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Steven A. Book
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RA01OACT1VE FALLOUT: An Overvfew of Internal Emftter
Research In the Era of Atmospheric
Nuclear Ueapons Testtng
llarvlnGoldman .
Moratory for Enertjy-RelatedHealth Research
Unfvwsfty of Callfornla, Oavls
~E8T GOPY AVAILABLE
March, 1983
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NOTICE
This report was prepared as an account of work sponsored by an
agency of the United States Goverrmnt. Neither the United
States Governnwt nor any agency thereof, nor any of their
anployees, makes dqy uarraoty, express or Implied, or assumes
my legal liabillty or responsibility for the accuracy, complete-
ness, or usefulness of any Information, apparatus, product, or
prQcess dfsclosed, or represents that Its usewou?d not Infringe
prfvately owned rights. Reference herefn to aqy sp?ciffc ca’n-
aercial product, process, or service by trade name, trademark,
aufufacturer, or othewise, does not necessarily const~tute or
imply fts endorsewnt, recmnpndatlnn, or favoring by the [United
States Govcrnnent or any agency thereof. The views and op+n!ons
of authors expressed herein do not necessarily state or reflect
those of the United States Gwcrnnent or aqy agency thereof.
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ACKNOWLEDGMENTS
Tharks me extended to Mrs. Susan Munn, MO helped review the literature,
toMr. Charles Baty, who typed themanuscrlpt, and to Dr. Leon Rosenblatt, who
critically reviewed the report. Special gratitude goes cut to Drs. Newell
Stanmrd, Pat Ourbin, Miriam Finkel, Leo Bustad, Roy Thompson, and Merril
Eisenbud, *O provided reference material and backgrmnd information. Th~s. .
m“k was supported by the Departmnt of Energy.
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TABLE W CONTENTS
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INTRWJCTION . . . . . . . . . . . ● . . . . .
A HISTORICAL PERWCTIVE . . . . . . . . . . .
DEVELOPMENTS IN RAOI0810LOGICAL RESEAR@l . . .
Health Effects ..*. .*. c*c *c’ .*Risk Asses-nt .**.*.. . . . . . . . .Envlrorwental Radloactfvlty . . . . . . , . .
RADIOMJCLICES 5 SIGNIFICWCE . . . ● . . . . .
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v RMIOI~INE . . . . . . . . . . . . .,o.~
summary*....****** ● **S***Envfronaentai PattUays . . , . s ● ● ● ● cMet@ollc Pathways . . , . . . . . , s . .Radfoblologlcdl Effects , . . . , . . . c w
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Thymld Moplasia. o....... .s. .Olfferences In Radloblolog!c [ff~ctivenessCstlmates of Thmofd Risk ●
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Means of Protecilon . .
RADIOSTRONTIlB4 . . . . .
Sweaty . . . . . . . .[nviromental PatluuysUetd)oltc pathways . .Rtijobtological Efftcts
am~ats~w . . . . . , ,
$WMry. ..o. o..[nvfromnentdl p~ttuaysbtabol!c P#thw#ys ● *P~foblo)qfc [ff~ct$ .
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VIII PLUTONIU4 . . . s . ● Q c
sunllury,*c ****cEnvlronnental PatWaysMetabolfc Pdthways . .Radiobfological Effects
IX URANIUM . . . . . . . . .
SUllWIMrye. ● ● . ● ● .
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✎Enviro-mntal PathwaysMetabolic Patkays and Effects
REFERENCES . ..o . . ..o. ..t. o
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LIST (I TABLES
Table 1. Some Important dates In the history of radioactive fallwt . . , 14
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1. INTROOUCT!ON
Thfs report Is a revlewof the literature on the radloblology of tnterna?
amfttem. Its pwpose Is to consider #hat has becaee known &at the radin-
biologyof fnternallydeposlted radlonuclldes over the last four decades. Our
prlMr7 emphtsls Is the Progression of rddlobtologtcal Infonnutlon through the
19SOS mdearly 1960s, when atmospheric testing of stunlc weapns was
occurrlfq wfth tncreasiq regularity.
Most of the over ?~referemes ctted in th~s report are from the openW
literature, tlthough use of technical reports wes somettmes also needed. Our
focus wssondeveloptng a ~dSO?)i3ble,documented chronology of the evolut!on
~f Imwledgo bout the rdfoblology of fallouk Ue have used w $cIentfflc
judgmtt ~out the slgnlflcance of avatlable lnfonnatlon fn dlstllllng an
enormous VOIW of 1lterature into a report of “this size.
Uedo not lnt#nd thfs report to be a complete suney of the subject. The
SClentlftc Itterature ts replete with overviews of r~iobiologfc studfes, and
*W h: not been reY!~ fn the epe!!l!terg?ure has ben r-vfOw@ in many
doaments, Includlng those on nuclear reactor safety (US MIC.,1975), “radiitton
risks (UNSCEM, 1977, 1982; MS, 1972, 1980), and radtatlon research In
general (IRRC, 1980).
In thfs report, sfter a historical perspective (Chapter 11), w *iLlr@~$
the genertl evolut$on of redlobiological research on Internal mltter$ ~ron
qua!ftatfve studies on their rudlotoxtctty to qwntltatlve assesmmt$ of the
rfsk fro expo$ures to thm (Chapter 111). Further, w look ~n 9Pneral at
fm~rtaot dev~lopmts fn t~ c~n~ern over fallout frm nuc!e~r woap~n{
detonttlons tkouqh th era of dtmtpkrfc t?stfng.
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M also consider iftfOfW4tfOfIon fission products that are bfOIWJfCdlly
fmportmt (Chapter IV), $Pectfically, w dfscuss In detafl Isotopes of
Iodine, $Wontfum, and ceslum (Chapters V, V!, and VI1, respectfvely). These
redtonuclfdes are cmponents of redloactfve fallout aml are readily taken up
by the body,
Finally, w also exemtm data for plutonlum (Chapter VIII) and uranfum
(Chapter IX). These l-st two elements, not woduced by flsston but rather
used In pmductng It, are generally consumed In the flssfon redctlon. Those
atms thet escape flsslon, however, can be dls~fied and may present Ptenttal
envlromntal MM health hazwds.
Forewh of the redionuclldes d!scuswd, w consider envlronnental path-
uaysthet am wlleble for the eventual exposure to hunsn populations and the
aet~ollc patlmmys that determine the tissues at rfsk folloulng exposure. Me
also consfder the redfoblologlcal effects of exposures given at high levels,
●nd, hen epproprjate, t~ risks ecconpanyfng lou-?evpl aposwes,
II.,&__.—______.-- _=. --=ik ----.*-
3 I
11, A HISTORICAL
Considerable
produced internal
PERSPECTIVE
Information on themetabolism ati effects of ftsslon-
enftters was avaflable in the 1940s. Most of it arose fron
work related to the development
(1947) explatnd that research:
of atomic weapons (Smyth, 1946). Hamflton
●
● ✎ During the early phases of the development of the
Plutonium Project, ft became apparent that one ofthc most e
serious problems to be encountered was the protection of
personnel worktng In this field against the hmense
quantities of radiation and radioactive materials prodwed
by the chain-reactfng pile. The most important hazard that
arises fron the release of nuclear enemy are radiations
produced directly from fission and subsequently emitted by
the resultant ftssfon products and plutonium. The fission
products can produce injury either as an external source of
rufiatlon or, tf they gain entry tnto the body, by acttng
as an internal radioactive poison, quite analogous to radiun
pofso!!ing. This ?atter cws!der3t!e~ !5 a major ccncern,
since the amounts requtred within the body to produce
l@urfous effects are mfnutecunpared to the quantities
necessary to fnduce damage by external beta and gmma
Irradiation ....
The flssfonof wanlum results In the Productlonof
thfrty-four radioactive elements, extendtng frm zinc to
europfum, and there have been Identifid nearly two hundrd
radioactive Isotopes of this large number of elements that
r[se fran flsslon. Stnce the possfb~llty of entry of these
fission products Into the body had to be consfderd as on?
of the prlnc~pal hazards to ttise wor+~ng In th~ ffeld of
atmnlc energy, It was n~cessdry to secure lnfomatictn us to
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the *sorption, dfstrfbution, retention, and excretion of
these radioactive materials. In addition to evaluating the
metabolfc characterist~cs of these substances, it was necessary
to dupllcate as nearly as possible, wfth laboratory animals,
the manner by thich fissfon product lmisoning might occur.
This Included a study of the behavior of these radioelements
following their introduction into the bodyby the three major
portals of entry, namely inhalation, oral ingestion, and
through cuts and abrasions of the intact skin ....
No satisfactory estimates or predictions of the possible
mtabollc characteristics of most of the fission products
could be made, sfnce most of these substances are radioactive
fsotope$ of ●lementsconcernfng whose metabolic properties
very llttle was known. In other words, there were no relidble
data available that could’make it possible inmost instances
to predict whfch of the fission products would be ~sorbed
from the digestive tract and rapidly eliminated, once having
gafml entry fnto the body, and which ones might be selectively
deposited and retafned in sune vital structure. Actually,
there was only one ffssfon product, radiofodfne, that hti
recefved sufficient study with regard to fts mtabolic proper-
ties, prtor to 1942, to permit a redson*le evdluatfonof the
mount that could be tolerated within the body without producing
damage. A secoti fission product, redfostrontiwa, had been
studfed before 1942, but not in sufficient detail to satisfy
the requirements of the medical research Pogran of the
Plutonilm Project. The nature of the metabolic characteristics
of the other fission products at that date was essentially a
completely unknown quality .,.,
In ddition to the fission products, ft was nece$sary
to ev~lu~te by similar tracer studfes the potential darqem
from plutonium poisonfng. Thit elment ts radtnactlvc and
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has a half-life only fifteen times greater than radium. In
eddftton, the quantltie$ to be jsolat~~ Purlf~ed~ and used
for a variety of purposes were considerable, to say the least.
Later, several other of the heaviest elements, ccmonl y cal1ed
the actlnide elements, With extend fran actin~um through
curium (element 96) were included for studyc These substances
either arfse dfrectly In the chain-reacting pile or appear in● certafn phases of the atomic energy program and present
potentfal health hazards because they all share the conmon e
property of radfoactIvity.
9D
There was also information available on fallout from atomic weapon detona-
tions. livestock that were exposed to Iocalized”fallout fronthe Trini& Shot “’ “
fn New Mextco in July, 1945 showed effects of the exposure (beta burns on the
skfrt)(Glasstoneet al., 1950)..
Fallout occurring ut more distant locations
was also observed in August, 1945, fn Indiana, when photo$raphfc film was
fogged by radioactive contaminants in packaging materials (Webb, 1949)’.
Research on fallout fran Trinity continued for a number of years after the
detonation (Larson, 1963).
Glasstoneet al. (1950) discussed the effects of these weapons, briefly
~ntioning the potential of serious p~siologicdl hazard of radioactive
fallout that deposits on the earth’s surface in appreciable amounts. These
autkrs also considered the problems of radioactive contunination of food and
water, and tabulated fission products and their relative importance at varying
times after fission. In dditlon, the biological significance of missioned
ur~niun or plutonium releasd jnto the environment was also discussed,
information on fissfon-producd internal enttters seems to have developwf
in three major phases. In the 1940s, studies related to themetabollsm and
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effects of radfonuclfdes were wrformed? The Impetus for this WOti
occupattonal safety, In eddltfon, sane medical work was also being
6
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done. In
the 19S0s and 1960s, the awareness of radioactive fallout changed the purpose
of much work to addressing publIc safety. Much of the wrk was environmental
in nature, tilch evolved into the discfpline of radfoecology. The first
symposlun on radionuclIdes In the environment was held fn 1959 (Caldecott and
Snyder, 1960), closely followed by a symposium on radfoeco?ogy held fn 1961
1 (Schultz and KlemrIt, 1963).
In the 1960s and up to the present, uoti has contfnued related to the~
1
ptilIc $@fety from fnternal emitters, though the drfvfng force evolved fran ,
contanfnatlon by nuclear weapom to the potentfal for contmlnation by nuclear
reactors ati related fuel cycle operations. Work also contfnued to address
, problems of occupatfona? exposure. Unlfke the research of the 1940s, vhfch
tended to enphasfze fmmedlate effects of hfgh levels of exposure, the more
$. contemporary wrk has enphastzed the consequences of lo~-term exposures and$
latent health effects of low level exposures as well as therwchan~sms ofF
these effects. Radlatton-induced
most of the more recent research.
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cancer has been the significant end-point of
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IIIe WVELOPMEMTS IN RAOI(B1OLOGICAL RESEARCH
Radloblologlcal research on Internally deposfttd fission products under-
went 8 number of evoluttomy changes fran the 1940s to the present. Thes~
changes occurred fn lnvestlgatlons on the health effects of these radio-
nuclfdes ad In attuapts to estimate the risks that acconpany Irradiation.
StudWon theenvlmrmmtal significance of radlonuclides also changed, as
. . prmptd by the recognttfonof f~ssion products in fal
ccaapanlonsof the testing of nuclear weaponsg
out as uwelcone
He*lth Effectg
Studies on the biological effects
progressed frwan Wtial production
of Internal enitters generally●
of radionucltdes to m?tabolic studtes on
thelrdlstrlbutlonmd excretion. Fran here, studies on the acute toxicity,
ellcfted by exposures to large amwnts of radioactivity, were next. Then,
since mat of the concern was for protection of the worker, chronfc studies
involvtng long-tern exposures to lower levels of radtoactlvfty w&done to
gatn understanding abwt the late effects that might be produced. The prior
experience with the late effects seen fn the radim dial painters prmnpted
long-tern studies uith other rtiionuclfdes in the 1940s, principally with bone
seekers such as strontlun-89, -90, and plutonius-239. In depth studtes of
these radlowclldes began in the 1950s, Men the Atmnlc Inerqy Cunmisslon
established several beagle dog colonfes around the country. Uork continues to
the present thae.
For ratflofodlne,the pattern of research developwnt In the IWO$ w35
,
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rdfo$c~ltfve and not radloreS~stant, tiich occurred (n the 1950s when
thyroidcancers were produced In animal models ?nd *en they uere shown to b~
produced In children years after x-lrradtatlon of the head and neck, was there
more study of the late effects of radtofodine.
The significance of ceslum-137 was not appreciated until the 1950s, when
It was found In the envlrofnent. Although lfmfted research on radtoceslum was
done in the 1940s, It Went through the pattern of testfng--metaboltw, acute
effects, l~te effects--later, and tn a chronologically cunpacted time.
RlsltAssessmen{
Acute responses
to predkt, tn that
to Irradtatlon were falrlyeusy to describe and, probably,
hfgh enough doses would ellctt acute effects, and louer
Of!@ uould not, ‘Safem exposures were at levels less than tolerance doses,
that ts, levels at thtch r~ove~ would occur.
Assessment of radlatlon risk tn the 1950s was In the contest of thres-
holds, tnjury and repatr, and lifeshortentng, Blair (1962) dlSCUSS~ radia-
tfon tnjury fn terms of acute reparable amd Irreparable I@urtes meimured by
llfe stuwtenlng. That low level radfatlon Indwed lifeshortenfng was
prfaarflya carclnogenesfs effect W*S not generally recognized (FRC, 1960).
“Early” lrJury fn exposed mammals WS frequently measured bycmparing pre-
cnd post-exposure blood cwnts, a Fact Ice alnust as wtdeswed as the use of
film bad~s for dosl~try.
for low-level exposures to pose risks for latent health effects was not
cons~stent with th thr~shold, or tolerance, dose concept then In voque. At
tht tlma genetfc effects ~re tkught to be wfttc)uta threshold, or I{nedr In
rcsfunse (?CRP, i~54), an opfnfon l$rqely Inflwnctwl !}?”t~ ~~rly r~$~~r~h or
k ‘-—..-_.—.___.— ..... .. . 1-
fmlt files. Only lster dld the stoch~stfc nature (@09st cancer) of t~
reswnse of $cmtfc tissue to radlttton become clear, Re~lrable Injury
(e.g. on $pensttogenests, ?wkocyte counts) was a fmctlontl phenanena and
Irrepamblo l@ury was an ‘eccleratlon of aging’ phenmenon that shortened
llfespsn.
Wth late effects such csbone cancers, the all-or-none principle
4e8crtbed above bec&ae the sII, none, or some prlnclple. In experiments with
9rWpS Of animals eMpOWd to $rtitd dosages of bone $eekers, differences t%
ntier% of cases of cancer and their times of occurrence -re observed.
Higher
enough
(Brues
doses resulted Inmwe tumrs at earlfer”tlmes than lower doses. Lou
doses dld not result In effects before mhels dfed of natural causes●
●t 0]., I*T; 6rws, 1949), thus lead~ng to the concept of a “practfcal
tlwwshold” (Evsns et al., 1972).
The shepe of the dose-res~nse curve for radiztfon-ind~d ctncers became
the s@wt of dehte In the 19S05. Several sctentlsts (1.eufs,1957; Court-
Brown, 1%8) ●spousal llnearlty as the proper way to express the re’latfonshtp
of dose a?uleffect, cltlng a proport~ontl Incre#se In effect wfth increasing
dose In Irradf#ted humeripopul~tfons u evidence for their claim. Others
(Ml@~ 19M; F~nkel, 1958; 8rues, 1958), *O based their opinions mor~ ori
~nlmtl @ta, consldere$ a curvilinear dose-response relationship to be more
approprlatee
The *te over the
tO thts time. This WS
report of the Comnit?ee
1980}.
proper shape of the dose-response curve has cont~nued
demonstrated by the r~ent ad contrwcrsy-rfdd~n
on tht 81010glcal ff(ects of lon{ztng ~~dlet!on (N45,
1- -. I>.- -—. ,. -—- ..—
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Thewonls of Mole (1958) seue cs fitting now as they ~re then written:
Uhatever the shape of the tsnplricallydetewnfnecfcurve,
It is aluays possible that the shape of the curve changes at
doses less than the lmmt used. Even if there were several
dose-levels at each of ~ich the response was nodjfferent
frtn the base-l~ne control, ~tmust be accepted that each of the
-Csuraxi responses has a stotlstical error. The possibility can
never be denfed that obsemattons on a much la~er scale would
have shown responses really greater than the control. Thus the
ex~stence of a threshold can never be proved by an eaplrical
dose-response curve. Equally, of course, for sfmilar reasons
the ~sence of a threshold can never be proved. Thus the
existence or not of a threshold can be determined only on
theoretical grwnds.
Aloq wfthand because of the uncertatnttes of radlatton effects, a risk
philosophy hed to be Incorporated fnto the establts)wmt of radfatton protec-
tion hazards (Twlor, 1958). This phflosoph =s necessary because radtatfon
standards, present for several decades already, were expressed in terns of
‘pemlsslble’ doses, ti~ch Iraplfaithe acceptance of some small, but undefined
(WMI undefinable) rfsk. R~sks moved frcrnbeing generally qualttatlve to beln9
quantifiable (lCRP, 1966), and have been the subject of elaborate calcula-
tions, ~lmarlly wfth regard to scfety frcn nuclear reactors (US NRC, 197S].
Rec~nltlon that radiation was hazardous resultd in the formtion of
several scientific adv!sory groups who m~dP recmmwndatlons of lifntts for
Occupational?sti non-occupational aposurmt Thesp recuwnendatlons Wrp
lstued in g~ fo~ Of ppri~dfc re~rts by: th? lnternatianal Cmnl$s!on on
R#d!ol~fcal prot~~t~nn (~CRp), foundpfi{n 1978; t~ N#tlnn*~ C~Ur!r{lon
RadlStlon Protpctton and %afurmmt$ (}fu~}, fo,mlnq In I<N6 frw ?n advt~~)’v
-. .
l?------- ~‘- —-. -..— . . “t-.— -m=- .-./.-*
11
cusmlttee out of the National Bureau of Standards; the Un$ted Nations’
Sclentiflc Cmm!ttee on the Effects of Atomic Rad#atlon (UNSCEAR), established
In 1955; the Natfonal Acadmyof Sciences/National Research Counc~l’s
(MAS/NRC) Cmelttees on Blologfcal Effects of Atodc Radfatfon (BEAR), which
ftrst ~llshed a report in 1956, and, later, the HAS/NRC’s Cunmittee on
81010gical Effects of Ionizing Radiation (13E1R).
● “ The Federal Radiation Council (FRC) was formed In 1959 to provide federd~
pollcyon human radiation exposure. In 1970, this task was transferred to”the
Envlromental Protectfgn Agency (EPA), Wtch also &sorbed fission- and
mdlcal-related matters that had been under the Atanlc Energy Cavnissfon and
the Department of Health, Education and Uelfare. ●The EPA continues to
function wlththe same responsibilities, with interaction with the Nuclear
Regulato~Conmlssion, the Food and Drug Mministratfon’s Burem of
Radiological Health, and other agencies.
Enviromaentsl Radlqactlvtty
At the same time radlobiologlcal research on the effects of Internal
emitters was evolving, so, too, was enviromnental research developing. Host
research in the 1940s was concerned with the wo~ enviromnent where man-made
or technologically enhanced radfoactfvfty would be encountered in much higher
concentration than in the general environment.
In 194S, when the Trinity shot occurred, radioactive fallout was first
producad Ioctlly (Glasstone et al., 1950). Fallwt contfnued to be recoqn!zml
a% t contaa~nant of the envfromwnt thereafter, from testing in the Pttclffcin
th I?tc 1940s (Carter ~ti Moghf$si, 1977; Perk{ns and Thmas, 19N7), h{~t {t
appars that most concern was about th? cmtanlnetlon of mter!bl cIPo$Pf tf’
!.
..,:’L.f<. ------...-----..- k .- .-.I
Themoredlstant nature of fallout deposition was noticed in 1945, but not
published mtil later (Uebb, 1949). In this case, mphdsis was on exposed
pbtographic film rather thdn exposed human populations.
That fallout was present at distances far from the site of detonation was
again ckmonstrated In the early 1950s in cnvironnental smples (precipitation)
that contained high levels of unnatural radioactivity (Meinke, 1951; Helter
and Glusscock, 1952; Clark, 1954).
sftes, however, was not considered
health hazati (AEC, 1953a).
Fallout occurring wtsfde of the test
to create any Immediate or long-range
Anetmrk of nmitoringstatlons for fallout radioactivity was established
In 1951 (Elsenbud, 1957). Fallout 9%r levels, fran data fmn those
statjons, were published by Elsenbud and Harley (1953). The presence of
fallwt 13~1 jn thyroid glands was first published by Van Hiddlesworth
(1954). The potential for health etfects from these radlonuclides, however,
was not ● cause for s~gniftcant discussion in these early papers.
Although there was local mrry about exposurp% fromtlw Nevafi test stte
In the early 1950s, serious concern about the health effects of radioactive
fallout arose with the detonation of iilarger weafmn in 1954 (Anonymous,
1954). A detonation on Harch
fallout that necessitated the
inhabitants fran thet4arshall
1, 1954 in the Central Pactfic resultd in
evacuation of 28 Americans and 236 native
Islands. Twenty-three ftshennan on a Japanese
trawler were also exposed to the fallout, and suffered sign{ffcant medical
●ffects. One of the fishermen did on September 23, 1954 (Arnold, 1954), frm
Itver d~ge (A#pendix VI, Conard et al., 1980). The Marsh&llesemanifrstod
●arly effscts 4S w]], and $howed a num!)rrof l~te @ff@cts, mny of thm
Wli)ted to exposure$ of the thyroid q~dnd, Onp perwn alw died frt~ drutr
SIyelogenou$ l~krmld (Con4rfiQt al., ~~?s, !d~~[i).
-.
-. .-.. ———1—-
13
~ltCWll *Wt the toxfCfty of radloact!ve fallout frun the detonation In
Harch, 1954, resulted in a
CIVI1 defense (LUPP9 1954$
1955b), th persistence of
1955c), ad global fallout
reportd on the effects of
series of articles about fallout as iinew peril for
1955it),fallout and government secrecy (Lapp,
fallout and the problem of internal emitters (Lappt
(LaPp, 1955d). The Atonic Energy Commission
the March 1954 test fn 1955 (AEC, 1955). Also in
““ 1955, Co~resstonal hearings were held to place on the public record factors
about the effects of atomic ~afms testing at the Nevada test sfte (;S
congress, 1955).
By 1%6, reportson the global distribu;lon of fallout ~311 and ‘Osr
frua weapons tests uere published (Van t4iddlesworth,1956; Hachta et~al.,
1956)0 By 1957, the correlation betwert weapms tests and 1311 fn human and
bovlnet~roid glands was established, and the Importance of cows’ mflk in
hunancontmfnation uas dfscussed (Comer et al., 1%7). At about the same
ttme, ~37CSuas shown u be in people (?4111erand Marlnelll, 1956), In
1%7, tingressfonal hearfngs to bring together Infonnatlon on radioactive
ftllout were held (U. S. Congress, 1957). Further hearings wre held in 1959
and 1%3 (U. S. Congress, 1%9, 1963).
ThediXlpllneof radioecology MS flnnly establish fn the early 1960s
(Caldecott and Snyder, 1960; Schultz and Klenxmt, 1963), Since that time ft
has becaae more sophisticated, with elaborate models of radionuclides in the
environment used to predfct exposures to humdn populations. Much of the
lnfO~atiOn tn these models, now used primartly for evaluating the environmen-
tal Sfgnlffcmce of various steps in the nuclear fuel cycle, had its origins
In studies of wedpons-related fallwt.
There were many occurrences and fnvesttqetfons that took place durlnq (~10
e~a of atmospheric wedpons testfng. U@ hdv(? !nc\uflo:i what we ronltripr
importantdates in thfs hfstory of rc3d!OdCtiV@ fallout in Ttb]r 1.
—---- —-. ... .+_ -.-* ---- ... ... . .. II
-..,,
&...-,.0
Table 1. Sane Iqxmtant Oates In the History of Radioact~ve Fallout.
——- ----..-.-—--—-- -——- --------—-. .—..-
Date Event Reference
—..—— .— ------.---—
1940s
1945
1945
1945
1946,48
1946
1950s
1951
1951,52,1953
1953
1953
19s4
1954
1954
1955
1956
1957
19s7
+.
$tudtes on awt~oltsmarx-1 effects offnternal unfttws
Trfnfty stwt, Alamo90nlo, New Nexlco
Local fallout fron Trlnlty
Fallmt fron Trfnity in Indiana
P&ctffc testlq
Local fallout on ships fran Pacificte$ts
Studfes onmetaboltsm and lateeffects of ~nternal enitters
Tcstlng begins at Nevada Test Site
Ftllout ~n predpltatlon in Michigan,Montana, and M Yor&
Heavy fallout fn Utah
Ulde dfstrlbutlon of 90Sr in falloutiapoebad
Fallout on f4arshdllesefron Pactftctest
$erfous radiation effects In fallout-exposed Japanese ffshennen
131] In an~ma~ t~rold gland$ ofanimals dfstant frcm Nevada test site
C0n9ressfon*l hearings on f~llout
137Cs found In people
Ccrrelatlon houn bet-en waponsftests and 13 ! \n t~r0i4 glands;
role of cow’ milk tn human expo-Swc% dlscu$sd
Uftiscsle reactor accfdentIn [rqlsnd
Chaps. V-IX, this report
Smyth, 1946
Glasstoneet al., 1950
Uebb, 1949
Cartermd ?foghlssl,1977
Glasstoneet al.:1950
Chaps. V-IX, this report
Carter and Moghlssl, 1977
Mefnke, 1951; Helter andGlasscock, 1952; Clark, 1954
AEC, 1953b
Elsenbud and Harley, 1953
Kc, 1955
Arnold, 1954
Van ?liddlesworth,1954
US Congress, 19S5
Mfller and %r{nellf, 1956
Cmar et al., 1957
I“ffpn!t,j,f,19?3
-—.. .— —.. 4---’wtv-,. -J
~- i
...
,
,’.
I
t
,..
..,4
‘.
:
; ,
...,,
,,
t
,’
.
.
.>
.s28.
Tsblo }. SOmt Important ~tet In the Ii!;tory Of Redloectlve ~allout.(Conttnucd)
-——. -------...-—— ----.—. ----------
1957
19s7,58
\%9
1959
1958-61
1960s
1961
1%1
1%3
1%3
1%3
1960s-70s
Coq~cssfonol hearfqs on ftllwt
Early PJpors ad dose-responserclatlonshlps P*1 !shed
Sywposlua on vadlonuclIdes Inenvlrofsmt
Co~resslonal iwarlngs on ftllwt
lWatOrW 00 weapons testtng
Studlcs on aet*ol~sm and late
●ffects of Intemd dtters
T8sttq WsW#
Wt Iowl symposim on radhecol ogy
Congr8sstonal horfngs on f al 1out
Syaposl- on rad!olodlne
U.S., U.K,, and U.S.S.fi.endstaospimrfc tssttng
U. S. Congress, 1957
l~f$, 1957; Court-Broun, ~’35~Hole, 1%8; Brues, 1958
US Corqress, 1959 “
Cartef and Moghfssf, 19?1n
Chaps. V-IX, th~s report
“ Csrter ~nd ?foghfssf,1977
Schultz and %Iement , 1963
US Congress, 196J
Busted, 1963
Carter and Hoghtssf, 1911
french, Chinese continue *tnrosphertc Carter ano *gnissi, i;;~testt~
——— ........—— -------. —— ...... ---
-— - —. - ...?.T- L
,
I
1
●
L
The 1940s -re a decede of discovery. The fission ucapons wre producw-1
ad along ulth their production, considerable new knowIdge about the metab-
olfsa ad effects of rdfonuclldes was born. The applfcatton of radfonuclldr~
to aedlcal procedures also showed great proodse ard resulted fn much
f?#folnlatto&
In the 1%0s, ft becem apperent that there were env!rormwntal and poten-
tial health consequences related to the weapons testl~. An envlromnentd~w,
auereness begen to develop, as dfc!concern about the long-term effects of●
contlrwd ~poswe to 10U levels of redfonuclldes, As s result, lamer
studfes -e begwt to eddress the biological sl~fflcance of these exposures.o
These would continue though the nut decades.
In the 1%0s, •nv~m~rttal and publIc haalth awareness became umre acute
prior to t~ s~gnlng of the nuclear test ban treaty. Rtdloecologlcal studtes
sti nodels kme ~re sophfst{cated. The long-term btoeffects studies
contllwti*
In the 1970s, with the near absence of atmospheric test(ng, most of the
r*loblolqk research took on an orientation related to wclea~ power ~nw
Ctlofi,sfnce thfs technology rcpesentm new sources of Occuwt ~onal and
~ulation uposwos ad enviromentsl contmtnttton. Concern was basictlly
tb s~-th ●ffects of Iong-tem, Iow-level esposures. There was also
c06c8rn ~at the ]tkeltbod of major reactor accidents tti s@\mwnt
rodlologtcal tipact.
The 1900s $hould tee the ccupletl~n of th Iorvj-t?m btoeff~ct$ $tudlm
bvgun dudes tarl !w, Thefr results wllI lpod, tt I* hopti, !O a~ ~ncr?a~ei
wndcrst.til~ of t~ rclatlomhfp of ftilatlon dos~, ●ffect, 4nl !lWIF,OWI
QttWs for tk pedlctlofi 0? rt~b; !0 pr)ple frcm ewpmu~r tn ‘c~P*~oT~f
depe$~tcd rtifomcl~ds$.
—._____
.● ✎✎ ✎✍✌✎☛
IV, MOIONJCLIES OF SIGNIFICANCE
17
Isotopes of Iodine, strontium, and cesfum have received the greatest
attention as canponents of radioactive fallout. Although other radionuclfctes
are ffssion products as well, few of them have the characteristics to make
them as Important biologically (Sternberg, 1968).
To be of radiobfologfcal significance, a radlonuclide released into the
●nvfronnent ffrst must have a physical half-lffe of sufficient duration so
thtt it will continue to be radioactive durfng the tfme requfred to enter into
biological systess tnd to traverse food chafns to reach the fndfvfdual who
consums it, Iodine-131, with Its 8-day half Iffe, exists long enough to move
though th atmosphere~egetation+cow-nfl k+people patluay. Strontfum-90 and
cesium-137 have half-llves of 29 and 30 years, respectively, aml can eas~ly
●nter the sane patlways for human
them to use other pathways as *el
and vegetatlon+eowaeat for 137CS
The signjflcant radfonuclfde !
exposure. Their longer lives also enable
, such as Sofl?egetation tow for ‘o%,
(Comar and Lengemann, 1967).
hould also be able to be effectively
assfmllctad Into the body. Iodfne-131 has easy access, because fti~iIefs
rqutred for nomal thyroid gland function and the body does not distlrtgutsh
between fsotopes of the element. Strontium-90 and cesfum-
body because they behave generally Ilke calclum and pota$s’
whfch tre fraportantccxnponentsof biologfcdl systems. It
-t~oll~ of each rad!onuclfde thdt determines Its potent’
efftcto Other ffsslon products t?d not
diet or tnto t!%$ue$ that tlwse three do
Resetrch on the radfoecO~OqY ati b!O
37 cav enter the
bm, respectively,
s the sgmcific
al for dir~ct tr)xfc
-..
G.. 1.
.
and excretion of a number of radlonuclldes, including barium-140, cerium-141
and -144, zirconium-95, ruthenfum-103 ami -106, and tellurium-127 and -129.
$tudfesof 106Rumetabolismwn also done by Thunpson et al, (1958) and
Furchner et al. (197)). Considerable work wis doneon radiobiologyof
radfocerlum (NCRP, 1978), not only because it is an abundant fission product
with a 285-day half life, but also because 144Ce is a beta-emfttfng boneWseeker that provides a valuable tool for understanding the effects of bon:
sedlng rtifowclldes (IURP, 1978). Reviews of the radioecologyof several
radtonuclldes h-w been publfshed, includfng r:thenium ami rhodfum (Auerbach
and Olson, 1963),the rare earths (Palumbo, 1963), and zirconfum (Held, 1963),
b
.—--- I_- -- -—
-T” -- ‘
1
● ✎✎
—
,- ... 19
V, RADIOI(M)I?IE
a!!!EKYIodine-131fs the primary radfoiodfne that Is of importance in rad~oactive
fallout. It has an 8-day physical half-llfe and is a beta and gmna emitter.
The t~rotd gland is the principal target o~an of 1311,
T’he-tabolism of Iodfne and effects of 1311, especially for high doses,
were known tn the late 1940s as a result of medical uses of radioiodine.
Wpothyrofdtsm was the prhsry radiolodine exposure effect, *ile thyroid
CWcinogtna8fs came W be appreciated as a late effwt of t~roid irradiation Ifi
the 1950s. Isotopes of Iodine were known to be canponents ~f radloactive
Cort-inatlon fra atomic weapons end ruclear facflftfes by 1950, and were
reported to be tn preclpttatlon in the open literature In 1951 ~nd In animal
t~rofds In 1954.
Fr~ the 1%0s fnto the 1980s, radfo~odfnes have been the subject of
researth, not only becwse of their role as a can~nent of radioactive fallout,
but .1so because of their position as potential envfrommrttal contaminants frcan
has led to an ●ven greater understandi~ of their btologfcal significance.
hvi~ntal Pathways
A rwleu Of tk literature indicates that 1ittle Informationon 131I in
tiw ●nvirwunent ●xisted untfl the mid-1950s. Nevertheless, in the Iote 194f15
thre was concern *out the hazad to anfinalsgrdzing on lad th+t wat cofi!m+-
nated with r~d!o~ct lvity froa afrl)ornewd$tes from the pro41Ktton of mJC!P?~
wter~als. Out of this concern, SIper(mental p!ans to wdlwte ttw ●ff?cfl 0’
13~1 fn shew were auti {n 194fli!ornhrg, 19(~4), In *!.7t!Ion, hy li~~~
.- .- -,. 1-
20
!
i
Isotopes of Iodine were recognized as contaminants of the env
detonation of atomic weapons (@asstone et al., 1950).
The earliest report In the open literature on 1311 in env
roment fol1owin?
rorsnental
$amples appeurfKfin 1951 when chemical separations were made on radioactivity in
snow In Mlchlgm (Fiefnke,1951). In 1953, an assay of 10 sheep thyroids in Utah
showed Me presence of 1311 2-3 weeks after an atomfc detonation in Nevada
“ (Uolff, 1957). In 19S4, the radlonuclide was shown to be ~n thyroid glands of
cattle snd sheep slaughtered tn Memphis, TN, San Francisco, CA, and Boston, MA,
but originatlq fn other areas of the Unitmi States, fncludl~ Kentucky and
Florlda (Van 14fddleswrth, 1954a). After his initial report, Van Plfddleswrth
(1956) described the global nature of the distribution of fullwt 131J In
ctttle and sheep thyroids, Soon, Cornaret a;. (1957) demonstrated a correlation
betueen increased concentrations of 1311 in t~rold glands fn human and bovfn~
thyroids with knmm atomic weapcm testing. These auttmrs also showed IngestIon
the role of milk
At about the
greater significance than inhalation for cows, and discusse’j
Ingestion in the 1311 contamination of people:
same the, Dunning (1956) pblished aetlmds for the ca!cuiatiun
—.-— —.. . L
!
I P“--”’”
(Rclllson et al., 1974). TWO populations were examind, the first befw
children in Utah and Nevada who lived in areas exposed to fallout from testing
tn the 1950s, ad the second, other children fran the same states awl frm
Arizona, who were considered unexposed. Tamplln and Ffsher, whose 1966 report
fscfted by Ralllson et al. (1974), retrospectfvelycalculatd average doses to
s1] children in Utah betwen 1952 ami 1955 to have been 46 rads (maximum dose =
120 Ws}. Later Mays, cited by the BEIR 111 report (liAS,1980), estimatwl the
wer~dose for expos@x!children to have been 120 rads, rangtng from 30 to 240
rti$. There was, however, no slgnlftcant Increase fn t~roid neoplasla in
expoW children Wn capered to the unexposed children. Benign thyroid
ne@asms ~re found in 6 of 1,378 exposed subjects and in 10 of 3,453 unwposed
comtmls. Noaullgnancles were found in the exposed group while 2were found in
tb%e * wre not apowd [Rallison et al., 1974).
hdine-lsl was found to be present in urfne samples of inhabitants of the
Ramhall Islands exposed to fallwt fn March, 1954 (Conati et al., 1975). At
~out the sam tl~, In 1955, Van Mlddlesworth, using a scintillation detector
for atemal mnltoriq of the thyroid, found detectable leve~s of 1311 fn two
peoplcat the Nevada Test S~te
presence of 1~~1 In lumen thyro
●l. (1957) pwentad mrt hman
Van Ulddlesworth, 1956). He also reported the
ds frua autopsfes. Soon afterwamh, Cuwur ●t
data on l~l! In thyrofds frmm autopstes.
-s.
—.—- -—
22
administration to a nurslq wanan (!411ler and
al,~ 1955), and to cows (Comar and Hasserman,
W*S shown. In the last case, the radfofodine
to provfde jnformatton about the secretfon of
studies in people and large animals, however,
Heetch, 1955), to goats (Wright et
1956; Lengemann and Corer, 1956)
work was part of a study designti
flssfon products fntomllk. These
*re not pblfshed until some time
after the transfer of 1311 throu’ghmllk was uscxfas u method to irradiate
● “ nursfng ndce (Rugh, 1951).
After these early reports on the radloblology of radloiodfne, studies on a
national ad international scale contfnued. The primary pathtayof 13~1 to
people was recognlzul as being aWrspherm@etation*Hllk+PeopI e, and pre-
dfetfve models fbrthis arxfother patlways have been developed (SoItiOt,1963; Yg
and Thmpson, 1%6; U5 ~C, 1977). The prominence of t~ thyrofds of children
In the 1311-flk pattuay was recognized. A major symposlwon radfofodine was
held In 1963 (8ustad, 1%4), In *fch were presented maw papers on these and
othar topics.
$tudfes on theenvfmuwntal aspects of radlolodfne have ccmtfnued to the s
present, not so -h because .,-~ :cR~!P#&j c~ncprn wer Short-term fd~lout fr~
nuclear tmpwns, but mre so beause of the potentfal for radtofodlne releasvs
froa nuclear reactors. Investigttlons into the chemfcal nature of the radto-
hdlne have been made to Identify r~dfolodtne species In nxl~ar r~a:tors
(p@lletleret al., 1978a, 197*), and evaluations of other Iod!nc twtor~$,
1291 for ex~ple (Soldat, 1976), have b~en aft*
. . “— -— —.... - .. A —
.
—.....,.
● ✎✎ ✍✍☛ 23
gland or released to
metabolism, has been
the body tiere they Influence growth, development, and
understood for some time (Salter, 1940). Hence, when
raffolodlne became avaflable In the late 1930s (LiYfngood and Seaborq, 1938), it
found pranpt utlllty amngthyroldologtsts and physic~ans who used the fodfne
fSOtope to trace patlataysof the element in the body first In rabbits (Hertz et
al.. 1938) and then in rats (Perlmen et al., 1941). Much of the early use was
relat~ to diagnostic evaluation of patients with t~roid disease (Ham~lton and
SOIW, 1940; Hertzet al., 1942; Hertz and Roberts, 1942a; Ham~lton et al.,
1943; C@tmbymi McCune, 1947; $oley and Miller, 1948; Uerneret al., 1948; ati
Skanse, 1949).
lheco~entratlonof rtifolodfneby the t~rofd fn developing young was also
studfed. Thyroid glands were shown to take up 1311 in utero In the rat
(@*8R ati Evans, 1941), the mouse (Speert et al., 1951), and the hunster
(Wsborough and Sedy, 19S1), and prior to hatching fn the chfck (Hansborough
●nd Kaht, 1951). The human fetal t~rofd also was shown to concentrate radto
Wineearly In ttsdevelopmnt (Chapman et al., 1948a). Not only was the
trmsfe~of rediofodfne across the placenta recognized, but so, too, was Its
Wement across themaunary gland, as evidenced in studies on lactating and
swkltrq ●ice (Rugh, 1951).
After tkseewly reports, considerable infomatfon contlnu@ to be produced
on themettiollsm of 13110 prhnarlly because of the use of the radfonuclirte!n
aadlcfne and fn physiological and end’ocrinologlcalstudtes. The w
Of Vm radlolodfne uptake test In diagnostic medicine resulted in
UfMkr$t~ndiq of how 131$ was handled by the thyroid and the ho~y.
Mrold uptakes of hman nroaates (2-3 days of age) -re first
despread use
ncr Pds P4
—. . . ..._____ —:.- 1-
. . . ... . . . . . . . .
Radiobfolodcal Effects
In the 1940s, there was already tnuchinformation shout the effects of high
dines of Wlofodfne. Radlolodfne was used therapeut~cally fn the treatment of
&aws’ dfsea~ to reduce the amount of thyroid hormone prod~ed by the hyper
utfve t~roid (Hertz and Roberts, 1942b, 1946; Chapman and Evans, 1946; Soly
8nd Hlller, 1948; Hoe et al., 1950; Chapman et al., 1948b) and in the treatmnt
●“of$&rold cercincna (Sefdlln et al., 1946; Keston et al., 1942; Frantz et al.,
1944; Sefdlinet al., 1949; Rawsonet al., 1949; Trunnel et al., 1949; O;byns
and~loof, 1951)* Radloiodlne was also used In the treatment of angfna Pc-
torls ad congestive heart fcllure In patfents wlm had normal thyroid function
(Bltqert et al., 1948; Freedbe~ et als, ~950~; the r-ultant ~pothy~oidl~
decweasd cardlw functton.
Uftbt* uceptlon of the Pattentsmentiond above who were tr~ated for
heut disease, most exposures of normal thyrofd t!ssue to r~dfofodlne were made
la aperfmental animsls. High doses were required to fnterferewtth normal
tmfd functfons; therefore, tlw thyroid was considered to be fairly radio-
reststant {Merren, i943)o Eapwiii-estG Mfic?:fitly h!gh dines & @fnfMln@
l~frtlu Imrmgenic capability of the thyroid, and can result tn effects that
are sfdlar ~ tlmse seen after thyro~dectcxnyor as a result 04 twroid disease
?nvolvfng 1OS$ of thyrofd functton. Hypothyroid tndivfduals often manifest a
n-r Of CWdltfO~, lnCIUd~~ dry, cold, and coarse Sk\n, Cotrse hdfr, #
decre~u fn swatlng, wakness, lethargy, constipdt~on, =ig~t 9atn, MPIW, ad,
2’1
iv ..-.... .— _
(Flndlay and LeBlord, 1948; Go?dbw et al., 1950). ‘
admlnlstratlon of a single large dose of radiolodine.
~e effectsof chrontc aposure to radfoiodlne in
hese studies in~olved the
sheep were reported by
8ustad et al. (19S7a) and Marks et al. (1957), Exposures ranged fra 0.15 to
1800uCi ~311 per day forperlods of a few months to 4years. Corresponding
tot-l doses tothethyrolds ranged fran 400-800 rads to over 100,000 rads, at
dose rates of 3.4 rads/mti to 30,000 r~sh~. At the lowest level
? (0.15 ~t/day) thyroids showed no damage,
i
whfle those at the hfghest levels were
ablate. Exposwes at intermediate levels resulted In slight, moderate, or
f Severo thyroldal effects, depending on the dosage, and the tin of exposure.
Alttmugh Impalment of t~rold function was the effect of Interest in this,
study, srnthyrold tdenows and a fibrosarcoma were also reprted (Bustad
eta],, 1957b; MarkS and Bustd, 1963). Slmllar effects maybe expected In
euthyrold wple after cawparable doses. Exposures required for ablation of Lhe
hwnt~rold were found to be 30,000-40,000 rads (Goolden ati Uavey, 1963).
Thwoid Meoolasla
Although 13’11was being used In the treatment of thyroid cancer in the
1940s, tbrewts apparently no work being done on the role of radloiodfne in the
prOdWthn of thyrofd cmcer tt that t~me. This ~s not to say that the
possfbtllty of the carc!n~enic nature of rad!olodtne was being ignored,
however. A 1946 edftorlal fn the Journal of the hnerican Wwiical Association
(AflO~S, 1946) statd that
L *+.. .— --.-——. -.--.: .—:
. 26
Nickson (1948), in djscussfng needs for protection for those wotiing with
radlofodlne, pointsxlout the need for understanding the potential for cancer and
other t~roldal effects that radiofodfne Possessde Later, Twnnell (1949)
warned●
The possfbflfty of thedeveloPm@nt of neoplasms fifteen
or twenty yea- after radioactive iodine therapy should
preclude its use fn all but elderly or otherwise bad
rfsk ptfentsg
tirneret cl. (1949) also brwght out the concern for subsequent thyrofd cancer:
It fsfkared by some that later malignancy maybe fmhcd
In thethyrold as a result of the effects of a radioactive .
egent .... Thfs ... rtifation ... makes ft lfkely that
malignant degeneration fn the gland may appear fifteen to
tfhen601dberg and Chalkoff (1951) report~ the production Uf ilwTuid turn=
In rats given 1311, they also mPhsized the need for caution in usiW
rtiloiodine fnmedfcfne. .
In 1950, Ouffy and Fitzgerald (1950) reported that several young patients
with t~rold cmcer Id received prior Irradiation. Later, Simpson et al.
(19SS) and Clati (1955) reportal on the association between relatively low x-ray
tXWWeS ad t~rofd cancer In chfldren. Subsequent studies, too numerous to
reference tn thfs report, but well represented by the long-term follwu~s of
Ulnship ati ROSVO1l (1970), ll~p~lmann et al. (1975), and $lodan●t al. (1971),
fndlcated that exposure of the thyroid gland to x-irradiation durinq fnfan~y anl
l&--..,———--— -- —- .—.:
- ,,
● ✎ -.,0
<’“
childhood $ncrmsed the fncidence of t~rold adenonas and cancer. rol10M-IIP
studfes on ~perthyrold patients treated with large doses of ’311 also
Itifcttd thet t~rotd denaxss and c~rclnanas were produced (Oobyn$ et al.,
1974).
The csrdnqenlc potential of 131I was also noted fn animal experiments.
Goldberg and Chalkoff (19S1) gave 400 uCI ~3~1 to 10 rats and found 2 thyroid
tlmmc
kn~acb [1963) sumnartzed the results of several studies done in the mid
1950s @ oarly1960s, Inuhlch the thyrofd carclnogenfilsof 1311 W~S
ewlwtod M capared with that produced by x-frradfat~on. in thtt review,
l~livageo~ld~~ to be l/10cs effecttve M x-r~ In the prductlon of
cancer, f.~, 10,000 rads frm 1311 would produce In rats the same level of
effects 4s 1000 rtis frm x-my.
Dfffermees fn Rodioblolmlc Effectl\eness. Obserwatlons of other t~roidal
effects fra diverse snimal studies support the ●x~stence of differences in
effectfvwtess of the two radlatlon exposures. McClellan ●t al. (1963), for
ex@xple, c-pared the hlstopathloglc changes In Irradiated thyro{ds of sheep
●nd esttmated 1311 to be &out 1/20 as effective as x-rays for the Prmiuction
of hf$tologtc ●ffects. !nmice, where the Inhtbttlon of goitrogenlc stimulation
‘was used as an Indexof radtation effect, 1311 was 1/4 to 1/2 C% effective as
x-rays (Uallnder and Sjoden, 1971). Data frcxnrats, using the same model as a
test for effects, suggest 13~1 to be ab~t 1/8 *S effecttv~ ts x-~rrad!at~on
(*ieg*t al., 1970). Another study in rats, using thyroid turwr{qenes(s as the
pfodut Ion of edenows, but of qual ?ffee!iven~$t
nmas (Lee ●t al., 1!!8?). Unfortundtply, &nimal$
-—. . 1- —-----
,.. –_
,t
,
,
I
?
Iri(
,
[
1
years After Irradiation when 62 percent of them were st111 alIve. Had the
anlmal$ been allowed to 1Ive longer, the productIon of tumors may have changed,
W the relatlve effectiveness of the two radiationsmay have been shown to be
dlfferent.
Differences In effectiveness In the production of t~rold gland effects by
varlws Iodine isotopes have also been observed. In studies of mice whose
“t&rolds tmre Irradiated wfth 1311, 1321, or x-ray (Ualtnder et al., 1972),
X-irrtdiatlon cnd 1321 (phystcal half-llfe = 2.2 hours) resulted tn slmtlar
effects that were grater than tkse fran 1311. In rats, usfm the Inhibition
of goitrogenests to cuapare the effectiveness;f 1311 and 132[, 1311 was
sbm to be only 1/9 as effective as 1321 (Book ●t al., 1980). Klasso\skli.
●t al. (1971), wtuJcanpared the thyroldal effects of 1311 with mixtures of
1311, 1321, Cd 1331 (p~sjcal half-ltfe = 21 hours) In rats, concluded
that the htstologlc effects of 1311 were only 1/10 to 1/25 times as pronounced
as tbse from the radloiodinemlxture. Studies conparing 1251 (physfcal half
llf@=60 days) and ~311 indicate that up to 20tims nmre rads are required
fn 1251 than fr~ 1311 for the s~e suppression of tracer uptake or
Inhlbttlon of goltrogenesls (Gross et al., 1967; Grieg et al., 1970; Vickery and
Ufllfms, 1971).
knee, It can be concluded that these radiations indeed have differences In1
their blologlc effectiveness. The differences, apparent between x-irradiation
and 1311, and amng radlofodines with different half-llves ad emissions, can
be consfderul to be related to the dose rat? and the dose distribution of the
Irradfatfons. X-#rradiatlon fs given at high dose rates ati results in tmifor~
~rradf~tlon of the thyroid, lodlne-132, a $t@rt-lived rodioiodin~, irra’!iat?f
St high dose rate>, and since its misslon$ are fairly energetic, !her~ ff fd~””
ly wifona irradiation, lodin~-131, with Its loqPr hfllf-llfelrr~~~t~$ a! *
-=’.-=s====- ‘-+”L%, ? -.
*. – .*,
Iwgr dose rat~ *M In a spatial!y less wlfona mlnnpr, tlmugh Ivo!tiblynot trl
too great an extent In smal1 rodent thyroIds. Jodlne-li?5,has an @ven 1o-r
dott rate, and, because of Its mfssfons of lowr emeqy, Irrtifate$
non-tmlfomly wfth higher doses to krmnogentc ports of thyroid fol1lcula~
cells ml lower doses to thefr ruclel (Gritq et al., 1970).
FOI1OWIW ●xposure to fallout from a thermnwlear test In the Paclftc In
1954, the exposed population of the Marshal1 Islands mhiblted a proportion of
thymtd dfsorders, Includlng neoplasla, much higher than would have hew
expectd. ThQ Nershallese, however, In Oddltlon to ~311 had also received
tOtd bOdy g- exposure end thyroid glati exposure to stuwt-llvml radloiorjln~s
133]-1351 (Conad et sl., 1980). The short-l~ved redioiodtnes have not been
$tudlod for carcinogenesls, but other ●ffects have I@lcated thet thetr
effectlvewss $huld be greater than thet of 131[, as discussed above, thdt
1s, they ect mre like x-lrradietlon.
lodlne-lZ9 (Tp ● 16 milllon yearn) ts another fiss~on produc~ radlo-
Itilne. It ap~srs to not have been considered en envlromental or health rfsk
until later In the nucle~r age, Wen Its slgnfflcance es e Foblem of s~nt
nslear fuel processing and storc~ or dtsposal uds reco~~zd. Its im~rtanc?
In tlm erwlronxent as ~ cont~lnant of food Items ues rwiewed by Soldat (1976}
and W@ et al. (1917). W toxfclty of 129! Is Ilmlted, however, because of
!ts vc~ low hilf-llfe (g@, therefore, low rultodctfvlty pr unft me$$) and
Mw%e the thyroid can conttln only a flnlte qwntlty of lodin~ {RoM , IQ77,
1981).
/“/
. .
l~A.— ....._. ____ ._. _
31)
-.:
Estimates of Thyrofd Rfsk. Several attenpts have been made to predict the rlsti
of thyroid neoplasla from Irradiation. Beach and Dolphin (1962), using data
frm several studies, descrtbed the thyrofd res~nse to dose u lfnear, corres-
ponding to a rate of 1.7S thyroid malignancies per S00 rads to the thyroid, or
34 maltgnanclesj106 persons/rad. Stnce the time at risk MS taken to be
?Oyears,thei rannualrisk forthyrold malignancies can be expressed as about
Id/106 persons/rad/year. Hempelmann (1968), with data fran other studies,
predictd a risk for mallgnanctes of O to 5.5 cases/106 persons/rad/year,and
for t~rold nodules of 38-53 cases/lt)6persons/rad/year. Dolphln (1968), fron
other data, estfmted the rfsk for thyrofd cance~to be 100/106 persons/rad,
or, conslderirg the time at risk to be 20 years, 5 cases/106 persons/rad/years
The Nattonal Acadanyof Scfences BEIR Report (tUS: 1972) estfmated the risk of
t~roid cancer to be of the oder of 1.6 to 9.3 cases/106 persons/rad/year.
Later, the Nattonal Academy of Scfences (NAS, 1980) estfmated the rtsk of thy-
rofd cancer to be approximately 4 cases of t~rold carcfnona and 12 cases of
thyrofd adenoma/106/rad/year. In the Reactor Safety Study (US NRC, 1975),
abs~~ute rtsk$ for ttyrofd malignancies aml nodules, based u~n d Iarye number
of studies, www estimated to be 4.3 and 8.1 cases/106 persons/rem/year,res-
pectively, or a total of 12.4 cases of t~rofd neop]asla/106 persons/rem/year.
For caparf son, these nu~ers can be canpared to an average annual Incidence of
t~rold cancer for both sexes, all ages and races conbfncdp of 3.6 per 100,000
fOr locations represented fn natfonal surveys (NCI, 1975).
Since these estimates for t~roid neoplasia are prlmarlly derived fron
external Irradfatfon, est~mates for 1311 risks should be lower to account for
the differences fn effectiveness of x-ray and 1311, as cffscussedabove.
rw
~ likelihood of hypothyrottjfsmfs low at Iowcfnses. %xon et al. (1977)
cued thfMf!Cil~ literature and found thdt llypot~roi(~fw wds r~nortd
Q
l-- .._—. *.—
G1
r-. .. -..0
31
followl~ doses above 1000 rads for external Irradlatlon and 20 rads following
1311 exposure. Frotnthe revlewof Maxon et al., the BEIR Conmittee concluded
that the tlmshold for the fnduction of ~pot~roldism was 2000 rads in external
exposure and 5000 rads for 1311 (NAS, 1980).
Means of ProtectIon
The t~roid gland’s affinity for Iodine not only makes it the target organ
for radioiodine but also provides a mans by which the thyroid maybe protected
fras rdloiodine. The administration of stable iodine suppresses the uptake of
rtdfolodfne by the thyroid by diluting the radioactive ~sotope and by invoking
hmeostatlc mechanisms tithln the gland that rduce the anount of iodide taken
upby the gland.
This so-called ‘blockingg abtlity of the t~roid gland was demonstrated soon .
after 1311 b-m available (Perlman et al., 1941), when rats were given
1311 wltheit~r Oo5 mg iodine as ~tassium iodide, 0.03mg iodine, or no
bdlne, that is, carrier-free. Subsequent peak uptakes by thyroid glands were 2
percent ad 7 percent for rats that received 0.5 orO.03 mg iodine, respective-
ly. Rats receiving only the tracer had peak uptakes of 65 percent.
The blocking abjli~ of the thyroid has been the subject of many paptm,
including those by Mans and Bonnell (1962) and Blum and Eisenbud (1967). The
Mtional Council on Radiation Protection and Measuranents (NCRP, 1977b)
ractnmended the adequate blockfng dose In cases of radioiodtne exposures to be a
dally dose of 130m~lltgrans of ptasslum iodide (and half that ivnountto
infants under one year of age). Admlnistratlon of the blocklng agent was
rec~nded to occur at thyroid doses of 10-30 r&js or more. lhta frm a later
study (Sternthcl et al., 1980
-’●
suqgestt?dthat thyroldal uptake can he suppresst+
—_..— -——. ..—- —
:*I I 327 ,,
-.
i’?,, markedly by a sfngle dose of 30 mg Iodfde and that suppression cwld be main-
tafnedwlt htillydoses of at least 15mg. Because there are a number of{ir;1 adverse condftfon8 fncludfng t~rofd abnonnalltles that may develop after
eXpOSUM to large quantities of stable iodfne, as dfscussed by the WRP (1977)
and Sternthal et al, (1980), care must be taken fn fts admfnfstratlon.
.{
j,.!
.“) !
iii
t
f.
i
,
i
●
—... ——J.,
● -r--+-
VI. RADIOSTROMTIU?4
M!m!4uStrontfum-4K)Is the important strontium Isotope fn radioactive fallout.
It has a 29-year physical half-life and It and its sbrt-llved yttrium-90
daughter eatt beta partfcles. Strontium behaves Itke calcium; hence, bone is
the prfncfpal site of 90Sr concentration. Unlfke the other fission products
dfscussed herefn, strontium has a long resfdence tfme arrJslow turnover rate
once It fs incorporated fnto bone mfneral, characteristics that enhance its
railobfologfc .sfgnfficance.
lhenuxabolfsm of radiostrontfun, ffi similarity to calclm, Its concen-
tration fn bone and transfer tomflk &re all documented ~n the early 1940s.
The effects were also fmplled In those papers that suggested its use in the
tr.etment of bone cancers. The carcinogenic potential of radlostrontlum was
documented by the late 1940s, after havfng been determined In animal studies.
Isotopes of strontfum~re known to be ccsnponentsof fallwt by 1950, and
reports of fsllout 9@r appeared in the open literature In the early 1950s.
Long-term studfes on the uffects of low levels of %r *an (and cootlnu?)
at several Itiratorfes
of this radfonuclide on
Environmental Pathways
to Investigate ati better understand the late effects
bone ml bone marrow.
Isotopes of strontlu were fdentlfled by 19S0 to be potential contributors
to Unvfromental radto~ct~ve contiunfn~tlonfran the detonation of atomic
mapons (Glarnstoneet 41., 1950), and subsequently 9%r was documented in
th operiliterature 9s a component of fallwt (Elsenbud and Harley, 1953,
1956). %n, the global n~ture of th fallout was di$cussrd u!th regard to
.
R. - ..-.- --=====e:?”~ - —--- —---+
---’——%E3—
uorld-wide meteorology (14achtaet al., 1956). In ddftion, fn~dsurmefitsof
go$rco~entr~tlong In foods &nd h~n tfssues Hremade, and the potenttal
haztdto people was conslderd (Libby, 1956; Elsenbud, 1957; KUIP et ~~.t
1967; lan~~, 1%8),
Work lnOthe early 1940s (Erf and Pecher, 1940) had reported the secretion
Of WWntiun fnto cows’ milk. $qne other aspects of environmental behavior O(
rediostrontlum, nanely, the uptake of the radlomcllde by plant roots, had+.
slso been Investigated In the 1940s (Jacobsen and Overstreet, 1947).
Studies on the transfer of %r arulother flsslon products tnto milk
were begun In the mid-1950s (Comar and Uusseman, 1956; Lengemann and Cmar,
19S6), Ingestion was considered to be the most slgnlflcant route of human
#$$lmfl#tlonof 9%F (Langtwn, 1960), ati dai~ products were considered the
prlaery sourceof 9@r In the diet (Russell, 1960). The transfer of ~%r
fmtbe atmosphere to diet to man was reviewed by a nwnber of autkrs (e.g..
Uesseman et al., 1965; Bennett, 1972).
●
*~~~~fc p~t~~y~
Even though som Investlgattons Into the nwtabolism of strontlwn were done
ew]ler (for instance, MCance ml Ufddouson, 1939), ft was not mt~l the
Wal~eblllty of radioactive stronttum (B9Sr) that Its aetebol~sm becam
Under%tuod. Wch Of th ~perlmentdl use Of rti~OStrOflt~umwas as a
substitute for calcfuB.
Etrly $tudles demonstrat&l the
their wtabolfc ~thways. Pecher
ttssw upteke of tn.jecttd8%r ml
two r~dlonuclt~s, After 24 hours,
Wel1
+--- .,. .
● ✍✍✍
✌
In th skeleton,as was 33 percent of the ~9,Sr. Pecher also notd the hf~!h
yield and ease ofcomtl~ of 89Sr, cunpared to 45Ca. Pecher and Pecher
(1941) also demonstratai Inmlce the abtltty of rad~ostrontlum to cross the
placenta and the muaary gland In mice and concentrate In young bones. Erf
and Pecher (1940), dsmentloned above, collected milk fran two cows fnjected
with 89Sr, and recoverul 11 and 8% durfng the*4.5 days after Injection.
Other studtes Included Investigations Into the bfltary secretion of
cslcfum and strontfum (Greenberg and Troescher, 1942), the fnfluence of growth
homoneon stronthns @osltfon (Ran and Relnhardt, 1942), and the effect of
parathyrofd extract on strontIun metabolism (TwedY, 1945).
TreXuell ●t al. (1942) perforaedmetabolic studtes of neop]asms of bone
usfn$ 89Sr, tilch was found to be taken up by growing bone ad by osteogenic
twer tlssws, Posstble therapeutic use of radioactive strontium was
mentioned (Tmadwell et al., 1942] as a means of”fncreasirq radiation dose to
sffectti areas, thtt is, as an adjunct to ongoing tnerapewtfc mettudologies.
~ asshllatfon of a nixnberof fission products and heavy elements, and
thelrdfstrlbution and retention were studied in rats byti~ilton (1947). For
8%rand90Sr, he found that 5 to 60% of an oral dose was absorbed, that
65% accumulatai in bone, aruithat they ~re exponentiallyeltminatcd with a
half-tlnwin the body ofmre than200 days.
Coppet al, (1947) also !nvestlgated themetabollwa of radioactive stron-
tf~, along with yttrium, cer!um, and plutonlum, Of these, only strontium was
absorbed apprecfshly frcm the gastrotntestindl tract. Absorption of strort-
—- .. ... .— :_.. _ - . ._
36●
formation. ?le~thergrowth nor decreased dfetary calclum or phosphors had an
effect on the nustabollsmof yttrium, cerlum, and plutonlum. Strontium was
eliminated with a half time of 3-4 months, much more rapidly than the elimina-
tion of yttrln, cerium and plutonium which had half-times of 1-3 years. Work
fn rabbits also Wicated that uptake of irtiected8%r and 90Sr by the
~skeleton was greater tn young animals than in old ones, and was inversely
relatd to calclum levels in the diet (Kidman et al., 1950). e
The transfer of radfostrontium from the lung into the bloodstream was also
investtgatai In rats (Abrienset al., 1946). Immediately after 30-min exposure
to8&ss SrC~2, nsmthan50% of strontium that wasdeposlted in the
lungs had been renoved fron the lungs, and 25%Was in the skeleton. l~e lung
burden was red~ed by half over the next 30 mfnutes, and after8 hours, only
2.5Sof the Inttlal burden was fn the lungs. Over 85Zwas skeletally.
deposited. Direct skeletal uptake of inhaled ~apons fallout radiostrontiwn
In -t anfmals was demonstrated in 1952 and was found to be preferefltlally●
concentrated In growing bone (Smith et al., 1952).
Altlmughtk behavlorof strontiumwas qualitatively shnflar to that of
C8]CiU, It was shoun In experimental animals that the ratio of strontium to
CdlCiW tn tissues was different frma the ratio of the two elements In the
diet. TO better quantify and predict the differentiation in tissues or
excreta, Comar ●t al. (1956) proposed the term “Strontium-Calcfum ~semed
8atto” (OR),where
-—. ..’
i
The OR denotedthe Individualtissues,excretions,or p~siological processes
Involvedin the preferentialutilizationofcalcfum over strontium,and when
less than 1, expresses such a Preference For ~ample~ the ~bone-diet for
rats on
causing
dlscrlm’
u coumercfaldiet was 0.27. The OR did not imply action by the tfssue
the discrimination. Instead,to denote the p~siological process of
nation in a gfven tissue, the authors utilized the term ‘Strontium-
Calcium Discrimination Factor” (OF). The product of the DFs equalled the OR.
That strontium was preferentially discriminated against by the placenta
was fbund in beagle dogs (AEC Project No. 6, 1958). The ORfetal bone-diet
was 0.31, based upon data from two pups, a value somewhat lower than the
o~dult b~n~d~etof 0.4-0.5 of mature beagles (Della Rosa et al., 1972).
The metabolic studies of radlostrontium intensified when its potential
toxicity as a conponent of radioactive fallwt was recognized and studies on
Its effects began. The radiobiological significance of strontiuu~tabolism
was discussed in reviews (Thompson, 1960; Loutit, 1962; ICRP, 1972) and
sylaposta(Lenihanet al., 1%7; Goldman and 8ustad, 1972).
Radlobfologfcal Effects
The tuaorigenic~ility of radiostrontiumwas recognized in the 1940s.
Strontium-89wasdescrfhad as a “producer par excellence of bone tumrs” by
Brues et 81. (1947), iAo reported that tumor development in over 3000 mice was
approxinwtely pru~rtional to dose and to time, with a latent period that
Itself was related Invemely to dose. Such a scheme was slwwn to flt data
that were av~ilable for human radlun dial painters. Besides bone tumrs,
*plastfc aneala dmd m~loid ntaplasla were cmnmn at necropsy (HnJPs ?t fil.,
1949)0
37
k-—= -– . . . . _-.. .._A.,__ ..
---–. ..: -— .._.
38.
,
‘!
The bone tumors that were producedwere sfngle and multiple,and, parti-
cularly in rats and rabbfts, there were many Instances of metastasis. Doses
raqing frun 0.05UCi/gmto 5.0 vCf/gm resulted in “considerable mmbers” of
tuners. t40stof them (61%) appeared fn long bones (Lisco et al., 1947).
Otlwwo* done at this time centered on the effects of 8gSr on preg-
nancy and the transfer of the radfonuclide fron mother to young via the
‘“placenta and manunarygland (Ffnkel, 1947). Anfmals exposed to 89Sr ineutero
or prior to~aning showed retatied growth, malformed long bones, anemfa and
bone cancers.●
In a symposiumon radlostrontlum (Goldman and Bustad, 1972) effects of
injected,ingested,or Inhaled90Sr In beagle-dogs~re reported. Studies
on 90Sr-treat~ beagles began in 1947 at $lrgonrte National f.aborato~,and
were subsequentlyexpanded into several large progrisnsat the the Unlversfty
of Utah, at the Universityof Californiaat Oavfs, and at the Lovclace
Foundation tn Albuqueq@. In these prograns, the beagle dog raaf’ned the .
expwlmental subject of choice (Book, 1980). The most significant ●ffects in
animals given adequate exposuresto Wr halve been hmis of him, iiwt!y
f)stf?osa?%~o and myeloprolfferativedfsorders,which includesboth neoplastic
hanatopofeticdfsease and preleukemicconditions.
All specfes that have recefved sufficient90Sr have developd osteo-
sarcaas, fncludirq dogs (pool et al~? 1972, Doughertyet al., 1972; Flnkel et
al., 1972), nmnkeys (Casarett et al., 1962), pigs (Clarke et al., 1972),
rabbits (Vaughan and Uilliimson, 1969), mice (Nilsson, 1972), and rats
(Moskalev et al., 1969). Myeloproliferatfve disorders have been noted in dogs
(Dungworthet al., 1970), pfgs (Clarke
al. , 1969). ?lfcedeveloped lynphatlc
(Nilsson, 1972).
——-— -————.
.*. ---* .
.-;3
.“
.:..
J
->
., !
lw~ arisl~ adjacent to bone have been noted in several specjes tredt~~j
ulth~sr. In fnice,squmous cell carcinomas were reported to ortginate In
the Imd palate and sebaceous gland of the external wd~to~m~atu$ (N~lssonl
1972). Squamouscell cwctnmas were also reportd in the maxillary sfnus in
rats (Moskalev et al., 1972) and In the lining of fnternaland external ear In
~~bltg (VaughanAnd Wlliamson, 1969)? Squamous cell carcinomas of the
gl~lva have been found to be importantlater-occurringeffects in beagles
exposed to g% (by Ingestion)from prior to btrth until 18 months of age
ati obaerwd forltfe (Parks et al., 1980). For the dogs, theglnglval tumofi
probablyreflect the results of continual Irradiationfrom 90Sr In teeth
that Ismatntalned at a high level, since teeth slmwa slower turnoverof
90Sr than does the rest of the skeleton (Della Rosa et al., 1964).
Fortunately,too few humans have been exposed to rtilostrontiumat high
enough levels for the risk of neoplasia to be esttmated. 8asd dn radium dial
painterrfsks, however, Mays and Lloyd (1972) estimatd risks frun ~OSr.
~~rbest estfmstes for the 50yr risk to an ind~vidualfor bone sarcoma frun
one red were (! x 1) i W-6, using a I{nparmodel, and (4 * 4) x 10-lO?
using a dose-squared model, The current ICRP (1977) estimate of r{sk for
g%r-lfke radtatfon Is 5 x 10-6 per ran. These numbers can be conpurti
with ● natural Incfdence of Aout 5 x 10-4.
.— .—
II()
VII. UADimsiuu
5!m!!uYCestw=137 is the significantceslum tsotope in radioactivefallout. It
Is abet~~dogmnis asaltterwith a 30-year physicalhalf-life. Since it IS
similar to potassium in itsmetabollsm, 137CS Is distributed throughout the
soft tissues of the body. Its relatively uniform distributionthroughout soft
‘~lssws brings about a declining whole-bodyexposure that Is relativelyshort-
ltved, since 137CS is not retained In the body fw long periodsof time. It
WISily WeS through
ical Investtgattons.
dose ca~nent uttl
food chains and has been the subjectof many radioecolog-
Cesium-137was not appreciatedas a sfgnlflcantfallout
tt
Enviromental Pathways
The ffrst re~rt of
was found to be present in people in the mld-1950s.
cesfum-137 in people cam after Its presence was noted
inmewrenents of *ole-body radioactivityby gamma sp?ctronetry (Miller @
Harinelli, 19S6). The persistenceof ~37Cs In the human body despite its
rslattvelyslmrt blolmical half-llfewas explainedby continued exPOSure Vla
the diet; 137Cs was present in meat and mtlk powders. The presence of
137C5 jnpeqle and in various foods and its relation to 4% waS reported
by Anderson et 41. (1957) who calculated that the significant contributors to
dietary 137CS wre dairy products. Dafry products and meat were considered
to be the primary sources of fallout 137CS, while inhalation and fngestfon
of drinking water were said to contribute rnfnimallyto the 137CS body burden
(Langh~ and Anderson, 1959),
The extent to which btiy burdens of 137CS reflect dietary ~mut was
be$t @ampllfiad ~n two human populations who were fitt~]eend of the
●
● ✎✎ ✎ ✎✎✎
envtrorssentalpatMays for rediocesIum: atmosphere*lfchefr’reitieerLaplaruler
(Lindenand Gustaff$ofi,1967) and atmosphere*1Ichen+caribouEskimo (Hanson,
1967). In these populttlon$,seasonal tnflumx?s ondi~tdry practices
~esultti In large fluctuationsIn ‘37CS burdens? Many other environmental
as~cts of 137CS ~re sunsnarizedby Davis (1963) and were addressedby
others In a symposfwnon radiationecology I
Metabollc DathwaYs
In the 1940s, flsston-produd radioces
Aberg and Hungate,1967).
urnwas administeredto rats
(Mmjlton, 1947). Absorptionfrom the gut was 100 percent; Its dtstrlbutlon
was thoughout soft tissues, with 45 percent depostted in muscle,and It was
retained In the rat with a half-timeof 15 days. Inhaled radioce!
redlly absorkd fran the lungs.
~emttabolism of 137CS was studied later in rats and several
animals by Hood and Comar (1953), *O found a stmflar wide and fa
ium Wds
faml
rly uniform
dlstrlbutfonthroughout the body. They also found that 0.2 to 3.5% of
~~fai~~~r~ 137CS -S tra~ferr~ fr~ pregnant rats to fetuses In late
gestation (at days 17 to 21, respectively) ~th a f~frly constant tissue
concentration of 0.063 dose per gm regardless of fetal age. A dairy cow ~s
.shom to secrete 1= of an injected dose of 137CS into rnllkover a 30-day
perfod. Fron an oral dose of 137CS, 10S was $ecret~ intom~lk in 30 days.
The ●ntrance of 137cs into an!mal tissues ~S pf~mar~lythrou9hthe
$ngestlonof contuslnataY foads. Abso~tion of cesium frau the gut is clme
to 100Z tn monogastricanimals (Rlchmti, 1958), but f$ generally only 5tM to
$m In rumin~nts (McClel\an et al,, 1961; Ua%$eTnan et al., 1961). Th?
rPdIKml tb$orptfon, along with the high fecal”to-urtnary r’8!\oof Pirr?[ti
‘.
—
-“——-”””
42
-.!...~r
!-9
,[
s
,1!
.
—-
.
137CS characteristlcally seen In ruminants (Hood and Comar, 1953), probahly
relates to the kfrxfand greaterbulk ofthefr diet (5avis, 1963).
CesluISbehaves In amanner that is p~sfologicully somewhatanalogous
POtassiua.Hence, cestum is distr~butedthroughoutsoft tissues, and can
expose those tlssws wfth beta and gamma Irradfatfons. Unlfke the bone-
●.seekfngradfostrontfw, however,retention ~s stswt (that fs, elimination
to
is
rapfd), ufth tissue exposure (and dose) declirtl~ with a half-period of about
2.5 to 5 mmths In people.
8ecause137Cs intake results fnunlfonn exposureof all tfssues, fts
sfgnfflcance cs a hazard to the most sensltlvetfssue must be balancedby its
dfstrlbutlon●nd dilutfon fnto all tfssues. ~eslum-137,Ifke tritium,fiich
also ts Untfomly
l~uryasuell as
dfstrfbuttitn
carcinogenesls
the body, possesses the potential for genetic
in sensitive tissues.
RadlobioloqfcEffects
Beglnnlng in the 1960s, the long-term effects Of 137Cs were studied In
beagles at ~nne Rational i.obur~iury,es ~.,.~.. ....J...-4~. ~~ gf~p (~977@).
Sfxty-ffve beagles fn a llfetlne study were given single intravenous
i~ectfons of 137CS ufth dosages ranging fran 1.65 t04,31 tit 137Cs/kg,
anong their age groups. Oestructlonof bone marrow resulted in 25 deaths
wfthfn 2 months after l~ectlon. Cancers were the main cause of dt?athof the
40dogs that survived acute effects (up to 12years post-injection), and
accumul~tedfron 700to 1609 rads. C~ncers acccuntmlfor 20 deaths,and
cancers were also found in t!ssues of other dogs dy~ng frmn other causes.
Meuroffbrosarccswa,i tumor of the ncrwe she~th that is rare In doqs, was th~
most frequently occurrtng cancer, ond WS found in n IJf the ~~ doq$.
●✎✍✍✍✍✍
☛ ✎
43
,Al$o nentloml h the ICRP Report (NCRP, 1977a) w?re 54 13- to
./ .: 14-month-oldbeegles fnjectedufth 137CS dfIdstudfed at the InhalatIonf/ ToxicologyResearch Instftute. A later swwnary (ITRI,1981) reported that 114/ mute deaths w’e observed, and 20 of 32 dogs that survfvecl acute effects died
:i of cancers. Eleven were still alive. Oosages ranged frun 0.9 to 4.0 IKl
i 137cs/kg ~ti total doses ranged frun600 to 2200 rads.
-.,-
*-4
--—.”.
r-—–—--------- --‘-
* *
,
VI11, PLIXONIUN
W!!!!Q!
Plutonluta-23is a man-made alpha emitterwfth a 25,000yr half llfe.
For plutoniumthat reaches the blood, Its target organs are bone and liverc
Inhaledplutonium may affect the lung as well. PlutontumIS an efficient
carcinogen.
*- Theutet~olisn of plutoniumati its productionof bone tumors were inves-
tigated in the 1940s. More elaborateand sophisticatedstudieson the
biologicalsignificancewere begun In the 1950s and 1960s and continue. Its
effects on bone, liver, and lung have been d~”nstrated in a number of
laboratoryanimal species.●
EnvironmentalPathwaw
Host of the ~nfonnationon plutonium in the “environmentthat evolved
during the 1940s was relatedto monitoring environmentalmaterials near
nuclear installations(Stannard,1973a). These investigations were centered
primarilyon aquatic environments and biota.
Alpha activfty was found in animals trapped In the fallout zone of the
1945 Trinity sbt severalyears after that detonation.
assumed to be plutonium-239(Olafsonand Larson, 1963).
released to the envirorsnentfrun atomic weapons testing
presenting serious potential for injury if inhaledor
The activityWS
By 1950, plutonium
was recognizedas
ingestedtiand calcula-
tions of hazards fran world-wide contamination by plutonium were also made
(Glasstone et al., 1950). Dogs and sheep intentionally exposed to the radio-
active fallout fran weapons tests in 1951 were found to have 239Pu in their
lungs (Smfthet al., 1952).
44
---
●
~_–.. .
● ✎✎✎�✎ ✍✎
ln19S7, studies u8reundertaken on uptake by
dW8ct Inhalationof plutonlumIn the radioactive
well ●s after inhalationof plutoniumresuspended
depositionon the ground (Stannard,1973a). Rats
45
the body and retentionafter
cloud after detonation as
by wind action following Its
and dogs were exposed durl~g
pJSSege of the radioactiveclwd, khtle dogs, sheep ad burros Wreex’posed
for a long post-eventperiod of up to 160 days at several down-wirrllocations.
The r@sults Imllcatd that dogs exposed to the cloud passage at the time of
detonation had higher plutonlun burdens than animals expos~ to resuspended
plutonium for long perfods of time, even though the animalsexposedto the
pa$siq cloud were not exposed to the highest airborneconcentrationsat
ground level.
8ecause of concern about plutonium in the environmentfrom atomic weapons
and$ later, the nuclear fuel cycle,considerable informationhas been
publlshed on tts radioecology(Olafsonand Larson, 1962; Stannard,1973a;
Healy. 1975; MEA, 1976; Friedman,1976; Hanson, 1980).
Plutoniumhas a low volubilityin water and biologicalfluidsand tends to
Mnonaetlle fn soils ml ~hermedla. Hence, plutonfumis much less likely
to move through food chafns to man than fission products discussed heretofore.
Nonetheless,plutonfum in the envfronnent contfnues to be a timely topic, in
view of fts role In the end of the nuclear fuel cycle.
Metabolic Pathways
Because plutonium played a major role in atomic weaponry, considerable re-
search on fts metabolism and toxicology took place in the 1940s. Studies in
rats on the distribution and excretion of plutonium in var~ous chcnfcal status
were made followlng intravenous (Carritt et al., 1947) or intramuscular
~“–””— —-——. - .—
t~ections (Scott et al., 1948), or after oral ~min~strat~on (H~llto?lt
1947), From each mode of exposure,roughly two-th?rd$of the asslmllatwl
plutonlum deposited In the skeleton,Wile the llver generallyreceived the
next highest concentrationof the radlonucllde.
plutoniumwas found to be so poorly taken up fran the gastrointestinal
Jrict that only 0.007 percent of an orally adm~nisteredamountwas absorbed.
Of that whfch was absorbed, 65 percent was deposfted In the skeleton. Removal
fromtb skeleton was ve~ slow (Hamf?ton, 1947).
Intravenously l~ected plutonium had Its trfghestfmnw’dfateconcentration
in liver and spleen. Leter, It was translocatedto bone (8rues et al, 1947).
The dtstrlbutlon and elimination of pluton~um was also studied after rats
were exposed to It by Inhalation (Scott et al., 1949). After nose-only ex-
posures of several mtnutes’ duration, most of the radloactlvtty was In the
head ●ml lungs, but after 4days, the lungs containedmost of th~ resfdual
actfvfty. The lung concentration declined uver the cwrse of the 64-day
study. After 64 days, 12 penent of the plutonium inhaled as plutonlwn
nitrtte was In bone, cunpar@ to 0.4 per cent of that inhaled as plutonium
dfoxlde.
ThemetXolisam of plutonlum was also studfed In 18 hunan subjects l@ected
wtth tracer doses of Z39PU In 1945 and 1946. As revfewed by Ourbln (1972),
bone am llver were shown to be the principal sites of plutonfum
PlutonlM nttiollsm In pregnant rats and mfce was also stud
1947). A very wll fraction of t~ected plutonium was found to
the placenta.
Stdles of factors Influencing them?tabol{wn ~nd depo%
Sevtral rwjlonuclldp~, lsoto~s of plul~nf~~, strontf~n, yt
tiposltfon.
ed (Flnkel,
mve ,across
.
-----. 47
utre done In rats at about the same time (Copp et al., 1947). Un?fke stront-
iw, but llkeyttrlum andcerlum, plutonfum showed behavior that -s
unaffected by the age of the rats mder study or by calcium or phosphrvs
levels In the diet. Thls suggested that, while strontium followed the
patbrays of calcium mettiollm, plutonfufn,yttrium, and cerium did not, and
that they =re deposfted in the skeleton by other mechanisms.
Ametbd of protection fron plutonfum toxfcfty was proposed by Copp et al.
(1947), who suggested that where contamination had occured, the dtet could b~
altered to dfminerallze the skeleton. By then demineralizingthe skeletonvia
dtetarychmqe, a protectivelayer of new bone would be laid down over the
plutonfum.
Subsequentstudies In rats showed the uptake of chronic, orally admi’n-
tsterd plutoniumto be 0,003Z (Katz et al., 1955; Ueeks et al,, 1956).
Uptake of plutonlun given as a single dosage to pigs was 0.00?% of the
athlnisteralmount (Us@s et al., 1956).
In pigs thenmtabollsm of plutonium after Intravenms, Intragustric,or
Intratrachealdmfnistration of plutonium nitrate was aiso srudied. Wiile
liver and skeleton were the principal sftes of plutoniun deposition, the quan.
ti~ absorbed depended on the mode of dminfstration. Less than 1 percent of
the administered Pu was in the skeleton and lfver up to 2 years after lntra-
gastrlc administration or fntrdtrachea] dosing. After an intravenous dose, 50
to 77 percent was in skeleton ad l~ver; tn thfs case, however, the plutonfum
nftrate solution was buffered wfth citrate, tiich may have contributed !O the
ci~fference(Busted et al., 1962),
StOv&r et al. (1959; 1962; ]968) studied the lo~-te~ ~tabOl~~w of p\!J.
tonfum in dogs whose SIeletal dn~ soft t!$$w r~t~nt~o,~Of injected plu!ontun
ues dotmfncd. Theneteho?ism of Inhaled p?utontum also was sturfted in
beagle dogs (Belret Q1., 1962) $ndlcat~ngthat not only its chmlcal form wds
Iaportan but, so too, ws the pdrtlcle sl?ewlthwh~ch It was assocl~t~.
That 23W ues not only reta~ned In the lungs but also continued to eCCmJ-
lM8 to bronchftl lymph nodes sug~std that these oryansmay also be
fmportanttargqts for plutonium toxfclty.
● . The met~ollsm of plutoniumwas reviewed by Langhan (1959). More recent
revleus Includethose by Vaughan et al, (1973) and &tfr (1974).
RadloblologlcalEffects
The effects of plutonlum-239were noted In*the 1940s.
studtes, “plutonf$m”,as ft was called, for hfgh exposures
Based on anhnal
*S descrtbed as
bchg shflar to effects of acute whole body radlatfon. Results of acute ex-
POSWS$ ma presented by Bloom (1948)and Fink (19S0). Plutonlsm for chron it.
●xposwe was seen to mmlfest Itself,with progressive lfver damage ~nd bone
tmrs (8rueset al., ]!?47). 7hemajorlty of
ia (62%) in mfceo rctt, @iti rabblt~ UCLUIIW---- -.4
1947). * aspects of the early toxtcologlc
nmj (1973b).
bone tunnm producd by pluton-
In the Sp!tie(Lf-<c e: 3?0,
studies were revfewed by Stan-
in the 19SOs ard later, the radiobfologlcaleffects of plutonlum wre
Studtd tn a variety of laboratory animal s~cles, Includlng mice, rats, rab-
bits, pigs, srnjdofjs. Many aspects of plutonium toxtcltywere presenttxlIn
vtrfous symposlc (Thcmpson, 1962; Hays @t a],, 1969u; Stover and Je@, 1972;
Mealy, 197S; J~c, 1976; Urenn, 1981). Other overvie~ were al$c publi$he~
(Hod~ ●t al., 1973; Rslr tt al., 1974; NAS, 19?6), as ~re blbllogrtphf~$
(Thompson, 1976; tf~~le ●t al. , lW).
r
i
●
,
,.. -..O<
~most significanteffects of plutonium exposure we bon? cancers, With
IWQ M prodwd In mice (Finkel , 1953, 1%6; Flnkel and 8fskis, 1?62) and
dqs (Jee et al., 1962; MY$ et al•~ 1969b] that were fqjectedwfth plutonium.
In dogs Met Inhaled 23*u (PhYsfca~ half-lffe = ~~ years), bone cancers
wn also Importantcwses of death, but some dogs also died of lung carcinma
and from fsmmnftts snd ffbrosls (ITRI, 1980). 5tudfes of dogs that inhalti
~Spu, ~~of Wan are still under study, showed radlatlon pnmmonltis and
ffbrosis m Importantcauses of death, with som tncfdent lung cancers (lTRI,
19$0). ?lanyother Imcstigaton also reported bone c~ncers and lung cancers
In 9 n-r of specfes exposed to plutonium, as revleued by 8alr (1974).
Nher bone changes were noted fn dogs (Taylor et al., 1962, 1972) and pigs
(Clinks, 1%2) injected with plutonium. Lfver degeneration was noted in m
(Fltiel W Bfskts, 1962) and dogs (Taylor et al., 1973). Acute hmatolq
changes ~ al~ noted fnmfce (Finkel ard Btskfs, 1962), pigs (Bustadet
1%2), ad dogs (Dougherty, 1973). Early lung changes
f- fnhaled plutonfum in dogs uere noted (Park et al.
The role of these WWI @twr anfmal studies In pred’
populations have been djscussed (Thwnpson et al., 1972
(fibrosis, metaplas’
1962).
ctfng risks to human
EMlr, 1974; Thcxnp$on,
Ce
Ctl
al ,
a)
.
Recmtl y,
deaths tn the
Uppr ltaits,
27 (2=) bone
Thompson @ li~chblz (1980) estlmutd the number of cancer
Unltax! States due to fallout plutonlum. They calculattithat as
B total of 125 deaths would wcur~ wfth 64 (51%) lung cancers,
cancers, and 34 (27%) liver cancers. They also noted, however,
that the possibilityof no cancer deaths fron fallout plutonlum was not
precluded,9t
Plutoniumhas effectfve radlologlc characteristics,yet It inefffcf:ntly
moves through environmentaland met~olfc pathways. Hence, plutonlm can be
described as having a hfgh toxicfty, but a lo~hazard rankfng.
●
51● ✎ ✎☛✎ ☛
IX, URANSU4
$!!!!mY
Naturally occurrfng, uranfum has an aceedfngly low half ]ffe and enlts
alpha particles. It Is concentrated fn kidney and bone. Uranium has been the
stiject of toxicologicalstudy for many years, and its nephrotoxicproperties
were known d century prior to work on its radiobfologicalsignificance. The
chemfcal toxicf~ to the kfdnqys of natural uranium overrides any potential
for radtobiologlctoxfcfty. Only wfth high speciffc actfvfty isotopesof
uranium is the skeleton at rfsk for subsequent radiation-relatedcancer
developwmt.
EnvlroranentalPathwavs
Uranium (23W, 234U, and 235U) fs naturally occurring and ts
dlstrtbuted ubiquitouslybut variably throughout the earth’s surface. It is
present In water and in foods, so that small quantities are ingested daily.
The KRP (?975), fron data of Uelford and Baird (1967), reported an average
daily intake of 0.9 pfcocuries of uranium. Approximdtelyequai mounts (ubout
22 pe~ent) of dietary uranium were derived from each of four food groups:
cereals ami grains; meat, fish, and eggs; green vegetables and fruits; and
root vegetables. Abwt 7 penent was fran dairy products,and 2 percent was
frcsndrinking water. Inhalationwas cortsiderfxlto be avery minor route of
assimilation.
The dose rate to bone fron natural uranium was calculatd to he about
12 uam/yr (tCRP, 1975). This value amounted to only about one-tenth of the
(
I
52
naturally occurrfng fnventory of uranium. Its subsequent transfer to man can
be expected to be like that of uranfum in nature.
Metabollc Pathw@s and Effects
Wanlumhas a long history as a subject of toxicologic study. Hedge
(1~?3), Inrevfewfngtk history of uranium poisoning fran 1824 to 1942, cited
over 350 references. Later researchwas reviewed by Yuile (1973),*O
dfscussed experimentationin animals, and by Hursh and Spoor (1973),who
sumaarlzed data on people. Most of the early sfidies,and the later ones as
well, for that matter, anphaslzedthe nephrotoxic effects of natural uranium.
In general, hazards fran uranium were consid;rd to relatemore to its
cheadcal toxicfty than to Its radioactivity.
wfth ? p~sical half ltfe of.4.5 x 109-years,
actfvfty of about 0.33 mfcrocurfes per gram.
This is because uranium-23f3,
has a very low specific
However, there was concern that
Tong-tens exposures of sufficientduration,
mfght pose a radlatfon hazad, such as that
dial fndustrywfththe radfum dfal painters
Martland, 1931; Aub et al., 1952).
●particularly enriched uranium,
whfch occurrti in the luminous
(?lartlandand Humphrfes, 1929;
Uork In the early 1940s (Tannenbaumet al., 1951) showed that tracer doses ‘
of uranium-233 as uranyl nitrate fnjected subcutaneously fnto mice and dogs
were prfmarfly In the skeleton one and two months afterwards, respecthely.
Formfce, 67 percent of the total 233U in the body was In bone, fine 14
percent was in the kidney and 1 percent in the liver, For dogs, 90 percent of
the total burden was in bone, 3 percent In kidneys, and 3 percent In liver.
That bone and kidneys were the prlnclpal sites of Wanium acclvnulatlunwas
also found by Neuman et al. (1’3411).
Even tloughmost of t~ retifned burden Inmlce MD3 rats was fn the
skeleton,tk total awunt ret~lned In the body was small (Tannenbaum et al.,
1951). LQ$$ then 10 percent of the I@ected quantfty of uranfum rema~ned in
the body l-?mnths tfter the lnjtctlonof non-toxic quantlttes, Wwn the
l~ectd qwntl~of uranium was at t hfgher, toxic level, a.smuch as 40
percent ues retained. The destructive ●ffects of uranium on the kidney
(Barnettati Wcalf, 1949) wre respnslble for the altered pattern of
urantw excretion In the latter grwp.
The toxlcl~ Of wanium cmpounds was studied In a number of animal
species dwlng the 1940s ml later. Admfnfstratlon of uranlumuas by
Iqestfonml Inhalation as well as byotherrnodes of aposure, and the
dumtion of Indlvfdual studies ranged franonenmth to tuo years (Voegtlln
ad Hedge, 1949 Ond 1953).
Thesl@iflcant target of natural uranfum toxicfty fs the kidney. Even
thugh there ts long tem retention of wanfum by bone, administration of
sufficient uranl!m to result tn radfatfon effects would be dffflcult. This Is
O@#use doseges wf vanium that are weii !tii :*,&fi.~~;: !: ~=mafy~ ~~
produce skeletal ●ffects would still be high @nough to lead to toxic, fatal
●ffects on the kidney (Bernwd, 1958). It fs the4.5 x 10-9yr half-lffe
ad the IW spectf~c cctlvlty of uranium-23EY(*bout 0.3 mlcrocurles per qrdm)
that llmlt tb ant of redfoactlvlty that can be incorporated {n the body.
Even uhen nat~tl uranjum !s enrfch~ beyond the normal 0,7% ~35U (h~lf-llfe
w 7.o x 108 yrs), as IS the c~se for urantum tMSM a(r~mfcweapom (e.g.,
%~~ 23%) and uran!um refftor fuel, the IW s~wcffic activtty of
S? mfcrocurfeg pr 9rm for ?~~l would llm!t the rw!ifft!on mp?$ur’?.
53
._ -.—r
i 54 -
I
I
! S&@18tal effects can be apected to occur wtth high sp?cfffc actlv~ty
J uranium isotope such as 23~ (half-life ● 1.6 x 105 yrs; speclffc acttvlty
;1
~iw 10 mflltcurles per grem) or 232U (half-life= 72 yrs; specfflc actlv!ty =
37.7 curfes ~r gran).f[
inded, f~ect ion of each of these two uranium
ii lSOtopes ues shorn to produce bone cancers In mfce (Flnkel, 1953). Natural
1 uranium, ho~ver, showed no Itiuctionof bone tumom.1t c-’
●
f
——--,.,.
-.-— .——— -—
REFtREHCES
Abr~, R., M. S. Slebert,& M. Potts,W. Lohr,and S. Postel,1946,
J4etabollsaofInhaledFissionProductAerosols,U. S. Atmic fnefyy Report—
CH-3485, Wllversityofchtcego. Cttd by HcC~ellmet al. (1972).
Mm%, C. A. mdJ. L $onnell,1962, MmlnfstrWlon of stable Iodfne *S t
nesn6 of mlucfng tbrold Irradlatfon resultlng frcm @halat!on of redfoactlve
fodtw, Mealth P?ws. 7: 127.
Anderson,E. C., R. L. Schlch,u. 2. Fisher,andll,Langhant,19S7,Rad!o-
actfvlty of Wople and foods, Sctence 12S: 1273.
ko~s, 1946, Edttorial, J. ~r. Med. Assoc. 131: 140.. —- ~—. .--
ho~$, 1954, The M-bab ml world opfnlon, Chalrmsn Strauss’s $t~tmaent on
Peclffc tats, Bull. Atantc Sclentfsts 10: 163.—“-. —. .....-.----
2-.: —_—_--_ _ ---- . ----
.. —._ —___
56
AEC, 1953b, Fourteenth Semiannual Report of the Atom<
July, 1953.
c Energy Commission,
AEC, 1955, Eighteenth Wnlannual Report of the Atomfc Energy Cunmfssion, July
1955, Appendfx 7, p. 147.
AEC, Prqject No. 6, 1958, Annual Progress Report, School of Veterinary
?bficlne, University of California, Davis, p. 24-25.
Aub, J. C., R. D. Evans, L. H. Hemplemann and H. S. tlartland,1952, The late
effects of internallydeposited radioactive materials in man, Medicine 31:
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