ML19309G987

Forwards K Drey Ltr Requesting EIS Preparation for Proposed Decontamination

ML19309G987
Person / Time
Site:	Dresden
Issue date:	02/26/1980
From:	Stevenson A SENATE
To:	NRC OFFICE OF CONGRESSIONAL AFFAIRS (OCA)
Shared Package
ML19309G980	List: ML19309G979 ML19309G987
References
NUDOCS 8005080103
Download: ML19309G987 (12)

Text

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'.s) s 8 0 0 5. o.8 o !c>3 February 26, 1980 a-TTk1Cb MkC(CS MCTTC(C c'SirI': St - ::-

-: Ci: Sr:-9 C%:e E A e; o:r. s: r D.C. E313 LTili: Uy4 C'A;.V Respectfully referred to:

Congressional Liaison Office Nuclear Regulatory Coanission l

Nashington, D.C.

20555

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2 ::

Because cf the desire of this office to be responsive t: all inquiries and corrunications, your consideration of the attached is

~

requested.

Y:ur findings and vier',, in

.,2 duplicate fors, alcng sith return cf the enclosure, cill be appreciated by

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Mw, 9.+4,

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U.S.S.

j For= ?2 l"

Janua:y 9, 15 0 M18 T O :,

ts*:e-t Ji-y Carter,~and to Pesses. Jchn Ahearne (Chairman, Nuclear Fe;.iat:ry Cc missien), Ocuglas Costle (Ac.inistrator, Environmental Prctection 4

Agency), Jacco Durelle (Chair an, Illinels F:llution Centrol Board) Charles 4[

M ean, Jr., (Secretary, Department cf Erergy), Charles Percy (U.S.-Senator frem lilinois), Adlai Stevenson (U.S. Semater % - ft1Tels), William Scott (Attorney General of Illinois), James Thompson (Govenor of Illinois), and Charles Varren (Chairman, President's Council.on Environmental Quality) e f

FPp: Kay Drey, 515 West Point Avenue, University City, Missouri 63130 4

l Next rent. an ex;eriment -- replete with knvwn and unknown hazards -- is scheduled to take place at cut nation's oldest nuclear power plant, no more than thirty highway miles

^

south-est of Chicago's suburbs. Commonwealth Ediscn plans to flush chemicals through its Dresden-One reactor te try to dissolve and remove an accumulation of radioactive i

corresicn procucts (crud) f rom within some five miles of convoluted piping. Citizens have written to the Nuclear Regulatory Commission and the Department of Energy asking that a full Environmental impact Statement (EIS) he preparedi at least one filinois l'

organization has asked for a public hearing. Instead we have been hearing fcr months now that if an Els is ever to be written, it will be af ter the fact, not before.

On March 19, 1979, I sent a copy of the enclosed letter to you (or yourpredecessor) ll listing some of the questions that seem to me to be undenlably worthy of examination by independent scientists -- that is, by scientists other than those from one of the federal agencies, private chemical or nuclear corporations, research laboratories, universities, or electric utilities which have already committed manpower and/or financial

' resources to this first in a series of proposed experiments. ' In addition, i filed a more formal request for an Els on March 30, 1979,with the N*C and DOE. The DOE answered, saying that since they were not expending any fiscal year 1979 funds on the project (their 58.2 million subsidy was apparer.tly contributed to Commonwealth Edison or Dow 4

l Chemical prior to 1979), they did not feel obligated to write an EIS. The NRC answered that receipt of my request had been appropriately acknowledged in the Federal Recister, j

l believe the other citizens who wrote received similar responses.

1 j

That is, to date there has been no public hearing, no EIS, and no opportunity for 4

incepence7t scientists to study the proprietary decontarination brew cr to reflect on j

the inmediate anc long-term impacts of its use.

The project is proceeding under the supervision and aegis of the people most committed to and ' dependent upon its success.

i To allow at least 10,000 to 20,000 pounds of chelating agents (complexing solvents) to be flushed through the Dresden Unit One reactor -- a 20-year-old hulk of co' roded, r

irradiated, brittle, leaking, man-mace, man-coerated metal gadgetry -- and to bring cut into the :leschere an estimated 450 to 1,100 pounds of radioactive wastes o4 the basis of assura ces f rcm men who have no alternative solutions to the permanent sh'utdown of this : rot typical reactor seems to me to be clearly contrary to the letter and intent j

of the National Environmental. Act of 1969

t is also just plain fri;M ening, tm Please recall that chelates have been found to be the very agents responsible for i

the unexpectedly rapid migration of radioactive wastes out of the Oak Ridge. burial trenches into the unprotected environment. Chelates also make It easier for radio--

active materials to be absorbed by roots of grass and vegetables - potentiaMy, then, to be further concentrated in the flesh and milk of animals when they eat the grass or plants. The NRC says that gravity and Oak Ridge's high water table are responsible l

for the liquid westes' mobility there. An ERDA (DOE) study, however, by geochemists aM a.

i w.e# f ron Princeten Universi ty, Oak Ridge National Laboratory, and Battelle-Columbus Labor-atory say chelates are responsible. This latter study also says that chelates are unexpectedly persistent in the environment. That means that the radioactive wastes bonded cnto them at Dresden will remain uncontainable end therefore immeasurably more hazardous for cecaces, perhaps for centuries, perhaps forever.

Even if they're buried as proposed in Nevada or Washington -- in areas which today are climatically dry and politically agreeable -- what assurances do we have that the future will mirror the past?

Anc what rlgnt do we have to assume that it will'8 Would you er a me cer of your staff please find out whether an Environmental -In=act b

State ent is to =e prepared before the Drescen experiment, after, or never?

Thann yo..

Enci:s.res '.'

• cans,. J.L., Crerar. D.A. and Duguid, J.0.

Scierce, 30 June 1978, Volure 220, p:. la77 - 1a81.

x etter t: ares ee,t :arter et al.

aren 19. m s.

2

19 March 1979 7 siden: Jinty Car er, and to Messrs. Douglas e s t: e ( Admini s t rat or,

Envirennental Protecti:n Agency), Jacob Dumelle(Chair:2n, Illinois 7:.;u:!:n Centro 3:ard), Jessph Hendrie(Chair:an, Nuclear Reguletory C:::ission), Charles 7ercy(0.S. Senator fro: Illineis), James Schlesinger (Se:re:ary, Depar:ren: ef Energy), Willia: S:o::(A::orney General of Illineis), Adlai S :e v e n son (U. S. Senator from Illinois), James Thompson

(;:vernor of Illineis), and Charles Warren (Chair:an, President's

::11 on Envircn: ental Quality)

Kar Drey, 515 Wes: Poin: Avenue, Universi:s Ci:y, Missouri 63130 FlIA TOR AN ENVIRONMENTAL MPACT STATEMENT CS A MAJCR TEDERAL ACTICS PRO-

IED FOR !H:S SPR:NG, 1:'9, IN ILLINOIS:

a iae U.S.

Department f Inergy is presently contributing 58.2 million toward the first of a series of decontamina:ien experiments designed :o disselve and flusn cu: radioactive corrosion pr:due:s frem nuclear reacters. In April or June (?), 85,000 gallons of a proprietary Dew Chemical solvent are to be flushed :hrough an estinated five miles of piping for 100 h urs within our nation's oldes: active commercial reacter(Coc=onwealth Idison's 200-megawatt Dresden plant, Unit one, near Merris and Jolie:, Illinois, on the Kankakee River).

This selvent may be che:ically similar tc, even identica; with, the vert ec: pounds which have been found tc be causint :he unexceetediv rarie migration ef radienuelides out of the Oak Ridge burial trenches anc possibly into the human food chain.

The clait ec tained in a letter I received last centh from the Department of Inergy that there is "reasenable evidence that it(the solvent) will not ribute tc the escape of the radiese:ive material, nc vill it cause nigra:icn cf radioactive substances through the envirentent" is not con-incing. Once :he Dow Che:fcal solvent has bound the radioactive =aterials.

e may ; se all hope of keeping those substances isclated frcm the biosphere.

' have 05:ained infor:a:icn and suggestions frc: professers of geochemistry,

ysics, biophysics, biolegy, biochemistry anc radia:ien oncology. Every one

f ther is as concerned ab:u: this experiment as I a.

They have helped farrulate(and explain) the cuestions that follow, and all believe that an environnental impac: assessment is imperative. Tc qucte one of the men fr : a le::er da:ed March 9,

1979:

"I think it is unacceptable that the DOE assure ycu that their chelating pre; ara: ion is envir:n=entally safe and, at the same time, refuse to divulge the nature f the material. We still kn:w relatively little abcut the movement of radio nuclides in the envirenment, but there is increasing evidence : hat natural ligands =ay ;ontribute to the process.

I should think tha: one would need to take care that the artificial ligands provided by Dow would not enhance the ecbility of nuclides in the biosphere and result in their concen: ration in the food chain."

lefore :his action is uncertaken the public is entitled to the assurance that rhysical and biological scientists whc are not financially and/or emotionally

ritted to :his project will have studied questions similar to these which M :llow, and will have conclusive evidence that the proposed Dresden experiment

an be perfcrmed witheut jeepardizing the human environrent. If not, the

roject should not proceed.

Firs, is it pessible : hat an envirenmental impa:: assessment and a negative declara:1cn have already been writ:en regarding the proposal to de::::a=inate Dresden Unit One? I have asked this question several times of the DOI, but have not received an answer. If an assessment was made, whi:h individuals of the Department of Energy made the decision : hat t r. i s

jec

will not affe

: :he quality of the human environment, and there-fore did not require an environmental impa : s:ateren: under 40 CFR 1500?

That is, was a nega:ive declaratien made by the DOE, and if se, by whom and when? !s a :cpy available? Did it address the fe;;owing questions ?:

What d :ield er labcrat::v tes:s demonstrate tc be :he =igration potential Of rati:a::ive vastes en: rapped in the De. Che i:a; selvent, assuring seme

-ere :: es: ape fr:: :uried containers in:: :he envir:nnent?

A:::rdin: :: an arti:;e rutlished in Scien:e. re:

200, 30 June 19?3, by

!effrey Seans, David Crerar and James Dutuit, che;a:ing agen:s were found

. :e :na verv su:s:an:es resp:nsi:;e for the :::!.;:a:ien ef radi:nuc;ide, em mMem 4 e

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3::- dis;:ss; ;its and ::en:hes in the Cak Ridge Nati:nal Laboratory. In a ; s::::a *. :::: uni:sti:: ft:

Dr. Crera;, the envir::sental i=p11 cations t

a:e ins::ited as foll:vs:

"2hile chelates a:e used because of their powerful met'al-binding

er

1es, i

is this same cha

acteristic whi

h =ay have undesirable a:vir:: ental c::s equen:es. Ic; example, IDTA, which is used in gy:*et; decontasiestien operations, is causing the =igratica of some

-: f::= inter:adia:e-level liquid vaste disposal pits and trenches g

g in the Cak Ridge Us:ie:a1 Laboratcry burial grounds. Because it f:::s ex:re:ely s ::rg cesplexes wi:n rare ea::hs and actinides, j

i I::A and si:11a: : tela:es may aise be :entribu:ing to =chilizatica

f these radionue; ides from various :arrestial radioactive vaste l

f fis;ssal sites a :u-d the country. EDTA is relatively resistan: to de:: posi: ion by :adia: ion, ther= ally stable up te about 200-2508 C, i

and rather slowly hiedegradable. Consequently, it is persistent in i

he a vironment. I: deed, the p;esence of significant concentra:1cas of ID A in 12 c ;f year old radioactive vaste at ORNL attests to i

1:s persistenc e. Therefore, whe:ever EDIA and similar compounds have 1

bee: introduced is:: the natura. environ =ent, the aqueous transport j

of ::ansitien metals, rare earths, and transuranics, which character-is:teally for: the cs: stable co=;1 exes vi:5 chelates, will be expec:ed :o oc:ur.

1 Jegradation ra:es of all three chelates (NTA, IDTA, and DTPA) were net rapid enough, even under ideal laboratory conditions, to preclude cen:ers about thai: release to the environment. Heavy metal schilizaticu can occur at extre=ely low chelate concen: rations, 1

as vitnessed at ORNL. 31odegradation, if slow or incomplete,

=ay' j

be s: inadequate bar:1er to their various undesirable environmental i

Des::uction of chelates by ther:a1 or *Le:1 cal =eans c:: sequences.

=

(su:h as ozonati:n', prior to environmental diswar,

appears to be

uch :::e efficies: :han biedegradation after di.narge."

2.

F:r hov many years have radioactive corrosion products, bonded with the p:c;csed Dov Chemical s:1 ents, re=ained fret of water after being solidified by the Dow Che:ical pcly=e process?

a i

Acc:: ding to Dow Chesi:al's publication entitled " Solidification ? ccess j

f:: lev-level Radioac:1?e Wastes", (Tor: No. 173-1026-78), only a fev 1

dese:1ptions of the sclidifi:stic: ;;ocess, whi:h ! understand is to be used f:: the 0:esdat vas:es, are included:

js "The Dov Solidifi:ation Process consists ef_ the ecmbination of a ti:dar -- a modified vinyl es:er resin -- with small amounts of a 4

l catalyst and a p:::c:er. The process encapsulates the low-level-radicac:ive vastes it:o a stable, solid and homogeneous matrix.

4 j

The ?:ocess, using polymer che=1. cry, dictates that it must solidify E

aqueous and slu::7 wastes, including ion exchange resins, evaporator 5:::::s, spen: da::::atination solu: ions, and filter sludges.

Tha Ocv Process solidifien radioactive vaste vi h no free liquid.

The Jov defizi:ic of ' free liquid' is liquid in er on the stainer upon completion of solidification l

spe:ime: or in the :

af:e: 3-7 daya of aging."

i i

a.

Has the Dev s:*idificatica process been tes:ed on reac:or l

sion ;;:du::s compa:able to those which will result fro =

the Dresde a:; art:ent? That assurance is there that the en-

apsulated vaste is going : be 1:v-level?

b.

When did 0:e :hemi:a1 firs develop its' solidification process-i l

f:: 1:v-leve". radi:ac:ive was:es? Tha: - is the ic gest duratica I

eriod fe

::e :f 1:s ":ctoliths" c: matrixes -- tha: is, h o w lo.w*

has such a s:lidified

v substan:e remained free of liquid?

Tha: vould b e :he 1::;-:er stability si.he solid polymer ever a ;erici f th:usands of years?

Jhs: is :he les:: rate-:f :he.';;;7 er unfe; burial ::ndi:icas, ::

the ;::en:

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f:: diffusi:

and ra" ease :f an:a;sula:ed rati:-

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During :he eva;: a:1:n s e;. is :he selvant vola: le, and if se, will an ion exchange resin ::tple:ely scrub :helated radienuelite fr:m the evaperate? (; a: : '. d b; cne person : hat his experience indicates it wil. no:).

T:: hcw =any yects have the barrels designed "or burying the solidified wastes been found to re:ain resis:an: te co::teien fro be:h the ;;:p: sed contents and fic: surrouncing envi:on= ental impac:s?

a.

According to a let:e: I re:eived fro: Mr. ?aul Petti:(ligh: Wate:

Reactor Secti:n, Oivisien of Suelear ?:ver Devel:pment. 00E) dated Tebruarv 6, 1979, the solidified was:es f::m :he Oresden experiment are te be shi;;ed in drums :o a com:ercial isw-level waste disposal si:e. Since additional wastes are ne longer being accepted 2: the nearby 5heffield, I1;inois burial si:e(in fact, the 11:ensee has jus: va'ked avsy, with :he NRC in hot pursuit),

will the was:es be shipped := Nevada, Scu-h Carclina, er Wash-ingten? Were the dru:s designed :: ::: ply with the Oe;ar::ent of Transportation's packaging and shipping regulations for 1:v-level or high-level wastes (49 TR ?ar:s 170-173), or to comply with the NRC transi: regulaticas for fissile materials (10 CTE 71 and 73)? And/or were the drums designed for indefinite burial?

b.

What is the esti:a:ed lifespan of :he barrels? What precautions are gcing to be taken a: the life-end of :he barrels to ensure continued containmen: of the residual radioac:1vity? Have any

=e:als been found that will resist the corrosive ac: ion of the proposed contents for even a decade? Is there ap: :o be any chemical reaction between the compounds going inte the barrels and the materials of which the barrels are ec= posed?

c.

In the June 30, 1975 Selence arti:le, Dr. Crerar and celleagues describe :he accelera:ec dispersal threugh the g:cundwater and the increasec uptake by rege:ation of the radi:nuclides when bonded to nonciedegradable chelates. If the buried drums with the solidified Dresden effluent were to corrode and the matrix were t: :::e in:c contac: with wa:er, would :he radionuclide-chelate c:mplex not become se;uble again? Could this solu: ion then rigrate :hrough the enviran=ent in the same manner found at the Oak Ridge burial si:e?

d.

If chelates are to be used, :an they be deactivated :.er= ally, chemically, or b i s.' c g i c a l z y before evaperation and solidifica:icn?

f.

Is it pcssible tha: any of the scivent with or withou: dissclved radio-nuclides may remain after the principal effluent anc first rinse water have been removed for evapora: ion and solidification -- and then be flushed in:o the Illinois River? If so, might the radienuclides absorbed oy the river's sedimen-usar the plant's cooling water outdall in years past become resuspended and migra:e into the reed chain?

a.

How much radioactivity and residual chelating agent are expected in the firs: rinse? How can" addi:ional rinses will there be?

Scientists have told me : hat they did no: :hink that chelated, radioactive metal ions would be removed by a de=ineralizer; although domineralizers nave a high affinity for naked ne:a; ions, I have been inferee: that they generally de no: receve chelated for:s. Or will :he :heit:ing agen: perhaps be :harged, and :hereby be rencvable 5"

the de:ineralizing step? 7e:;;e with whom I have spoken see: surprised :: lea:t tha: the ;urift:stic.n af the first rinse -- : Se ren:va; :f :ne residua; e n e.' a : i n g agen: 1 and : hela:ed ne:a; i:ns -- was :: :e c:ne w :t a desinerali:er.

3 What is the ex;;ana:i:n f:: this a:;aren: departure fr::

adi:1:na; ;;ac:i:4?

According :o Mr. ?e :i:'s le::er :f Te:ruarv s, 19??, ':he f:rmu.a:::= :f -he ::.

heri:a; sc.ven:

1.

kn:vn :: COI staff bu: is pr::e::e: f::: re; ease :: :he publi: br a ;r::rie:ar" gree en:." 3:.'ven:s usei f:: :e::::2-ira: 1:- turreses 6:

a:; ear fa::. :ies nave :eer ins::1:e: elsewhere.

ve"er. :

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00E, 1:v and Cce::nvaalth Iiisen representatives as bein; "che*ating agents" (pren unced key-lay *

) -- that is, a che:ical cespound(typically crganic) capable of ferring clavlike =ultiple bends vi:5 a =etal ion. Typically these agents are also non-irrita:ing to skin or eyes, a characteristic of the solvent which Mr. Fettit happened to =entien.

Assuring the components cf the selvent fit the definitten of a chelating agent, is there any likelihcod that there vill be enough residual after the primary effluent and' firs: rinse water have been removec, that some =1ght be flushed in:e the Illinois River along with future routine releases of the ccclant water? (The ccelant-water discharge canal empties into the Illincts River at the confluence of the Des Plaines and Kankakee Rivers a: Illinois River Mile 272.4). Hew tightly dcas t'.e selven bend etals? That is, if sc=e were to pass through the sedi=ent near the canal's discharge point, =ight it leach ou: addi:ional radionuclides which have accumulated in the sedi:ent near the outfall? Or if it is a relatively weak agent, =ight the sediments attract radioactive retals out of the chelate solution. :hereby increasing the arount of radionuclides in the sedi:ent and the pctential for further conta:ination of the benthos? (The E?A repor: entitled " Radiological Surveillance Studies at a 3 oiling Water Nuclear Pcver Reactor", BRH/ DER 70-1, describes the centents of the Dresden Unit One liquid vaste effluents during tests in 1967 and 1968. Two later :o:panion studies at reactors in Massachussettes and Connecticut describe the significance of the concentration of racicnuclides in the sedi ents).

6.

What will be the i= pac: ef the sc1 vent on the future safe operation of the Dresden plant?

According te the hock, Oangereus preperties ef I n d u s t r'i a l Materials, by 5.

Irving Sax, published in IEt3:

"One fallacy in the initial concept of stainless steel or other

'impervieus' surfaces is that they are truly i: pervious. This has been shown to be false. Stainless steel after one vigerous cleaning is found to deteriorate in that more and more sterial may be absorbed er adsorbed anc retained on the surface. Successive cleanings have been fcund to bece=e cre difficult and to require scre vigorcus me:heds cf decantacinatien." (p-149) a.

I understand that the NRC is responsible fer making certain that this project will net cceprecise the integrity of the reac:er vessel and its parts. What assurances, however, does either the NRC cr the DOE have that this =assive cleaning effer; vill not increase the surface fouling of the reactor syster in the j

future, causing an acceleration in the buildup of crud in its

=any nooks, crannies and blind holes? Will even strenger chelating agents be needed at Dresden Unit One for future decontamination effor:s, assuming the stainless steel properties quoted above frc: the Sax beck are correct?

b.

Could an acceleration in the rate of buildup of crud after the decon arination prcject increase the poten:ial for pipe cracking or rupture? And aise increase the radiation hazards to verkers?

'J h a t assurances are there tha: the men who participate in the Dresden deconta=ination experimen: vill net suffer fro: exposure to the c::bina: ion of the solvent and the radi: active esterials suspended in the selven: in either the aquerus er gasecus f:::s?

One cf the possible reas ns for the increased incidence of leukeria and

ancer at Por:srouth and c:her naval shipyards which Drs. Thomas Nafarian and Theodcre Celten =enti:n in their c:::unica:icn published in Me lance:,

May 13, 1975, is that: "Other fac: rs(asbestos, stoking, industrisi s elvent s) =ay have interacted synergistically with radia:1en :: :suse

=cre dea:hs fr : cancer and leukeria than radiation alene vould have caused." (es;hasis added). I reali:e that one of :he prirars reas::s fer trvin; :: devel p an effe::ive de::ntamina:ist p S:ess is :: re:.:e the a:cumulati n cf gar a-emitting cer sien p;rdue:s whi:n ir turn :1 se hi;h ra.iati:n fie;ds within pera:in; nu:les p:ver :lin:s, 2n: : r e r e b '-

ne:essitate :he airing Of ex:essive numbers f reprir arf 2 -: erin:e

- as s.

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5 a.

A:::: ding :: a letter dated March 13 frc= Mr.

A.

David A:ssin(5/ste: !: clear Research Inginee:, ". e=envaalth Edis:n),

thir:*/ verkers vill be needed during the ;:esently ;;epesed i;C-hour p:::e:: And although eas : 10 b> Mr. Paul Petti:

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f the 3cv s: ven: itself during :he dec: :a:Ina: ice peratien, wha: hazards say i: pese to uc:kers when it is in c::bina:icn vi:h radica::ive =aterials?

hat p ::edures are to be taken :: rake :ertain that :he radiocu:11de-: hela:ing agent is :::al'.y :entained and will not in fa:: ::=e in contact with the V::kers? What is :he radiati:n d:se expe: ed per hour at e *: e cater f:c the rea::cr ::ntainmen: vessel, the effluen: piping, th6 avapc:stien and solidificati:n equipment, and the dru:s preparatory :c and during shipping? What shielding vil'. be erected to protec: r n, workers?

e are cuesti:ns of prof:und 1 port. To prs eed vi:h the Dresden experiment

-i.e they ttain unanswered wculd 'e agregicus ic'.y For the safe:y of

re pub;i: and the workers, and for the pre:ection Of cur country, can ve de=anc :ha: a full environ = ental impae: state =ent be prepared

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mately 3.4 u 10-'Af (this studyl. Actual K., values for '"Co in burci ground wa.

ters are therefore signi6cantly lower than the theoretical value for neutral systems containing no EDTA and are somewhat greater than the expen~. ental value for neutral systems tentaining 10-$Af EDTA.

The importance of sediment sorption Migration of Radioactive Wastes:

• • P"'i'F ' ' #

" " d' "" # d* *i8

tion rates within geologic substrates has Radionuclide Mobilization by Complexing Agents been rnodeled by Marsity et of. (9). Us-ing variables such as K, rock per-Abstract. lon exchange, gelfiltrution chromatography. and gas chromatography-meability. and hydraulic gradient, they x

?

mass spectrometry analyses hm e ' demo'nstrated that ethylenediaminereiraacetic calculated the migration rates of "*Pu acid (EDTAl. on extremely strong complexing agent commonly used in decontami-huried at the bottom of geologic forma-nation operations at nuclearfacilities. es causing the low-level migration ofcobalt-60 tions 500 m thick. The results show that

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from intermediate-level liquid waste dispos vi t>it and wnches in the Oak Ridge

"'Pu with a K, of x 10'.1ypical of a Nation.:1 Laboratory burial grounds. Becos

. wms extremely strong complexes chemical setting devoid cf complexing with

,v hs and actinides. EDTA or simd + 'helates may also be contributing to agents. tock fractures. and similar fac.

.the r~ tituation of these radionuclides from va.ious terrestrial radioactive waste tors tending to reduce sediment adsorp-burial sites around the cougy.

tion. will not migrate to ground level un-til more than 10' years after burial, the From 1951 through 1%5. intermediate-pacity of the shale and soil for the radio-migration rates being slowest in those level radioactive liquid waste at Oak nuclide.

geologic forma:i3ns with lowest per.

Ridge National Laboratory (ORNL) in it is this last factor that is of pr icipal meability. With a half-life o' 7s 400 Oak Ridge. Tennessee, was disposed of concern in this report. The isotope "Co years. Pu would essentially be compiste-in seven different seepage pits and has been found in concentrations up to ly decayed by the time of contact with trenches UI. Since 1944, solid waste at 10$ dpm/g in the soil and up to 10' dpm/ the surface environment. At the other ORNL has routinely been buried in shal-ml(450 pCi/ml)in the water in areas ad-extreme. in a chemical setting character-low trenches in six different burial jacent to seepage trench 7 and in lesser ized by no sorption (K, = 01. Pu would grounds C). Ground burial of radioactive concentrations in the vicinity of trer ch $ reach the environment in 6 to 14.500

~

waste is an effective means of di posal if and pit 4 (Fig.1). Traces of various al-years depending on the permeability of the radionuclide can be copfineo to the pha-emitters such as isotopes of U. Pu.

the geologic formation (9). That is, in the geologic column through geochemical Cm. Th. and Ra have also been detected most confming formation Pu would have processes. Although the Cnnasauga :n water or soil from the area around decayed about only one-half of one half-shale the predominant bedroc' of the trench 7 C-1). We show here that "Co is life before it reached the surface. In for-ORNL bunal grounds, has an extremely transported in the groundwater from the mation6 of low to moderate permeabil-high adsorption capacity for most fssion trenches and pits as organic complexes.

ity, migration of Pu over 500 m would by products, trace quantities of certain A portion of the migrating "Co is ad-have occurred in only tens to several radionuclides are migrating from both sortied by oxides of Mn in the shale and hundreds of years, the movement being solid and liquid waste disposal sites O).

soil H-6). Additional evidence suggests four to five orders of magnitude-more Several factors have contributed to the that some U is migrating by the same rapid thriin the situation K, = 2 x 108 radionuclide mobilization. One is that mechanism.

In the Oak Ridge setting. the adsorp-the annual precipitation at ORNL. over The following experimentally mea-tion capac;ty of the Conasauga shale for 127 cm, is greater than at any other ra-sured distribution coefficients (K,) illus-inorganic forms of Co is very high.

dioactive waste burial site in the country trate the pronounced effects that organic Hence, mobilization of this radionuclide Cl. As a result, water infiltrates into ligands have on the adsorption capacity in the absence of strong complexing trenches at a faster rate than it can be of sediment for trace metals. We deter-agents, rock fractures. and other factors dissipated and mixes with the waste. In mined that the K, values for "Co in tending to reduce sorption would be neg.

addition, groundwater levels are com-weathered Conasauga shale at pH 6.7 ligible. However, in the presence of paratively shallow and a high-density and 12.0 were approximately 7.0 x 10*

strong chelates, rock fractures, and oth-surface drainage network is present. and 0.12 x 10' respectively. In the pres-er factors tending to decrease sorption.

There is also an abundance of fractures ence of 10-4f ethylenediamineletra-the K, is drastically reduced and mobili-in the underlying rock, which diminishes acetic acid (EDTA) the K, values were zation rates may be, accelerated by sev-the rock's sorptive. capacity because the reduced to 2.9 and 0.8 (7).

eral orders of magnitude, exchange sites adjacent to the fissures The actua! K, values calculated from A compilation cf selected radionuclide are saturated with the exchangeable ions "Co concentrations in soil and water analyses for filtered water, weathered in the waste C). Finally, the presence in from various wells in the ORNL bunal Conasauga shale, and soil samples col-the waste of complexing agents such as grounds are similar (8). The K, values for lected between June 1974 and June 1975 organic chelates used in decontamina.

"Co from wells in the vicinity of trench 7 from wells in seeps adjacent to pit 4 tion operations and natural orgame acids range from approximately 7 to 70, aver-trench 5. and trench 7 is given in Table I from the soit promotes the formation of aging about 35 (see Table 11. The pH of 00). Locations of pits. trenches, and strong complexes with certain radio-w ell water ranges from 6.0 to 8.5 F). and sampling sites are shown in Fig.1.

nuclides that reduce the adsorption ca-the EDTA concentrations are approxi-A surprising initial observation, first SCIENCE. YOL. W. 30 JUNE IQ r8n407378Wo.icsm.50o Connsht e 197 AAAS IC

o erse enorgame groundwatcs somponents in edes to difierentiate between 'he '

t ip groundwater did not readil) eseh.mpe men.n sulf ate. nmale. bseat bonale, e.o.

sadionuchde mobsh/mg ellech of 9 n.

with cation.csenange resins (RcA)n 101.

honate, chioside. orthophosphate, and therse ehelates of low molecular weight

~ Na

• form). Data from sescrat samples es en stronger lig.inds such as p> sorhos-and 'those of hurae substances of higher show that only about 5 to 10 percent of in.o e and metaphosphare w.n in.

molecular w eight, we fractionated the Co could be adsortied by the resin.

uthesent to produce the ion.eschange groundwater samples. using pel filtration the other % to 95 percent being retained c.utmn richasior of ""Co obsen ed in the chromatography IGFCI. a procew w hich in solution as a tightly bonded comples.

samples 11/). However. in the presence separater. solutes according to size (12L

!! seemed apparent that whatever agent ef ser) low concentrations fl0 'M and Since most weak inorganic. metalhc was responsibie for this clieet was aho iew of multidentate chelating agents corrplexes are sorbed during the GFC preveming corrplete adsorption of cer.

uch as diethylenctriaminepentaatetie procew. the presence of trace metah in a fain radionuclices by the Conasauga acid (DTPAh cyclohexanediammeteira. given fraction of an clution profile dem-shale and soil.

acetic acid (CDTAh F.DTA. and aho onstrate, an awociation between the Subsequent ion-exchange anal) ses r.atural organics such as humic and fuhie trace metal and a ligand in that fraction

)

that we carried out demonstrated that acids. "Co resisted adsorption by the (13.14 h the strength of"Co complexes with pos-resin.

Elution profiles of a concentrated f

groundwater sample from location RS7 near trench 7 for Sephades gels G 10. G-Tabic 3. Selected radionuelide analpes of weattered Conasaup shaic and soil and filiered

15. and G-25 are illustrated in Fig. 2.

waver samricsj0.'.2 gm) and corresponding K. vaiues from melh in the vieiruty of pn 4. trench Each of these clution profiles contains

5. and trench v.

tbree fractions decreasing in molecular w,,,

Aqueous Aoucous Adsorbed weight to the right. The blue dextran g

Date 8H "Co "Co g.*Ch.

peak coincides with the fraction of the code idpm/ml) idprn/mfl idem /ml) sample having molecular weights above RS3 24 6 e 1975 12M0 90 0 NAt 700. Between 90 and 95 percent of the RS5 25 June 1975 1290 39.0 NAt

• • Co and 70 percent of the U present in RS7 26 June 1974 3050 6A9.02 43.700 65.3 the sample are correlated with the T7Ill 31 July 1974 3930 5th 0 86.900 32 6 T712 31 July 1974 3450 547.0 2x.600 52 3 midd!< fraction. which represcrits a T7-l)

> August 1(r74 3740 P l 6.0 24.500 30.0 group of organics with molecular w eights T7-14 31 July 1974 two 227.0 6.600 29.1 less than 700 plus the Na'-salts of sever.

T'7 15 31 July 1974 2090

15) 0 1.%0 6.9 al polyvalent anions. Between 5 and 10 RS9 24 June 1975 3130 t60,9 N At percent of the "Co and 30 percent of the

'see so m oianc.lped swaier trorn Ps: ao comm 7.5 p.ns per haaon or u m) nerceni =u U are associated with the fraction having (k

c et R molecular weights above 700, and no h

e s0 t

• • Co or U are observed with the smallest molecular weight peak. which through

[7'

(

(

[

infrared spectrophotometry was deter-0 200 400 soo int I

mined to be comprised principally of NANO and !<aC). Reliable Pu analyses 3

.. sue 1

of the GFC fractions could not be ob-tained.

5[3 6

Infrared spectrophotometric data in-Rss g

dicate that the large molecular weight

y[

fractions associated with minor "Co and

[

U transport are humic substances. Be.

Rs cause groundwater in and very close to

/1 a

the trenches is typically low in humic h

content. we believe that humics are not 3

/

l 850' major contributors o radionuclid ' trans-

[

[

port from the trenches. On the coctrary.

RS2 2.

Rs5 we believe that humics become associat-a

[

ed with radionuclides some distance p3, l

7 f-from the trenches. particularly in the f

4 Rs7 Seeps where groundwater humic con.

I y [I

]

centrations are the greatest.

Rs5

'j as3 After we had completed the GFC frac.

\\

,g tionations, the identities of comycxing

/--

agents in the major radionuclide-bearing C'"'

~

p fractions were still unknown. We sus-pt pected that the e materials were synthet-

" '" I ic chelates, but humic substances of f

iM/

lower molecular weight could not be Fig. I. Loc.non of sm.itl scers unocidied *Hb re

1. 2. 3. and 4 and trenches 5. r.. and 7

1. "*I

""I '. E

1. ' E "

Contours re in feet ifroen ulj. ICounesy of 0.4 Kee,:e Nunnal 1.aboratory. O L Ridge. Ten, siew of their greater acidity and metal-neucel complexing capacity relatise to the spe.

14 3 SCIENCE. VOL.. :(D

aes of hegne* rwiectil.o u right rif L Samp6e C5 I td'Co h

_ _ _ o,ggn,c c,een

%t estracted the rmddle (il C frav tion wri5 c.*nt.oned the largest radio-clide concer.tr.itions with chloroforrn f,p e i

~

nu

\\

G lo l

8'*"*"

i

_ f !, g[k

\\

to remose co cpounds that would inter.

l lete in tne suscauent analpit All the j I ll '

radionuclide remaened in the aqueou-

/

'r h {i

=

e phase after tr.e chloroform extraction.

(

'N

's.,,

The auueous lay ers were then esapo.

3 j, 3

rated 1o drynco and methylated to facili-b 7, b [/

tale gas chromatography-maw spec-

[

G 15 lh.

s's trometry (GC MS) analysis (/61.

The GC pro 6le for the methylated

[ / l ',\\

l1

'f' l1

,,\\

if fraution is inu trated in Fig. 3. We used

~

8 3. /!

MS to demo. strate that the domirant 0

/

\\

f peak represents the tetramethyl ester of

/,

_g

',,,t..._,'

' s,___

j,j EDTA, an extremely strong chelate i

comnionly used in decontamination op-

.,' /\\

erations at nuclear facihties t/h.

i c.25 Through use of an internal CDTA stan-j'i

, N

dard, the EDTA concentration of this

/ \\

l\\

/

sample has been calculated to be ap-j\\

l

\\

/

i proximately 3.c x 10-'Af; EDTA has also

, s,

\\j

\\

• e been detec!cd in samples RS3 obtained

/#

' )..

\\

near pit 4 and RS9 near trench 5 t/81.

'l'

---

- ^

Other constituents detected in trench

\\-

4'o 5'o 6'o io s'o 9'o 100 lio leachates include palmitic acid. phthalic Eiution volume tml) acid (191. and other mono-and dicarbox.

F ;. 2. The GFC cluison pro 6tes of groundwater from RS7. a sm ll scep cast of trench 7 [from-ylsc acsds. uhach are much weaker com.

(131). ICourtesy of Lommdoxy eruf Ocwweruphy. Scuttiel plexing acents than EDTA. he concen-trations of strong chelates similar to EDTA, such as nitnlotriacetic acid (NTA) and DTPA. are below the detec.

tiori limit of this analysis, which is up-proximately 5.0 x 10"Af. Because NTA is 'biodegradabic. it would not be ex.

pected in signi6 cant concentrations in the groundwater even ifit had been origi-nally present in the waste (20). Both DTPA and otner rnultidentate chelates

~

were used only sparingly in decontami.

Tetramethyl ester nation at ORNL during the 1950's and of EDTA 1

19&s and consequently do not appear j

10 be signi6 cant in the radionuclide rno-bilization at this site.

We thus reasoned that EDTA is the Unknown, probably the dimethyt dominant rnobilizing agent in samples ester of a dicarbonyisc acie RS7. RS3. and RS9. A minor portion of

[

the mtgrating "Co and U is associated with natural organics. Ligands such as methyl ester of small-phthalic. paltmtic. and other carboxylic mo"C u'* '* *e'ght c ar.

acids may also be contributing to '"Co

['D l"a e c c a

[

ard U mobihzation to a sma'l extent.

internal standare Re. dent:6 cation of EDTA as a radio-

,, [,,,

'"I nuclide mobilizer in the ORNL disposal g

area raises a question about the suit.

%l abilits of this chelate in decontamination i

~

operations. Although EDTA is used in gj W

decontamination because orits powerful metai binding properties. this same char.

Time (minutes) acteristic also leads to radionuclide mo-28 21 le

.I5 12 9

6 3

bilization. The radionuclide mobilization caused by EDTA in the ORNL bunal 29c 260 230 200 170 140 llo so so grounds pret aHy does not.it present im-Temperature (*Cl l

pose a health hazard. However,its con-Fig. 3 The GC profile of GFC punfied and methylated groundwater sample RS7 30 WNE to los

uwpArymormgammimw syrgra-wriardMr.7.iQimcaoa. tricTmics c% avaar MrcWarmuudear egaggaea..

,19tn around the country. and therefore West Valle). New York L41. 31). and and reacion base been decontaminated l'

its presence in low and intermediate-Maxey Flats. Xentachy till. The Chalk h> means of a wide sariety et reagents Ic[el waste. constitutes a potential for River facility in Canada has expenenced encludmg strong acids, bases. or oxidiz-the retc.ne of undesirable amounts of r.i-similar migration problems Lf2). Actual mg agents, which can rse neutrahaed be-dionuclides. Because EDTA is remtant migration of Pu. the presence of Pu in the fore final burial, or relatiscl> mild com.

to decomposition by radiation 111. ther-dissobed fraction of leachates and the plexing agents such as citrate tartrate.

mally sery stable (221. and only slowly existence of mobile Pu-contaminated oxalate, gluconate. phosphate. basulfate, bicmiegradable (23), it is extremely per-leachates in waste pits have been report-and fluoride which will contribute to ra-sistent in the natural environment. In-ed at the Hanford. West Valley and dionuchde mobility in the ensironment deed, the presence of signif cant concen-Maxey Flats facilities, respectisely (29-to a much lesser extent than EDTA.

trations of EDTA in waste 12 to 15 years 3/). Complexing agents are either pres-Excellent reviews of ditTerent decon-old attests to its persistence. Therefore, ent or suspected to de present in waste at tamination solutions and techniques are wherever EDTA and similar compounds Chalk Riser. West Valley, and Maxey available (21). Many of these reagents a

has e been introduced into terrestrial dis-Flats 0 1 J2).

used either alone, in combination. or in poul sites, the aqueous transport of The use of EDTA and similar com-succewise treatments have been shown transition metals rare earths, and trans-pounds in decontamination operations, to be extremely effective ahernatives to uranics, which characteristically form and therefore their presence in low-and EDTA.

the most stable complexes with chelates, intermediate level waste in the United JEFFREY L. MEANs may be augmented.

States and the rest of the world. is wide-DAvD A. CRERAR There can be no question about the spread C1). Throughout the world, low-Department ofGrologicoland strong complexing capacity of EDTA and intermediate-level radioactive waste Geopirysica/ Sciences, and similar chelates for certain radio-is being buried along with chemicals that Prinction Unirresity, nuclides including the rare earths and ac-are likely to cause the migration of Princcion. New Jersey 06340 tinides. For example, all of the trivalent hazardous isotopes such as Pu over the J AM Es O. DucuiD rare carths along with Am**. Cm *. Pu'*.

long term. Indeed, trace levels of ra.

Energy and Environmental Sysicms 2

Pu*', Pu'*. and Th'* possess at least as dionuclides are being released by Assessment Sectirm.

high or higher complexity constants. K,.

groundwater transport at many radio-Bartclle Columbus Lahorotory, for EDTA as Co (241. Both EDTA and active waste disposal sites in this coun-Columbus. Ohio JJ201 DTPA are used in the therapeutic remos-try, and migration of radioactive transi-g,,,,,,,o..d %

al of transu*anics ingested by humans tion metals. rare earths, and transuranics

1. E G. Sirunness. OuA R.dre Aeri. bb Arr.

because of the strong complexes formed is probably being aided by chelates such ORNLJu 32; ti%::: W. de Laruna. K. E.

with these elements (231. Our evidence as EDTA. Consequently, if the use t1 N,7'U, c'i, $'$o##sD. $. '""'

suggests but does not prove that EDTA EDTA and similar compounds is to con-

2. D. A. w ster. u.S. Gro!. Sun. Ocea ric Arc e

n.r:7 <i97ea is also contributing to the migration of tinue. waste solutions should be treated

3. T. F. Iemeneck, ficuliA revs 9. 40$ IW1.

trace levek of Pu. Am. Cm. Th. and Ra.

for the removal or destruction of the che-g, y J((; f,$'y Ta A'Ia' '8f d

3 which hase been detected in the soil lates prior to final disposal in the ground.

Is. 467 0 970).T. F. Lomensck and D. A. Gardi.

7l;f'.,Carns.n. J r.. U.S. Grot. Jun from seep RS7 approximately 100 yards Another alternatise would be to use suit-3, (90 m) east of trench 7. For example, ac-able substitutes, compounds that are ef-P. H tenides were found in concentrations of fective in decontamination but do not fa-431-G Otos; R. J. Pickenng U.S. Grol. 5,*i.

P,of. rap. m.n o%9). u.s. Grot. Sm. r,cf.

O: 8 dpm'g of 23*Pu.110 : 7 dpmfg of cilitate radionuci;de mobilization.

Pap AJJ.> oOO).

P. H. Carngan. Jr..T.

Tamura. H. H. Ahee.J. H. Beverage. R. W. An.

'"Am. and 495 : 20 dpm'g of'"Cm in a One such useful substitute may be dre.. Jr.. in o,pos,i of s,s.o.c.., u,re,s...

• '"a'

"*J 5"'/d" "

weathered shale sample collected at a NTA. which is a potential replacement

'" 5'".n'l Atomic Energy Agency. b.8'"8enna tw"*o".

naison depth of 71 cm in well T7-12, which is for phosphates in detergents. This com-pr. sw J. o. Dueu.a. out u.oer Aurt. ub.

adjacent to uell RS7 (4. 5). In addition, pound is rapidly biodegradable (20) and

",'R ' M $ $ Ud' 8'd N"'t D *-

o chelates increase the uptake of numer-is a strong ligand, although slightly

4. J. L. Means. D. A. Crerar. J. O. Duguid. co&

ous trace elements by plants. Con-weaker in complexing capacity than

3. 7.Iu^eIY4 c,, of,#'#%',,'g',$

yp sequently, the ecological recycling rates EDTA.

Duru'd a r'er*2'oa 6 E. A. Jenne and J. S Wahlberg. Trans. Am.

of certain radionuclides such as 23'Pu and The biodegradability of other chelates G,open. va.

46.17o o%g

'"Am. and therefore the possibilits of such as triethylenetetraaminehexaacetic 7 Aa " 318 'dP'n 8' * d' ment] = (**Co tarris mii m 0....mm hivered aqueous e hase)-*. Lar+

their entering human food chai.s. in-acid (ITHA). hydroxyethylenediamine-raior>

A. s. lues were deiermmed by ihe" creases in the preseiw of compiexing triacetic acid (HEDTAl N-(2 hydroxy-

[n"j'l[nyi f",,,U",','lg',,d '"n *"d *,'j"ld asents 96).

ethyb-ethylenediaminetriacetic acid riernaie chemecal comromeon unid couilibn-In the United States, there are six (H EEDTA). ethylenediamine di-(0-hy-

[*,nTc'n',"o ** # "" * ""

commercial and five Energy Research droxyphenylacetate) (EDDHA), and 8 Se caJculated the actua! K. **1ues f'om ca*b ronmental sosi and anociated miersutsal mater and Development Administration terres-DTPA is apparently not well known.

samp;e,. us,n, ine same denninen as m ot trial radioactise waste burial sites which Some of these compounds are stronger t { d[MlQL,',d*",'g 88'"**u J Ma'-

have in the past received or are currently ligands than EDTA and therefore would to Grouna ier s.mries.ere coriccied m poi >eih.

receiving low-and intermediale-level ra-be more effective in decontamination.

@"4[',$'d[,'u'"dn,7,", y,y,y,b,f $,',j dioactive wastes (27). Varying levels of however, the use of such compounds. if aie sciennon and ihen tarough c.:: m Mai.-

radionuclide migration from original dis-nonbiodegradahle, could lead to esen n. I,"n *,'o*,.",','c"n'],,,,,,,,,,,,,,,,,, d s,,,,g posal sites base been observed at four of more migration fror. disposal sites than hund.co m Nuer, cr ine ocurcJ wmr.e ihre e cotumn : e) 30 cm hised so !$ cm meih kenwn these waste burial sites other than that caused n> EDTA.

ici. v.r..cm ui.on.ncn.n,e resin, at a no.

ORNL, includ ng the Savannah Riser Numerous other alternativ es to the

,, '.[]

,Py'j,Q**

g, Laboratory. South Caro!ina (28); the use of EDTA and related compounds are

.here u>r in the present arrocanon. -e mon-l too sctEscE. vot. :m

eetwed she'cluteJ frastions for radeud.de con.

iras:ss or tfrtalloss Comfrire (Necce.al Puh.

tent a:nd absorh.ince.st 24 Em. uung an m.ime h6 ation No l*

Chenes. % is ec e ), f.emd.m.

e, eltretu*ict spectroptcomettr. We avulp std Imai

• to esm; a mvhichannel sn.ely tes. enJ U m g 23 A C James ano

• M laglec./fruith pan 28.

deiermineJ by MS. with esonore delution il t tv'll. V H $ Ah. #4 I 12. %St14726 14 J. l.. Mr ins. D A Creras. J. I.. Amseer. /p..

26 A % li cc. st=J 22. "4 slV72L %. V laps.

n,J O. e naocr. 22. C? (19*76

.end A. S (addm. eNI.41, 42' 814'he. \\ Q 14 H R. Plumh and G F. I.ec. M,,rer Ars *..sul Hale and A Wallase %=14.e 109. Oh IICOs.

tIMit

27. Ahrraasts ee for llaarovac M essers from h ear.

13 K. C. beck. J H Reuter. E M Verdue. Gr.

sors naJ Foss.towne taperatums m^she L uR thnm Cosmors m Arca 34. MI (19141; M. A.

ILocht.% user Reactor) f eet Carer tYubhcanson u

kashed. Lul ars. Ill. 2YE (1971).

7tW1. hnergs Research and Desclopmeel Ad.

16 %e inethylated organic aceds in CFC fraci.ons menestr pon. w sh ngton. D.C. 1976L sok 4 a

a usms f(i percent BFs sn methanol. as proposed seciam 24.1.

by L. R. kudung ia irr Ars. 6. #74 1197211

28. 5 O. keichert. J. Graphis. Ars. 67. 426) w

17. J. A. Ap te% Decontamanusma nf Neclear Rear.

fl%21 armes and Zrin,fimrat (Ronsid Ne* York.1970:

29. S. M. Pnce and L. L. Ames, m Trennerwaemm

18. E. A. Bondicise of OR N L mas the Erst to sugsest Aschdrs sa sAr Emisroamrar iPubl.c.atson SM.

shaf **Co was transpor1ed as a compien mesh 19917. Internauonal Atomec Energy Asenc).

EDT A 441. Hn suggestion was based largely on Vienna.1976L p.194.

eon enchange. diasms and paper chromaiorra.

40 R.14eer and P. thskand.Sesta Dats I. 4 (19771 rhy analyses, and the knomledge that EDT A

31. G. L. Meyer. m Traaiersai m NnchJes sa s4r s

mas commonly used in decontamenateon opera.

Eanrrm ment IPuhhcanon SM Ivv!IUS. Inier.

emns at the lahorainr3 nauoruf Atornic Energ) Agenc). Varnna,1976).

19. The dimethyl esser of phihahe acid (probabh

p. 2)l.

mera orparai appears in the GC profde of a d f.

32. P. J. Parsons, en.5croed Cimf. Proc. Choll An.

ferent sampie frorr seep RS7 cr. Cuauda T!D 762/ 18%21

p. 16. health 20 R. D Sanher. T. A. Taufh. E. J. Ma6ec in rhts. 9.11 t l* tt t

Trure Mrrals sad Metal.Orsonalairrecs.one m

33. Thn project was funded by Energy Research Asieret H'sters. P C. Seriger. Ed i Ann Arhor and Deselopment Adm neuravon suncontract S.

Sceence. Ann Arbor,19'41. rr. 237-2taa. C. B.

4228 %e thank O. M. Sealand of ORNL mho

% 4rten. m $ntsnel m Tent Enninamrats (Ac.

• 4s of insalwahic awstance en the coleccieon ademic Press. Ne= York.1973L pp. 473.aw, and an.nlysn of sampict we thank B. F. Jones M. K. Fareuone and J. M. Tied c. Appl. M,rrr.

and I. A. Breper of the U.S. Gudog>ca! Surve).

i luol. 29.1$4 t1975L Weston. Va. and T. Iamura and E. A. Bondertu

21. J. A. Ayres. Aarsche.NorrA.rst Brp. ANu E.B.

of ORNL who oliered construcuve suggesuons.

90 (19711; A. B. Meservey. Prog. Aert. Earry's The GC and MS an lyses were done with the arr.4 4. 377 tl'r616 awstance of %. T. Rainey, C. A. Pnichard.and

22. A. E. Mattel!. R.1 Metekaan. A R.Fned.J.

D. C. Canada of OR N L. we thank R. l w lker S. %wori. D. T. Mac Millan. Cor. J. Chem. 53, of ORNL who did she U arulyses and T. G.

a 3476tl975L

23. T. M. Tiedje. Appl. Microbiol.10. 327 8 tF73);/.

Scots of ORNL who dkl the Pu. Am. and Cu analyses.

Eanraa Qual. 6. 21 e 19*7L

24. L. G. Lhen and A. E. Martell. Stabihrv Coa.

8 December 19774 revised fi March 6971i i

i 1

4 i

L l

l l

SCIENCE. VOL, 2m. 4 Jt'NE ten i

lui

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