select a sample site and remove large cobbles and grav-el. This is one of the three sites where the samples were collect-ed upstream of D-Island.
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Uranium-233 in the Hanford Reach Riverbed
channels.TRACusedthesameprocedureasthelaboratoryusedforU-233/U-234,U-235,andU-238analysis,withtheintensityforthe4825keVpeakofU-233toseparateU-233fromU-234.
TRACprovidedtoEcologythefinalbreak-outofU-233on25March2005,fortheblank,tracer,andtheHanfordsamples,includingthebackgroundsamplefromVernitaandaduplicateanalysis,providingqualityassurance.SeetheAnalyticalResultsonthenextpage.
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Uranium-233 in the Hanford Reach Riverbed
A
naly
tical
Res
ults
— U
-233
sep
arat
ed a
naly
tical
ly fr
om “
U-2
33/2
34”
in a
lpha
spe
ctra
inParagonAnalytics“IsotopicUranium
ByAlphaSpectroscopyRaw
DataReport”(7Decem
ber2004).
Sym
bol:
N
m
E
Y
A 2s
S
ampl
e
Sta
rt E
nerg
y
AliquotM
ass
Bas
e C
hem
ical
Act
ivity
Unc
erta
inty
Nam
eFile
[keV
]ChannelsCounts
[g]
Efficiency
Yield
[pCi/g]
[pCi/g]
MethodTracer
URB225L4804.181-185
02.
0.3163
0.754
0.00
0 --
MethodBlank
UB225B
4803.179-183
02.
0.3163
0.754
0.00
0 --
Ve
rnita(B
KG)
UA2541
4802.180-184
02.02
0.2839
0.847
0.00
0 --
D-Is
land
“1”
UA2542
4802.180-184
32.
0.3141
0.815
0.01
0±0.012
D-Is
land
“1”Dup.UA2542D4802.179-183
72.01
0.3015
0.845
0.02
4±0.018
D-Is
land
“2”
UA2543
4806.181-185
52.01
0.2976
0.766
0.01
9±0.017
D-Is
land
“3”
UA2544
4807.180-184
32.01
0.3107
0.804
0.01
1±0.012
Foreachsample:
“StartEnergy”isthelowestenergyinthefirstchannelinthesamplespectrumFile,entirelyabove4800keV.S
pectral
channelsabovethisenergyareinsensitivetothehighestenergyem
issionofU
-234at4776keV.Thisdistinguishes
the4825keV
alphaemissionofU
-233decayfrom
theclosestemissionfrom
U-234decay.
“Channels”isthecountingregionthatcom
prisesthefirstfivechannelsbeginningabove4800keV
ineachsample
spectrumFile.E
achchannelisabout10keVwide.The4825keValphaemissionofU
-233isthuscenteredcloseto
the
mid
dle
of th
e 5
chan
nels
of r
egio
n co
unte
d fo
r U-2
33.
N=N
umberofcountsin“C
hannels”countingregioninthesamplespectrumFile.
Activity(A
)ofeachsampleiscalculatedasfollows:
A=(27pCi-seconds/counts)xN/T/m
/I/E/Y
where:T=LiveCountTime=18,000seconds
and:
I=Intensityof4825keValphaemissionofU
-233=0.844
Uncertainty(2s)oftheactivity(A
)ofeachsampleiscalculatedasfollows(nom
inally,95%
confidenceinterval):
2s=TwoStandardDeviationsofN
countswithinthesamplecountingregion
(withnilblankandbackground)=2A/N
1/2
Toconvertµg/kgofU-233topCi/g:multiplyby9.63
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Uranium-233 in the Hanford Reach Riverbed
Confidence The isotopic separation procedure for the Analytical Results of this report is an ordinary analytical practice.However,thisanalysisisnotpartoftheanalyticallaboratory’sstandardProcedurePASOP14R9for isotopic uranium analysis.
ThereissomeconcernthatthefewalphacountsintheU-233regionofspectralinterestmightbenon-random, false positives. Besides U-233, the other radionuclide having intense alpha emissions in the 4800to4850keVenergyregion-of-interestreportedintheAnalyticalResultsis
Thorium-229: 4814keV(9%intensity),and4845keV(56%intensity)
Thorium-229(Th-229)isthefirstradionuclideproductofU-233decaychain.Ecology’scontractlaboratoryforalphaspectrometryusesTh-229asaquantitativespikeinitsisotopicthoriumanalyses.Therefore,Th-229isaplausiblelaboratorycontaminantinsamplepreparationorotherprocessesinthelaboratory.TherearescenariosinwhichthepositivesamplecountsintheAnalyticalResultsmightbeattributedtoTh-229insteadofU-233.Thesescenariosareprecludedbythezerocountsintheregion-of-interest in the background sample, tracer, and blank spectra.
ThereliabilityoftheconfirmationofU-233inHanfordriverbedcolloidsreportedheredependsprimarily on zero (N) counts in each of
tracer blank background(VernitaBKGsample)
Thesezerosweighheavilyagainstthecountsforthethreesamplesandtheduplicatebeingfalse.Thesethreezerosprovidecumulativeconfidenceofthevalidityofthepositivesamplecountsinthethreetestsamples, ranging from 3 to 7 counts.
The Ecology Department does not presently accept any conclusion regarding the presence or absenceofU-233initsalpharesults,becauseitscontractlaboratory’suraniumisotopicanalysisisnotcertifiedforU-233.Ecologyhasaskeditscontractalphalaboratorytoundertakeaspecialstudyin2006to“showthe‘peaks’forU-233inaspikedsampleandcomparethattothepeaksintheU-234,U-235,andU-238,sotherewillbeaclearunderstandingofhowthelaboratoryisable to determine that U-233 is not present[emphasisadded,Reference1].”
TheEcologyDepartment’sefforttodeterminethatU-233isnotpresentintheHanfordReachriverbedcallsattentiontothestrengthofdifferentbeliefsinregardtoU–233.ManybelievethatU-233ofHanfordorigincertainlydoesnotcontaminateriverbedcolloids;itisamatterofidentifyingwhatevererrorshaveledtofalseclaimsforthepresenceofU-233.Forthem,severalmoreindependentstudieswillberequiredtoconvincethemtochangetheirbelief.
TRAC had proposed and tested a theory that U-233 of Hanford origin contaminates riverbed sediments.TRACestimatedthelikelihoodofU-233intheriverbedat80to95%,beforethepresentstudy.ForTRAC,thepresentstudywasanticipatedtobeanindependent,skepticalconfirmationofanalreadyestablishedtheorywithitssupportingevidence.
Asaconfirmationstudy,the18counts(sumofNcolumnintheAnalyticalResults)inthethreetestsamples plus duplicate are positive 4.2 standard deviations, in comparison to a total of 0 counts in the backgroundplustracerplusblank.Asaskepticalconfirmationstudy,theseresultsarepositive beyond reasonable statistical doubt.
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Uranium-233 in the Hanford Reach Riverbed
Withthisindependent,skepticalconfirmation,beyondstatisticaldoubt,itwouldbejustasdifficulttoconvinceTRACthatU-233isnotpresentintheriverbedasitwouldbetoconvinceEcologythatU-233ispresent.
Thisgreatdifferenceinopinionhasarisenfromcorrespondinglygreatdifferencesinpre-existingbeliefs about the nature of contamination of the Hanford Site and of the Hanford Reach of the Columbia River.Toappreciatethepresentdifferenceofopinion,onemustrecognizehowstronglypresentinterpretationsofdatadependonpastexperiencesandfirmlyheldbeliefs.
Theissuesofwhatconstitutesasufficientdeterminationofscientificfactinthecontextofpre-existingbeliefsisthesubjectofBayesianstatistics.SeeReference7foraninformalintroductionto inferenceandtheinfluenceofevidenceonfirmlyheld,butopposingbeliefs.
Thedifferencebetweenthepreviouslyheld,stronglyconfirmingandstronglyrefutingbeliefswasincorporatedintothedesignofthereportedstudy.Advocatesofthetwodifferentbeliefsparticipatedinallphasesofthisstudy,undertheauspicesofthestateEcologyDepartment.Eachparticipantagreedwiththeprocedure.Therewasaninformalagreementtoaccepttheoutcomeofthisstudy.SamplesplitswereretainedbytheEcologyandtheHealthDepartmentsandTRACfortheirown,independentchecks,attheiroption.
Implications ThereadermightalreadyanticipatefromtheabovediscussionofConfidence,thatthereismuchatstakeovertheanswertothetechnicalquestionofwhetherU-233ofHanfordoriginispresentinsedimentsunderlying the Hanford Reach. Hundreds of thousands of dollars of labor and laboratory costs have been spentonthisquestionsince1999.
The presence of U-233 in riverbed colloids raises a specificconcernforthefuture health of biota in the riverbed of the Hanford Reach. The poster children of this concern are the hatchlings (alevin)ofwild-spawningfallchinooksalmonthatspendtheirfirstmonthsamongthecobblesintheHanfordReachriverbed.
Thisspecificconcernfocusesonradium-225(Ra-225),whichistheseconddecayproductofU-233.Radium-225mimics calcium. Calcium is an element essential for life. Salmon hatchlings are believed to absorb calcium —and hence Ra-225— fromriverbedwaterintheirhabitatundertheHanfordReach.
Radium-225hasahalf-lifeofonly15days.Thus,anyharmRa-225mightdothesalmonwouldoccuronlyduringthealevinstage.TheRa-225mightreducethestrengthofthewildsalmonstock,whichwouldaffectabillion-dollar-a-yearcommerce.
This study raises general concern for the degree that public and regulatory oversight of the Hanford Siteisweightedbypre-existingbeliefs.Reference2reportsunmonitoredradiumenteringtheriverinseepagesfromHanford’s300-Area.Thus,thepresentstudyjustifiesreviewofthedegreetowhichpre-existingbeliefsinfluencethemanagementstrategyandclean-upofthesite.
Animportantresultofthisstudyisthewiderangeofitsinterpretations:betweenpositiveconfirmationofU-233intheriverbedatoneextremetomereanalyticaldatarequiringfurtherprocedural
Salmon hatchling (alevin) - Photo: Army Engineer Corps.
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Uranium-233 in the Hanford Reach Riverbed
evaluationinthelaboratoryattheotherextreme.ThiswiderangerevealshowlittleisyetknownaboutHanfordSite’spresentandfutureimpactsontheColumbiaRiver.
A comprehensive, independent, environmental assessment of the Hanford Reach river corridor is neededtosupportdecision-makinginorderthatclean-upofHanfordSitewillprotectthepresentandthefuture of the Columbia River.
References(hyperlinkedwithinwww.radioactivist.org)
1•Hanford State of the Site Meeting Comments, Uranium-233 —letterbyJayManning,EcologyDirector(December2005)
2•Radioactive Bioaccumulation in Clams along the Hanford Reach (March2005)
3•Uranium-233 Detected in Hanford Reach Sediments (November 2003)
4•Trouble in the Columbia Riverbed —increasing radioactivity under the Hanford Reach (October 2003)
5•Hanford Radioactivity in Salmon Spawning Grounds —quality,extentandsomeimplications(August2002)
6•Questions and Answers on Uranium-233 at Hanford (August 2002)
7•Why Reasonable Minds Differ —learningmodeledonchangingconfidenceinbeliefs(April1997)
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