NUREG/CR-1658 The Environmental Behavior of Transuranic Nuclides Released fronn Water Cooled Nuclear Power Plants Prepared by V. T. Bowen Woods Hole Oceanographic Institution Prepared for U.S. Nuclear Regulatory Commission \N o\ ^^ Q\4 NOTICE This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, or any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for any third party's use, or the results of such use, of any information apparatus, product or process disclosed in this report, or represents that its use by such third party would not in- fringe privately owned rights. The views expressed in this report are not necessarily those of the U.S. Nuclear Regulatory Commission. Available from GPO Sales Program Division of Technical Information and Document Control U. S. Nuclear Regulatory Commission Washington, D. C. 20555 Printed copy price: $3.75 and Notional Technical Information Service Springfield, Virginia 22161 m -□ m 5 □ BL/WH 3- D D □ m o a NUREG/CR-1658 RE The Environmental Behavior of Transuranic Nuclides Released from Water Cooled Nuclear Power Plants Manuscript Completed: September 1980 Date Published: March 1981 Prepared by V. T. Bowen Woods Hole Oceanographic Institution Woods Hole, MA 02543 Prepared for Division of Safeguards, Fuel Cycle and Environmental Research Office of Nuclear Regulatory Research U.S. Nuclear Regulatory Commission Washington, D.C. 20555 NRC FIN B6153 W HOI DOCUMENT C'XLECTION ABSTRACT E n V i r been that mote conta Point thi s t i n s near taken Plymo show two a waste be ve onmenta analyze of the from re m i n a t i Point has bee from n Mills to from t uth are slight, reas bi r a d i n ry prof 1 sample d from a Pilgrim actor ou n . No s or P i 1 g r n clearl ear Main n e Point he efflu as, howe but def ogeochem u c 1 i d e s i t a b 1 e . s (wa bout No. 1 tf 1 ow edime im 1 y evi e Yan show ent c ver , ini te ical coul d ter , the rea s ha nt s have dent kee . rea anal biot , re stud eas sed two ctor ve u ampl sho in Bi ctor . F a sa acto ies ily i m e n t s reacto . No n e q u i V es fro wn rea severa Ota so conta rom th mples r cont of the be car an r si wate ocal m ne ctor 1 se far mina e Ma f req amin fate ried d bi tes r sa ly s ar M con dime mea tion i ne uent atio s of out Ota) noted mpl es hown i 1 1 s t t a m i n nt CO sured only Yanke ly pr n. I 1 ong . and have , and re- reactor one a t i n ; llec- from when e and ove to n these -1 i ved woul d 1 1 7 TABLE OF CONTENTS Abstract List of Figures and Tables Acknowledgements Introduction A. Background B. Overview of study Materials Methods Results A. Discharge Data B. Environmental Data Discussion A. Nuclides Studied B. Release Patterns C. Environmental Samples 1. Millstone Point, Conn., Reactors land 2 2. Wiscasset, Maine, Maine Yankee Reactor 3. Plymouth, Mass., Pilgrim 1 Reactor Summary and Conclusions Appendix - Table of Common Names and Taxonomic Detail References page 1 m II vii li ix page 1 II 1 II 2 II 3 II 5 II 6 II 6 11 6 II 13 II 13 II 15 II 15 II 17 II 25 II 37 II 46 II 50 II 51 List of Figures and Tables in the Order of their Appearance page Millstone Point Reactor #1 MONTHLY DISCHARGE ACTIVITY 8 II II II Jt2 " " " 9 Maine Yankee, Periodic Discharge Activity 10-12 Millstone Point, Daily Discharge Activity 16 Millstone Point Collecting Stations 21 Millstone Point, Conn.: Long Island Sound Surface Water 22 " " " : Sediment Cores Radiochemistry 23 " " " : Environmental Samples - Biota 24 Maine Yankee Collecting Stations 31 Wiscasset, Maine: Surface Water from Montsweag Bay 32 " ", Area: Surficial Sediment Radiochemistry I 33 " " " : Sediment Cores Radiochemistry II 34 " " " : Environmental Samples - Biota I 35 " " " : " " -Biota II 36 Sampling Locations around the Pilgrim Nuclear Reactor, Plymouth, Mass. 41 Plymouth, Mass., Area: Water and Sediment Radiochemistry 42 " " " : Environmental Samples - Biota I 43 " " : " " -Biota II 44 Biota Samples for Comparison to Plymouth Area (Table 14A and B) 45 Appendix-Table of Common Names and Taxonomic Detail 50 TABLE 1 II 2 II 3 II 4 Figure ! 1 TABLE 5 II 6 II 7 Figure 1 2 TABLE 8 II 9 II 10 II 11 II 12 Figure 3 TABLE 13 II 14A II 14B II 15 VI 1 Acknowl edgements We could not have proceeded so far in the present project without the support and cooperation of Mr. Philip Stohr, of NRC, whose help it is a pleasure to acknowledge. The work at Millstone Point was facilitated by assistance from Dr. William Renfro and Dr. Ralph Briscoe; that at Maine Yankee was comparably helped by Dr. David Sturniolo , Jr . of Maine Yankee and Professor C. T. Hess of Univ. of Maine. The collecting by, and analysis of samples at, WHOI were carried out by a number of colleagues, among whom special mention should be made of H. D. Livingston, J. C. Burke, D. R. Mann, A. G. Gordon, L. B. Graham and W. R. Clarke. All of this help is gratefully acknowledged. Substantial amounts of data, reported here as essential to the understanding of this program, were obtained as parts of other projects, most prominently that funded by the Dept. of Energy under contract DE-AC02-76-EV-03563 . A005 and by the Environmental Protection Agency as part of the Mussel Watch Program under contract with the University of California; we are grateful for this support and for the freedom with which these data can be used. IX THE ENVIRONMENTAL BEHAVIOR OF TRANSURANIC NUCLIDES LEAKED FROM WATER-COOLED NUCLEAR POWER PLANTS INTRODUCTION A ser to mo 1 ease plann prese ments e i t h e a 1 1 r i proac ident menta s i m i 1 ments seem which to as appea known each 1 ous del , d to ed di nt ig and r the butes h to i f i a b 1 exp a ri 1 1 repr to ho each certa r bet el em relea probi e the be aquati sposal noranc of the chemi of th this p le tra erimen es amo esente Id w i d gener in w h a ween t ents w s e d mi m that havi or c e n V i s or a e both exten stry e loca rob! em nsuran t and ng the d, est ely, a a 1 i z a t t s i m i he tra hose r xture. faces a of tran ronments s the re of the t to whi f the re 1 e n V i r lies in ic el erne by the c behavio a b 1 i s h i n s well a ion brea 1 a r i t i e s n s u r a n i c adioisot nyone t suranic , wheth sul t of geochem ch this lease m nment . the us nt rele omparin r of th g those s those ks down in g e el emen opes ar rying radi er in acci istry i s c ateri A ve e of ase a g the e var gene cond . It chemi ts an e al s to pred onucl ide the cou dents, i of thes ontrol 1 e al s or s ry promi each pre s an env di ffere ious rad ral i zati i t i n s u is also cal beha d those compon i c t , or s re- rse of s our e el e- d by pecial sing ap- sently iron- nces and i e 1 e - ons that nder val uabl e vior may better ents of Pursuit of this approach has led us to study a substantial number of releases of artificial radionuclides, ranging from worldwide and close-in fallout from nuclear weapons tests, the liquid effluent releases from fuel reprocessing plants in Great Britain, France, and the USA, leakage from solid waste containers dumped at sea, to the discharges from water-cooled nuclear reactors used for electrical power production. In this last project, we have been sup- ported partly by the U. S. Nuclear Regulatory Commission, and it is this work we are reporting here ing water stream. Altho some smal 1 of th ed to is 1 i pi uto el eme cl ass that produ fluct or ev c n s i espec i nter ugh t trans amou e coo nept ttle ni urn, nts a of are cing uate en as derab ially actio he f uran nts , ling uni u ques and s am pera nly oper wide cert 1 e V of ns irst ic r det wat m 23 tion vi r eric ti on seco atio ly i ai ne al ue some f th of the a d i n u c ermined er stre 9 and i that t tual ly i u m and s. Bee ndary f ns of t n ways d at th i n hel of the e n u c 1 i se pr Tides 1 arg am, a ts da he ov all curi ause u n c t i he pi that, e tim ping biol des r ocesses , these ely by nd prob ughter erwhelm f such urn, res of this ons of ants, t if the e of re to esta g i c a 1 , el eased cert are the u ably pi uto ing p heavi ult f orig the d he ra y cou 1 ease blish or s a i n 1 y produ r a n i u 1 arge ni um repon er tr rom t in, i ay-to tes Id be , wou time edime res ced m CO ly r 239. dera ansu he s n pr -day f re pre Id b con ntol u 1 1 s in in very ntent estri ct- There nee of r a n i c econd ocesses power 1 ease di cted , e of stants , g i c a 1 , MATERIALS Through the good offices of Mr. Philip Stohr, NRC, we received from the operators of the two reactors at Mill- stone Point, Connecticut (Millstone Point No. 1 and No. 2) and of the Maine Yankee reactor at Wiscasset, Maine, samples that represented their periodic storage tank dis- charges for parts of the years 1977 and 1978. These were replicates of the discharge samples that the operators collect routinely for assay of major radionuclides. In the case of the Millstone Point reactors, the samples were adjusted to represent the monthly discharge experi- ence. The series we received began with January 1977, continued through the year (without samples for August or September), and through the first four months of 1978. In the case of Maine Yankee, we received a separate sample to represent each discharge event, the volume representa- tion being adjusted for those of the various tanks dis- charged. Discharges occurred as seldom as once or as often as eleven times a month. The period represented by samples we have so far analyzed extended from 20 June 1977 through 25 March 1978. As di stone t i n s cri te smal 1 Febru No. 1 treat sul te ders nucl i detec pies charg No. 2 ly cl scusse Point relea r i a K vol um ary an , howe ment w d in a of mag d e s in t i n 1 i ze we e. Th , sine eaner d below. No. 1 d sed woul For tha es of sa d March ver, an as i n t r very su ni tude , the d i s imi ts . receive is incre e the No in its d our ata , d be t rea mpl e 1977 a d d i t duced bstan in th charg Begi n d was ase a 1 scha i n i t i was t rathe son , -- 25 di sch ional . As tial e con e , br ning incr ppl ie lant rge t al exp hat th r 1 arg we beg ml pe arges stage shown reduct centra i n g i n g with M eased d to b had pr han we ectatio e a c t i V e (by an by a r perio from Mi of was in Tab ion, c 1 t i n s them t ay 1977 to one oth Mil oved to had ex n, fr ity c ur en s k i n g d. B llsto te di le 1, ose t f tra 00 cl , the 1 i ter 1 ston be s pecte om Mi oncen viron 11- tra- mental for etwee ne Po schar thi s two nsura ose t n , th per e No. ignif d . '■L onl n tlie int ge re- or- nic our e sam- di s- 1 and icant- It wo able d i s c h ent s that did r cern trati of th being arran ent s cries uld obv to supp arged ,w tream. the sto epresen and hav ons tha e b i 1 assess ge prop tream, out to i u s 1 y 1 ement i th a This rage t t the e prov t ente gical ed. U r t i n so tha be un be of these series woul d anks w major ided a r the and se nfortu al sam t this dertak con sam of both ere sour n es envi dime nate pi in par en. sidera pies r sampl e have being ce of timate ronmen ntolog ly, we g of t t of t ble val epresen s of th given N correct the nuc of the t , for i c a 1 re were q he cool he i n V e ue to ha ting the e actual R C c n f i ly sampl 1 i d e s of nucl i de c 1 a r i f i c 1 a t i n s h u i t e una ing wate s t i g a t i ve been tanks efflu- rmati on ed and con- concen- a t i n ips ble to r efflu- n still In addition to the discharge samples provided by the re- actor operators, we obtained series of samples of or- ganisms, of sediments, and of water, in the environments of these reactors, and of the reactor operated by Boston Edison Co., at Plymouth, Massachusetts (Pilgrim No. 1). Most of these samples we collected ourselves but some were provided by the environmental survey teams of the reactor operators. In the Wiscasset area we were sub- stantially assisted, through the good offices of C. T. Hess, University of Maine, Orono, by the people and faci- lities of the Darling Center, of that university. A list- ing of these environmental sampl es , together with their status in analysis, was included in the Progress Report submitted October 1978 under the subject contract. As discussed there, some additional samples have been ob- tained; additional analyses have been performed under an extension of the subject contract, and substantial num- bers, both of samples and analyses, that are highly rele- vant to the interpretation of the NRC-supported work, have been completed with support from other agencies. METHODS Our radioanaly >, , ^^ . ber of publications. 'onroc mav ho ""^oful tical methods have been described in The following summary list of "ul : a num- We engage regularly in analytical intercompari sons organ- ized by the International Atomic Energy Agency, the U. S. National Bureau of Standards, or the Department of Energy. Published reports of our performance in some of these may be 1 i sted as fol lows : 1. Fukai, Ballestra and Murray, 1973. ]_n Radioactive Contamination of the Marine Environment (IAEA, Vienna), pages 3-27. 2. Noyce, Hutchinson, Mann and Mullen, 1976. j_n Proceed- ings of International Conference on Environmental Sensing and Assessment (Inst. Electr. Electron. Eng., N. Y. ) paper 19-5. 3. Volchok and Feiner, 1979. A radioanalytical Labora- tory Intercompari son Exercise, U. S. Dept. of Energy, Rept. EML-366, 43 pp. Other performance information is either summarized or ref- erenced in the methods papers cited above, or in the var- ious articles reporting and analyzing our data, that are cited in the Discussion below. RESULTS Ql§9[}§r9§_9§^§ • The an out in No. 1; deal in 60co, 244Cm; sampl e of the the an vol ume of the period a 1 y t i c a three Table not al For date alytica of the total repres 1 results on the discharge samples are set tables: Table 1 dealing with Millstone Point 2 dealing with Millstone Point No. 2; Table 3 Maine Yankee. „Qata,are presented for SSpe, 137CS, 238pu, 239,240pu,'^24lAm, 24^Cm, and 1 nuclides were, however, measured in each the shorter-lived nuclides, data are shown as f collection of the sample. In each case, 1 result has been multiplied by the total discharge represented to yield an estimate activity of that nuclide discharged in the ented . Environmental Data: For convenience, the data referring to the environmental samples, water, sediments, and biota, as well as the Fig- ures showing respective collection locations, are inserted in the Discussion sections concerning the various reactor environments. Since most of the radionuclides that we have measured are not unique to reactor operations but are present worldwide as the result of atmospheric testing of nuclear explosions, we have included in the biota tables, comparison data referring to relatively nearby samples that we believe have experienced only fallout contamination; these data derive principally from the Mussel-Watch Pro- gram (Goldberg et al , 1978, and Bowen et al , to be pub- lished) supported by EPA. In the order of their insertion and tables are as follows: Figure 1: Millstone Point Collecting Tabl e 5 : Mill stone Water. Tabl e 6 : Mill stone chemi stry Mi 1 1 stone in the text, these figures Stati ons . Point, Point , Conn Conn. Long Island Sound Surface Sediment Cores Radio- Table Fi gure Table Point Environmental Sampl es - Biota . Maine Yankee Collecting Stations. Wiscasset, Maine: Surface Water from Montsweag Bay. 6 Table 9: Wiscasset, Maine, Area : Surf ici al Sediment Radiochemi stry I. Table 10: Wiscasset, Maine, Area :Sediment Cores Radio- chemistry II. Table 11: Wiscasset, Maine, Area :Envi ronmental Samples • Biota I. Table 12: Wiscasset, Maine, Area : Envi ronmental Samples • Biota II. Figure 3: Sampling Locations around the Pilgrim Nuclear Reactor, Plymouth, Mass. Table 13: Plymouth, Mass ., Area : Water and Sediment Radio- chemistry. Table 14: Plymouth, Mass ., Area : Envi ronmental Samples - Biota. Table 15: Biota Samples for Comparison to Plymouth Area (Table 14A & B). o CO o +1 +1 o O '^ V£> r^ ^ — , n r-< r. o O <- a >£> Ol cr> «3- +1 o in +1 vo r- f— t LJ O O +1 o 00 o +1 CVJ o •a: CO o en a. ■•- 00 tj o •a- 1 — CM »«• Q. • F r-i o ( ) fO +1 +1 +1 w CTi CTl <3- 4-) O r- C OJ u IT) >^ CJ O o ro O ro oo f-H o o o ^ ^ f— < ID +1 +1 +1 +1 +1 + 1 + o f— t in f— 1 in CO 00 o . CM r^ CM CTl u> «i- ro «3- ro O un CO oo' o CO o o T3- 00 f— * »-H +1 +1 +1 +1 +1 +1 +1 o OJ ro cr> •a- o 1^ o ' C\J CO »d- 'S- E o •n CM ro * r-. o CO E a: .-" t/l ^-^ C_) •-- (_> ^ <_>o ro E O I— ( C-) o d o CD o +1 +1 +1 +1 +1 +1 vo o in t— * o •a- CM r^ t— t 00 in o 00 d CM o CM O o in f-H m o f— t CM l-H O ro . . o o O o o o +1 +1 +1 +1 +1 +1 .—1 o un in o »— ( «* o ro o CO w—t (NJ f— t ro *— f CTl r^ «3- O o o o o o O O o o o o o o +1 +1 +1 +1 +1 +1 +1 n o CM in in ro r^ o ro ro in in 00 eT> a- t-^ o «a- O o o o o r-H o o o o o o O o +1 +1 +1 +1 +i +1 +1 r~ in ^ in CM in m t-H «»- p-t 00 ^ ro ro o c o +-> u o 0) o ■•- O E O) -,- C_J Ll. o o ^ E O o o o o o CM O f— < a> ro o o o O o o 4-» u 01 i~ +1 +1 +1 +1 + 1 +1 +1 ro r—i in o CM in in in r^ ^ ■♦-> o •■- /I > •— " — I CI t- ro o o (O vo o o tn •a- o o CO o o +1 vo d CO ro r^ »— » f-^ «a" •— ' CO ^ •-' CO •-' '-' 4-> s- C TJ (O o cr Qj a. - 00 .^ 0) >, 3 ••-> . . . s- >, c C3> a. •»-> > o c: JU n re 3 3 3 a> CO VO (O o c +1 +1 V) m 00 o o V PO U3 f— t ■4-> CVI f— 1 01 O + 1 o o +1 C9 a: c/1 Q. •■- OO O ro E o •a- CO o o •a- O 0-) o ro o o in o O o +1 o +1 o +1 o +1 t— t in vo in CO o o +1 vo .-H CD O +1 o •— ' •— • o + 00 o o C\J P^ a; o. E la o c o CD _. - <_) <_) O E U3 Li.<_) o DEO eg o o +1 o +1 o o +1 en vo CD +1 00 CO o o o o +1 vo Ol S- s- o >. o (U , J ^?, in 13 S- Q) .— o +-> o+J •r— >co r— — n C\J CVJ "3- ro en ro en vo o CM 00 PO 1-^ vo ro en en tn p- en en r^ 1 — en en en 00 r-. cn +J-0 C C "3 O "3 O) 00 .— en E «t ■ 00 d +1 to o o o +1 00 o CM O O o CO o o o o 00 o o o o o o o o +1 00 o o •— 00 o o o o +1 o +1 n 00 o *— 1 o O Q PO Cr- o C_) « o UJ —J Q <_) -^ o o CO O to .a tu J3 4-> 4-J 4-> •M > > o o o 3 u U u a o o 01 A! ^ «: o o o o z Q o o 10 CO o D. ■•- . o 00 o o o ro c +1 CNJ CD o O V CO o •a- o o c> +1 en •— I o o c o o co - O o ce a\ _J CQ a: D- o o o o CD O o o o o u- o o LT) E Q ' — 1 1/) H 1^ 3 Q) +J O ■f- ■ — 1 O CNJ CO CT\ f^ CTi C\J CD •— f 00 O^ f^ (NJ Od CO eg en O C\J yD csi CD CM .—1 a\ o CNJ »— < r^ c\j CO "3- «3- >* "a- CO m •a- 0-) CM CO ^ o o 00 O O ■a- O o CO o o o o ^£) CO o o f— t o o f— 1 o o o o CO CO O CM

o r^ ro o t-H E o o O i- o ^ o o n E Q CO o o Ll_ <_) O UT) E O c o u a; la T3 O 4-» ■o 0) ■l-> u O) s- o u ^ 0) in B i- 3 O •f- > — ' u ■o n] ■•-> 21 TABLE 5 Millstone Point, Conn. Long Island Sound Surface Water* (Radionuclides in disintegrations per minute per 100 kg water) Station #2 #3 #4 #5A{outflow inner plume) 134 Cs 3±3 2±2 3.6±2.5 0.5±0.6 #5A(particulates >lp, from outflow, inner plume) #5B(particulates >lu, from outflow, outer plume) 137 Cs 29.6±3.6 31.8±4.0 27.0+3.1 43.8±4.3 90, Sr 28.6±0.2 25.5±0.3 30.4±0.2 26.0±0.6 238, Pu 239,240 Pu 0.019±0.006 < 0.003 < 0.010 < 0.010 0.002+0.001 0.101+0.015 0.108±0.017 0.090±0.020 0.090±0.030 0.032±0.001 0.0008+0.0005 0.034±0.003 For station locations see Figure 1; samples collected 20 October 1979. 55 Fe 7.4±1 11+2 llil 29±2 26.7+0.2 12.7±0.2 22 TABLE 6 Millstone Point. Conn. Sediment Coresl Radiochemistry (Radionuclides in disintegrations per minute per kg dry sediment) A. Station 2, Core #3 Section 1 Wet/ 55^ 8 137^ 238- 239, 24C L 241, cm Dry 1.532 Fe 1588±41 Cs 273±2 Pu n.79±n.04 21.9±0. Pu 7 Am 0-1 1-2 2-3 3-4 1.40 1065±26 411±2 1.22+0.11 38.6+1, ,2 4-5 5-6 6-7 1.34 1088±59 336±2 0.92±0.09 32.4±0, .9 B. Station 3, Core #2 0-1 2.03 ^ 325±46 600±4^ 3.27±0.19 129±3 32.3±1.5^ 1-2 1.65 274±39 487±3 2.58±0.16 102±2 2-3 1.89 244+49 603+4 2.87±0.18 121±3 3-5 31.9±1.6^ 5-7 1.95 245±34 641±4 2.47±0.14 112±7 7-9 9-11 1.83 388±26 498±3 3.37±0.21 130±3 11-13 13-15 6 15-17 1.96 625±66 723±3 6.48±0.15 215±5 46.5±1.6° 17-19 19-21 1.93 ... 483±3 4.98±0.12 148±4 — 21-25 25-29 36.1+1.9 6 29-33 1.77 121+32 281±2 3.34±0.22 92±3 4 5 Inventories, mCi/km2 30.5 45.5 12.07 % estim. delivery 128% 38.6% 610% Notes : 1 = For locations see Figure 1; samples collected 20 October 1977. 2 = 70% >62u, 30% <62p from wet sieving. 3 = 34% >62vi, 66% <62u,from wet sieving. 4 = mean ratio 238pu:239pu = 0.028. 5 = mean ratio 24lAm:239Pu = 0.287. = No Curium detectable. 7 = 134cs less than 1/60 of 134 + 137cs. 8 = 55Fe data decay corrected to 1 January 1975. 23 oj o en o o o +1 +1 CD +1 cr» ^ o o o o o U3 ro 00 in ro vo I— 1 n O .— t CM C 1 t-H CM --H o .-« o o o OO o o oo o o o o oo ao o o oo o o + +1 +1 +1 -fi +1 +1 +1 +1 +1 +1 -a-o CSJ C\i 1 — U3 n CM r-t V ^ r^ >rt ro .-H CO o o o oo O o OO o o C300 C300 OO (O 2 en •I- -^ CO 1 0) a. o CM CO ^ in lo IT) CM 0.-4 I— t r— 1 CM •— • CM O oo o o o o O O +1 +1 +1 +1 + 1 + 1 + 1 + 1 cDr-~ LD rj- en en O i^ LT) ro CTi n Q- 3 fc C m •f— i/l fc , s_ m ni 4-' n r-. c a) VI LlJ 1- c _J c: o OJ o • f— •a. S- •t-> +J •!-> C •r- to o ■•- a. -a a> c c •>- o 4-> on i— -o c o CM •— t O O O 1 o CM O I 00 o o o ■— o I +1 +1 +1 -a +1 C oo XI CM O »— t LT) O O CM O O 00 «3- + 1 O CD + 1 ro O ro O o o CD CM tsi •-•o O O o • • o CJ O O +1 + 1 +1 +1 o r^ crtcM CM CM Ort CM^rrO CMCMCM CMCM OOO OOO OO OOO OOO oo ^CT^CM cncoro locm CMCOOO I— *f— *f-H I— ICM oo oo OOO OOO oo o in o o • o o ro ncM ^ •-< ID in ^ o oo O'-^ o o o o oo oo o oro ^ > • < • . • o o o oo oo (.i C5 oo o +1 +t +1 +1 +i +1 + 1 +1 • ID 00 CM .-■CO in 00 OOO C_5 O oo •—•CM ,—i C 1 o V V o oo oo o o o oo OOO o o Id 00 ■!-> o CM r^ ■M •♦-> 0) S- i. i- 3 nj fO IT5 in Q. Q. D. l/> . — ■*-> ■" ■*-> ' — ■M , 1— OlM- 0 l/l in in in +j 4-J ■!-> •!-> +-> ■*-> ■♦-> ■4-> -4-J -4-' -4-> -4-1 I. 1- S- 1_ s_ s- i- i- i- s- s- s- na fO (tj «T3 ro (O to fO fO <^ (tJ ro a. U- CL Q. CL CL a. o. CL Ql CL CL 4-> -M ■M ■»-> -M -W ■4-J -4-J -»-> -4-» +J +-> i*- M- ><- 14- <*- 14- 14- 14- 14- l»- 14- <4- o O O O o o O o O O o o l/l l/l OOOO OOOO l/l l/l oooo oo oo CI Ol t/ll cr i. O s- i- =3 ai QJ OJ •o El ♦J ■4-> q; Ol m in OI >, >> . 1 O O s: S-l in in in in in in in in in in in in '3 3 '^ -3 '3 3 3 3 "3 3 -3 -) "O X) -D -0 -o-o -n XJ -0 -o "n T> Ol OJ (U OJ 01 Ol OJ OJ Ol 2:2: sis: ^s: 2: sis:^: o ^ 1^ r-. en > o , 'Ol •=c , ,_, ,_, CI t— 1 . . -»-> 4-> •1— 1 ■*-> . — > c q: a: C c C El t_ _J cz fD rt3i "D CO CL Q_ ■*-> c CL CI 01 a_ •M3 COO -3 c UJ 00 a. OJ Of , •>- »— 4 •»— ^J 4-> ro ■»-> OJ =31 C to E l- c l/> (/) "1 -^ U1 i~ 01 i/) ■0 HI ^ c <-Y t — in b u c • 14- -0 -,- OJ .—4 ■4-> C u ••- S- 3 0) OJ CJl-O *^ (U \J- ^-o • o o o o CD • . o . . +1 o o <■> o +1 o o o o 0> +1 +1 +1 +1 <* +i +1 -H +1 \X> r^KO en n LD \0 ** «x> r^ O O O o o o o o OO r-. +1 + O ^ kO .— ^ o +1 in •"] r^*a- vo U-> CM .-t PO CM ■— t LO •-* Kt o .-H o •r ro 1 — 1 ID ro m CM-— < o o o o o o O O O OO d d d d d ■4->d d d o do +1 +1 +1 +1 -f wi +1 + + 1 +1 +1 +1 ID CO <£> n oi OlO OO r^ »— « LDCM m «a- O .-1 o .— o C\J O rt OO o o .— o n cMn o o o o o n n n o o o OO OO o o o o o +1 +1 +1 ^ —« CM CO ro CM o CM o +1 05 n o o o +1 +1 +1 a^ ^H r^ oj n OO o o ■H +1 OO OO O O CD o o o o o o o o o o o o CSJ o o o o o m o o • o o - +1 o >a V o o .006±0 .004±0 .005±0 o +1 t— « o o +1 OO n o .010±0 .005±0 ND o o o o CO LO CM ^ o +1 Loro . LO ■ • • O O o o" .— 1.— 1 o' o ^n OO +1 O +1 +1 +1 +1 +1 +1 +1 +1 +\ +1 •— 1 +1 CM r^ LD CO ro •— « cn C 5 r^ ro*3- . CM •— < ro.-< CM *3- CM iTiw—t*^ CM LO ro CM -a- 'iS- ro ^3- cncorn -e- CO CM O o o +1 +1 +1 a^ \£} r^ o +1 CM O ft o o o +1 +1 +t LO «* 00 O O +1 +) CM CM ro CM ^ CM CM eg ro CT» o —I s- CD -.- «I > ^O LD o> CT> CT> Ci CT>CL 3 0; = ^ J^ I^ ,_, o^ CT> (O Qj O ^ o z LO r-^ 00 vo r^ r-^ r- r*«. r*. r^ o^ o^ LD r^ 00 LD r-. 1^ p^ rs. r^ p-^ O^ CT> O^ 0^ O^ O o -T3 I— (U o a*4-> ■ u c: fD I CM >> 4- -o -»-> o QJ O > = z. z QJ 3 * 0) •M in C o E < CM ro ^ O <3- -Q z: E >^ E OJ a> LO <— LO fO •— < na • 35 TABLE 12 Wiscasset, Me., Area :Environmental Samples - Biota II SANDWORMS ( Nereis versicolor ) (Radionuclides in disintegrations per minute per kg wet weight) Collection ^ Sites Sample Whole Worms Date 1-9 Aug. 1977 50.3+0.4 "8p,/239p^ 0.036±0.004 239.240p^ Wiscasset 4.71+0.145 (Area 1) Cleaned " 2 " 12.2±0.3 0.023±0.010 0.36±0.025 Sediment 3 4 M 1524±10 (508) 0.041±0.005 62.5±1.6 (20.8) Portland Whole Worms 11 18.1+0.3 0.036 ±0.007 1.69±0.08 Cleaned " " 7.6±0.3 0.045±0.021 0.325±0.029 Sediment '^ 4 II 111±3 (37) 0.028±0.013 9.57±0.82 (3.2) Notes: 1 Wiscasset worms from mud-flat just N. of diffuser; Portland worms from area expected to represent only fallout i.oni.ami- nation. 2 Cleaned by being allowed to evacuate gut contents. 3 Sediment data as dpm per kg dry sediment. 4 Sedinent data calculated as dpm per kg wet sediment, assuming wet/dry ratio =" 3. Ratios: Wiscasset Tissue concentration as % of v-.'hole-worr.: concentration 24% 7.7:: Portland Extractions: II II II Fraction of each nuclide soluble after 44 days in b^: Formaldehyde sea vater 42% 19.3% Wiscasset Whole 3% 1% Cleaned 63% 18% Portland Whole 4% 8% Cleaned 116% 12% 36 Faili we di from set vant of re 90Sr (Bowe progr at a bars eel 1 e (doc samp! anoma the n Cape conce ments expl bay m be de that ng CO d obt the r ut in sedim actor was a n et ess a poor prote nt se kwi se e, li- lies u c 1 i d Cod B ntrat { L i V re th ight posi t thi s operati a i n ( V i eactor Table ent ana output s we wo al, 197 t the t pi ace . c t i n g P diment ) from ke the ei ther es meas ay fall ions, a ingston e hypot concent ed cent happens on f r a a 1 outfl 13, t lyses of 1 uld e 4). ime Insp lymou trap the P other in th ured . s wel nd ra and h e s i s rate rally m the P i 1 c a 1 f i s h e ow. The d ogether wi , The wat 37cs or of xpect of a Evidently f sampl ing e c t i n of th Harbor for any ma i 1 g r i m 1 o s in the P e concentr The core 1 within t tios, repo Bowen, 197 that the fine sedim Evident grim rman ) ata f th a er sa Pu; coas ei the , or F i g u r and D teria utfal lymou a t i n from he ra rted 9); t gyral ents ly we 1 re one rom smal mpl e its tal r no the e 3 uxbu 1 s c 1. th a s or nea nge for his ci r from hav actor water this an 1 numbe showed ratio 1 seawate rel eas sampl e will s h ry Bay a r r i e d Our Dux rea, sh in the r the c of radi near-sh core wa c u 1 a t i the pe e no ev perat sampl a 1 y s i r of r sam es we was t ow th form north bury ows n rati enter onucl ore s s tak n of r i p h e i d e n c ors , e s are rel e- v i d e n c e to pi e re in aken at the an ex- ward Bay OS of of ide edi - en to the ry to e In a way, it is odd that we have not found a site with re- actor contaminated sediments since we seem to have found evidence for such contamination of biota in several places. The relevant data concerning samples from the area about Plymouth are set out in Tables 14A and 14B; comparison data from mussels, collected either in Boston Harbor or the Cape Cod Canal, are set out in Table 15. 37 It is worthwhile to start by pointing out that macroalgae, like Fucus , Ascoph.yl 1 um , or the mixed Red Algae analyzed, are wel 1 estab I i shed as showing seasonal variability in their concentrations of many trace elements; we would not, then, expect to be able to compare directly collections taken at different times. Much the same is proving to be true of mussels (Bowen et al , to be published). Examples of this phenomenon in the case of macroalgae are comparing the samples from station 1 (Table 14A) late October 1976 with those collected early May to be seen col 1 ected 1977: Fall Chondrus Fui 1T?( icus 7n gae 25.2 137^5. 1.07 239,240p^ 13.4 " ; 1.9 47.9 " ; 2 Spring Chondrus Fucus Red Algae 38.1 II ; 0.67 12.7 II ; 1.33 21.9 It ; 0.66 It appears that the seasonal change has led to increased 137cs in Chondrus , decreased in the Red Algae, and no change in Fucus , while each spring sample shows lower Pu If we at ab diffe fall- compa curre col 1 e and b Ascop 137CS si te s p r i n at s i Al gae site that betwe of th we me The P L i V i n stanc been compa out th rences col 1 ec red to nt fro cted F e h i n d hyl 1 um than 1 are g were te 2, (a CO 2 both the ge en the ese sa asured u data gston e , exc charac re g e sa tha ted sit m th ucus the , an are al so ri c and 11 ec in nera two mpl e tha can and eeds teri iven spe me time, t charac Fucus or e 2 , w h i e P i 1 g r i from si bar in P d Red Al those fr richer her by a s i g n i f i c t i n of fall and in this sites, s c n t a i t were s be comp Bowen (1 the ran Stic of CI es how teri Asc col ever ze t ophy 1 ected , then he site 1 1 um f r ch w m 1 te 1 1 ymo gae cm s in P 1 mos antl mixe i n mix It ned uffi ared 976) ge t fall e no reac com uth are ite u . t a y ri d ge spri ture shou cone cien wi t ; no hat out w belie tor out pared t Harbor, s i g n i f i 2, and At site factor Cher in nera ) w n g ; it are no 1 d be p entrat i tl y el e h those ne of t those d c n t a m i at we s . om ve fall si Si cant the 3 F of 3 Pu ere is, t tr oint ons vate sum he s ata nati i f f er xpect Examp ite 1 s mos . or te 3, te 1 ly ri first ucus in 1 also. riche howev uly c ed ou of an d to m a r i z ampl e p r e d i on in e n t sit to see 1 es are ( F i g u r tly up- spring- downst Fucus , c h e r i n two fr col 1 ect 37Cs th The R r in P u er, pos omparab t that y nucl i cause a ed by s , for ct to h the 19 es e 3) ream 1 n om ed an ed at s i b 1 e le none de 1 arm. i n- ave 70- 38 1971 period. The concentration factors in algae that are indicated, using as basis the data of the water sample in Table 13, range for 137cs from 20 to 150, and for Pu from 1000 to 2000, These are very like the ranges, for Pu, re- ported by Livingston and Bowen (1976). My til US cerm shown to 13 Table expec al one unusu have samp] site the " high edul whic ng earl i e 7Cs and s 14A a ted in . At s ally r i been re e from 3 , and normal " in some is, the F~we hav r, most to Pu m nd 14B a this gen tat ion 1 c h in 13 ported e site 1 , three of range . r a d i n u common blue muss e most informati other data for c ost of the musse re not clearly o eral area (see T , the sample fro 7Cs, but elevati 1 sewhere (see Tabl that from site 2 the four from s Those mussels t cl ides are as f o el, is the on, and as omparison. 1 samples s utside of t able 15) fr m 29 Octobe ons as grea es 7,11). , one or th ite 7, all hat appear 1 lows : animal con- we have In respect hown in he ranges om fallout r 197 6 is t as this The other e two from are within abnormal ly Site 1: 10/ Site 1: 5/ 29/76 28/78 13 55 Site 2: None Site 3: 6/15/71 Site 5: 10/27/76 Site 7: 9/23/76 ^Cs Fe (ratio to el sewhere ) Pu is 390, vs 30 to 50 137 Pu Pu Cs, Pu (but these may be in fallout range for that year; see Livingston and Bowen, 1976, Table 3) We have high P u , are rela These ar site 7 h seen in 24lAm to Pu-Am mi tainly 1 ium fuel contrai n 239,240P remai ns of its p no qu one ted t e fac igh P a mus 239, xture ess t Su di cat u. U to be r i r i e s t i n from si the tor of u was a sel (or 240pu 1 must h han 3 y ch an ed ) by nfortun measur ty posi that t te 5 a utput 2-3 (P ccompa other ess th ave be ears a r i g i n the re ately ed , ha t i n . he si nd on from u ) or nied envi an 5% en pr nd f r is al 1 a t i v the 2 ving te 1 e fro the P 10 ( by th ronme real oduce om th so CO ely 1 4lAm someh 55 high Fe and the two m site 7 are real and ilgrim 1 reactor. 55Fe) effects, and the e lowest 24lAm we have ntal sample); a ratio ly establishes that the d very recently, cer- e irradiation of uran- nfirmed (or at least not ow ratio 238pu to sample from site 5 still ow gotten jostled out The other animals reported in Tablesl4A or B fall into two 39 cl asses : grazers Stronqyl ocentrotus largely eating gra Bucci num , and the gram we had some d analyzed mussels, by some mechanism than do the grazer poses in undertaki this question and area of sporadic h uranic nuclide was might systematical concern. Comparis and with analyses leads us to the fo 1. Stronqyl oc entro like Myti 1 us : Thes d S p i s , Bal anu z e r s : T Eider D u ata, fro s u g g e s t i exhibit s on w h i ng the p especi a I i g h e r c o t e s , t i s 1 y rise on among reported 1 1 owing tus and s , an Fese ck. m ana ng th h i g h e ch th resen ly to n t a m i sue c to le the by L concl Litto are H£ At the lysis at i nv r acti ey fee t proj estab nation oncent vel s h data p i V i n g s u s i n s r i n a f e are Li ttorina , ula ; or marus , pred Lunat start of star ertebra n i d e c c d. One ect was 1 i s h w h of gra rations i g h e n i n t s r ton and 2, 3, from site 3, pr radi onucl ides . Spi sul a from si concentr a t i o n e Neither lobster t rat ions of 137 than, or even a B u c c i n u m and L, observations on times higher th from comparison 2, or reported concentrations an area that so stream. rom sit obably show no evidence of ators , ia . of this pro- f i s h eating te predators ncentrations of our pur- to explore ether in an zers with trans- in predators ugh to cause eported here, Bowen (1976), e 2 , and Bal anus Pilgrim 1 waste te 8 exh xpected nor e i d Cs or Pu s high a u n a t i a p s t a r f i s an in t h of site by L i V i n escal ate metimes ibits probably about double the Pu from fallout alone. er-duck show evidence of concen- in their tissues that are higher s, those inferred for their prey. robably agree with our earlier h in showing tissue Pu two to three eir prey, but there is no evidence 3 data with that either from site gston and Bowen (1976), that these systematically in organisms from receives the reactor coolant 40 70° 40' W 70°30'W BLACKMAN PT FIGURE 3 SAMPLING LOCATIONS AROUND THE PILGRIM NUCLEAR REACTOR PLYMOUTH, MASS. 42°00 N 4r55 N NAUTICAL MILES 2 -I 41 TABLE 13 Plymouth, Mass., Area: Water and Sediment Radiochemistry (Radionuclides in disintegrations per minute per 100 kg water, or per kg dry sediment) Part A - Water Analyses: Collection Date 90 137 238n 239,240n,, 238^ ,239p,, Site:* 1976 Depth - cm Sr Cs Pu Pu Pu/ Pu 1+ Oct. surface 36.2+0.6 32.0±0.5 N.M. 0.15±0.06 Part B - Sediment Analyses : 1 " Oct. 20 0-3 Grab 66.1±1.5 0.29±0.04 8.2±0.3 0.035 2 Oct. 19 0-4 Core 157±3 2.6 ±0.2 61.5±1.7 0.042 4 Oct. 19 0-6 from Anchor 59.7+1.3 0.68±0.07 21.3+0.6 0.032 Cape Cod Bay Aug. 0-1 Core 187±6 2.5+0.3 101±3 0.034 0.037 0.038 0.043 0.036 0.034 0.032 0-3 Grab 0-4 Core 0-6 from Anchor 0-1 Core 1-2 Core 3-4 Core 5-6 Core 8-10 Core 12-14 Core 16-18 Core 187±6 2.5 +0.3 101±3 181+3 2.8 ±0.2 75±2 176±2 2.6 ±0.2 69±2 181±3 2.7 ±0.3 62±3 174±3 2.5 ±0.3 69±3 198±3 2.4 ±0.2 69±2 107±3 1 ±0.1 33±1 Notes: * = For locations, see Figure 3. + = Water directly from Pilgrim I outfall, X = Sediment from plant intake basin. 42 o ■-• o en n O >a- VO "3- O c> o O o o o <-> O +1 +1 o +1 +1 o +1 en vo e^ liJ o\ ro VO O CM CM ro v£> o <-i in tn O o •— t .— t .— I o o o o o o lO ro o m o •— I t— I o to r^ c\j \0 CO \£t in po f-t o o o +1 +1 +1 vD in (c o —• — I o --« o O O .-H foo o«— «o ooo x: CM o ^ 'a- lO C\J m in in vt m in o CVJ CM •— « f— < o O f— » f-H O o o o o o .— * o o OsJ o o C\J o o <-) o CM r^ O o o o o o o o o o o o o o CD CO o +1 o o tJ +1 +1 +1 +1 o +1 +1 +1 n +1 n n in »^ r^ r^ +1 in ^ +1 ro XT +1 o ro in m C\J ^ ^ C\J t—i •— t in ^ o o o en tn on in f-H o o o o o o o o o o o o o «— t o o o V o V V 0) QJ o o o o o o o o o o o o o o o o o o CL CO CM CM PO CM ^ ro ^ in o CM ro ^ CM 4-> tJ O O d d d d d V) +1 +) +1 +1 C5 +1 +1 +1 o l—t d +1 o <-) O CNJ ^ in 0^ +1 t— t r^ o^ +1 +1 +1 ro +1 CT^ +1 CT> in ro ^ r^ on CM «— < o (\j «— ' ^ a\ ro rH CM to r^ •— 1 CM in c +j Jj tj 1- m C7> 0) » c b- b 3 3 o c: 3 1. U 1 ^- o> 3 i^ m a> a> ^ V) <1> fD 0) la c rtj =3 > o> (/> t/> ro >> > >> cn •^ V) cn U 3 3 m -C XI c i- u o -o ■M TJ -o r -» (U o >-l 3 <4-> 3 i/l QJ >1 > a> >» CT> cn +j >» 4-> £ = - 3 = 5 3 < 3 u o - - - ~ s: O " " CM CM CM CM CM CM CM CM CM CM CM 43 o en O O £3 o o ^3- O OD O CD ■-> Z O O in n o o o «a- "O CSJ m «:r M- in CO CTi o o o o o o CO o O .—1 o o o o o > o o o +1 +1 +1 +1 +1 o +i +1 +1 o-i 1^ LD Ol LT) +1 r^ p^ CM 3 -C i/i Ol ro l- ■»-> l(- O cn CO ^ 1 s_ OJ in U- 0) f~- 0) a. ■!-> a^ CM »—* I— t r-( o O o C5 O 3 ■ O- O o CJ o 00 +1 + 1 +1 +1 +1 CO CO CO CO in CM CSJ CM o o o o in 00 r^ «3- (M O .—1 o C7 o O CM O o o o o O o d d C3 +1 o +1 +1 +1 + 1 in +1 CM CO 00 lO (Nl CM CO f— 1 o o o O t— t o o o , — (_> ID 1- r~ *-> OJ CO C a. f— t CO Ol •=a- l- irt c: c o o LiJ s- •r- _l .,— ■M m > lO ■a c 1- t— LU Ol CM U. Oi c ID i- ■1 — m et in o CM O +1 PO + 1 in +1 O f— t in CJl +1 +1 * "3- CO CO ID (M CM . CO CO ^ . O ... O +1 o o o +1 in +1 +1 +1 o . t— I in in . CM • . • CM i-H CO CM »— < • +1 in o o o V d +1 CM CO CD 2: OJ 3 o T3 0£ Ol o i/i 3 t/> O in 3 1 — O 3 ■o in 0) OJ > in 3 ,— •f— in O tA Ul en m I/) tn l/l •r— c >, — • 1 — c >,— ■r— •(— O , — (O , — f— o f— , — f— s- 3 3 3 . — 3 3 3 Ol c •>- c •!-> O cu +J 1— o I— cu o.— Or— o <*- u o M- C O o ■I- OJ ■!-> +-> fO fCJ UTD O .— O 1- o-o <*- 0) ■!-> CO u a> 01 s- !- S- 3 O Ol O 01 -O c (U a. Ol <: O) OJ o c o X IT3 O) C "O Ol u 03 _J r^ r-^ r- = in in CX3 c 3 0) c 3 Ol 3 = E — 1 4-> ■l-> CL l>0 . 1 — P-- CO CO CM CO CM 00 ,—i in CM in a. Ol tn c 3 - cn 3 *-> Q. 0) l/l a. 3 n3 O) o OJ CU o o i/i in +J Ol c in 3 >, O f— U lO c QJ in (D OJ U ■!-• •I- HJ .— o Q.->- 3 .— ■O Q. 3 I <4- T3 1 O in 03 OJ OJ I I I ,-ICM CO 0) o o « QJ +J I — -^ >— oo o <_) CO C^ CO CO CO in c ^ S c O lO i- OQ 00 /"A TABLE 15 Biota Samples for Comparison^ to Plymouth Area (Tables 14A + 14B) (Radionuclides in Disintegrations per Minute per Kg Wet Weight) Collection Site 3 Boston, MA i Cape Cod Canal Date Organism 137 Cs 238 Pu 239,240 Pu 241 Am 9-22-76 Mytilus edulis 1.8±0.3 0.002 0.11±0.02 0.008±0.004 8-18-77 " " 2.1±0.2 0.004±0.002 0.16±0.01 0.02 ±0.01 9-25-76 " " 1.9±0.3 0.012+0.006 0.13±0.02 0.020±0.008 8-19-77 " " 3.9±0.2 0.021±0.005 0.26±0.02 0.05 ±0.01 Notes: 1 = See also fallout-contaminated mussel data on Tables 7 and 11. 2 = Soft parts only 3 = About 32.5 miles NW of Pilgrim 1 reactor site 4 = North end of canal; about 17.5 miles south of Pilgrim 1 reactor site. 45 SUMMARY AND CONCLUSIONS It is of ou An appre data , quest u 1 1 i m expl i surve year, here pi ann years samp] pure prof 1 analy a b i 1 i a1 , 1 that matte reaso r stro f our ci abl e or th ions ate! y citly y work This is jus ed to ; that e and/ good f ted en ses of ty of 978) s both N rs of nabl e n g d i s early time e r i g h f i n t e to con (page . . . det i s a t the provid any c or ana ortune ormous biota data f upport RC and this s to pref sati sfa di scuss would b t sampl rest to cern NR 7 ) : " T ailed s 1 ong-te bare bo e a ske n c 1 u s i lyze ne . We s 1 y in r col 1 ec rom the ed by E EPA wo ort . ace th ction ions w e need i ng CO us , C. Ou he fir t u d i e s rm pro nes of 1 eton ons ot xt can houl d espect ted un Musse PA. I ul d be 1 s sum at the ith NR ed to verage r thos r i n i t St yea will gram" . pre! i for th her th be dr emphas to th der th 1 -Watc t appe n e f i t mary out C em pro V , to e we ial r wi begi Wh mi na e pr an d awn i ze e i n is p h pr ars from with t come of p h a s i z e i d e e i t answer b e 1 i e V proposa 11 be d n only at we h ry work g r a m i eci sion from th also th terpret rogram , ogram ( from wh some 1 he sta the p d that her en ei the ed cer 1 Stat evoted in the ave to , that n subs s what ese da at NRC a t i n by th Goldbe ere we i ason tement reject. an ough r the ta 1 n ed to second report was equent to ta is has of the e avail- rg et si t i n We are to the year, The mi compl e sional or of redef i change of thi betwee that w have b wi thou there our un NRC to in con f ami 1 d e c i s and do stake te avo d i s c u the Di ned wo s , and s comp n the e comp een sh t b e i n can be happy c n s i tract i a r wit ion to not wi that we i d a n c e s s i n vision ul d hav at 1 ea 1 ete ab agency lete th ortchan g at fa no tho s i t u a t i der it, admi ni s h the stop sh to beli of an f the of Re e per St to sence and t is re ged, ul t, ught on; i for trati type support appear eve we y commu ways i actor S m i 1 1 e d argue of any he rese port wi and fur to shor of corr t woul d the Age on . f cha of t to be see n i c a t n whi afety us to again i nte arche th a therm tchan e c t i n be p ncy t nge of his pr compl n NRC ion w i ch the Resea adapt st oth r a c t i v rs i t strong ore th ge NRC g. or s s i b 1 chan pol ojec a i n i s pa th u int rch , to ers . e CO supp fee at w . of a e, a ge i i cy that 1 ed t after one ng about that, rt was the s. An occa- erests of NRC, were being some of these The result mmuni cati on orted has been ling that we e were led, b V i u s 1 y , mel iorati ng , nd we urge ts practices 46 Summary The d 1 i ved at V:i c n f i provi b i g e to be p e r i to ha to be or ev Mai ne Analy of bi both to be least the s tempi we na likel be! ie proje that have chemi e V i d e react a n t i - win gest ing p ata CO radio 1 1 ston rm tha de the ochemi true d , in ve red usef u en mea Yanke llect n u c 1 i e Poi t eno base stry, of Pu 1977- uced 1 , an surab e or ed so des i nt , a ugh 5 s for at 1 and 78, the 1 d we le -- P i 1 g r far concerning the amounts of long- n wastes released from the two react nd from the Maine Yankee reactor, 5Fe, 60co, 134,137cs are released to very useful tracer studies of their east sporadically this appears also ses of s Ota arou that eno useful , sporadi ort of 1 ated at ve not y y that m ve , furt ct so fa can be u high pro cal stud nt that or site nucl ear be a s u i al so tha ubl i c ac ediments nd both M ugh trace and that c c n t a m i c a 1 b i g the start et found uch more hermore , r has pro sed for i babil i ty ies of th from the acceptabi forces, t table loc t it will ceptance . in the a i n e Y a r is a V we hav nati on e ochemi of thi the s u i work wo that th V i d e d u denti fy of be in eir was point 1 i ty cr he same us for have g area aro nkee and a i 1 a b 1 e e found to provi cal expe s projec table fo ul d be n e e X p e r i s with a ing othe g suitab te produ f view i teria , factors b i g e c h reater d und Ma P i 1 g r in the enough de the riment t. At ci , an eeded ence g gener r reac le 1 oc cts . f defe especi that em i cal i ff icu i n e Yanke im 1 have se enviro foci of f ramewor s that we M i 1 1 s 1 n d it is q to do thi athered i a 1 i z a b 1 e tor sites i for bio It i s , f nding NRC ally agai suggest a studies, 1 ty in ac e , and shown nments at k for re con- e Point ui te s. We n this basis that geo- course , 's nst site sug- h i e V - A set of more-or-less specific conclusions follows: Concl us ions Nuclides Studied 55Fe is clearly a major waste product of each of the reactors studied, approximating the levels of 60Co rel eased . 47 134CS is rele 137CS, so tha be used as a radi ocesi um. 238Pu is rele ranging from in d i s t i n g u i s Cm is now bei TTTllstone Poi either Maine Release Pattern The rates of die tors of th products 1 i ke Am or Cm. Fu those easily nuclides that pulses of hig nuclide trace Environmental S Mi 11 stone Poi iJbFe in the e particles, wh associated . these tracers have so far f Without a lar son, however, elusion, thou Point area co The only biot show reactor discharge can done, so far Mill stone Poi envi ronment , Maine Yankee ased, generally, at nearly uniform ratio to t the change in this ratio with time can guide to dating movements of released ased at 1 to as hing rea ng relea nt, and Yankee o s rel ease e rates 55Fe or rther st measured could b h concen rs . amp! es nt sampl TTluent i 1 e only This sho in 1 c a ailed to ge body it woul g h an in res show a sample c n t a m i n al. Alt no e V i d e n t radio very high ratios to 23 high as 5. This shoul ctor Pu from fallout P sed in only very smal 1 has not yet been detec r Pilgrim 1 . of radiocesium are not of rel ease ei ther of a 60co, or of transuran udy will be needed to (by gamma spectrometr e used to identify the trations of long-lived ing h is as one uld h 1 sed find of se d hav corre ed re s fro ation hough nee h acti V as sho soci at third ave 1 e iment , and d iment e been ct one actor- m this are t much as app i ty im wn the e d wit of the d to d accumu sampl e core an un , that origin area hose t more w eared p i n g e s foil h eas Pu i e p s i 1 atio , sue data avoid both ated that aken ork s showi on i 9,240pu, d be useful u . amount from ted from useful pre- c t i V a t i n ics like Pu, identi fy y) waste occasional radio- owing : All ily filtrable s similarly t i n of ns, but we h pi aces . for compari- able con- Millstone contamination, clearly from the houl d be ng how ts local fl ushed , sampl es contami n the reac of these ing and others e si te from ation tor s cert redes ertai occupies a much more restricted, less well We have not yet analyzed any water the area that show evidence of reactor , but sediment samples from all sides of ite prove measurably contaminated. Some ainly reflect the conditions before mov- iqn of the waste-stream outflow, but nly post-date this change. Both algae 48 and she! 1 f i sh fro evidence of react present diffuser activities; compa Portland, contami the reactor waste chemical-physiolo from fallout. Pilgrim 1 occupie enough to our lab tensively in its samples or sedime actor contaminati deal of evidence In each case thes the reactor along there are enough tion is sporadic case were the lev enough to cause c levels approximat contamination in evident that with reactor operators an elegant series would invaluably cal fates and rat nucl ides of react erated that would much more plausib for prediction of reactor accidents supplies. m several loci about the area show or wastes. Worms from near the have taken up both Cs and Pu radio- rison of these worms to those near nated only by fallout, suggests that s were measurably different, in gical behavior, from the same nuclides s a well fl oratory so neighborhoo nt samples on. We hav of reactor e have been the mainla data to sho and relativ els of radi oncern -- g ed those ch the 1970-71 just a lit , the Plymo of environ c 1 a r i f y our es of movem or origin. support mu 1 e , model s the effect on local m u s h e d si we have d. We h so far, e, howev contamin col lect nd shore w that, ely qui c n u c 1 i d e eneral ly aracteri period, tie coop uth area mental e ideas o ent of 1 Informa ch more than tho s of was arine en te, that sampled q ave found that exhi er, found ation of ed from n . And in local ly , kly lost, s measure , when CO Stic of f It is, eration f could be xperiment f the bio ong-1 i ved tion woul detailed, se now av te spills vi ronment IS near u i t e e X - no water bit re- a good biota, orth of each case contami na- In no d high nf irmed , al 1 out however , rom the used for s that geochemi - radio- d be gen- and a i 1 a b 1 e or of s or food 49 Appendix Table Common Names and Taxonomic Details for Organisms listed in Tables 7, 11, 12, 14A-B, 15 Plants ^ Common Names A. Brown_A]^gae Fucus vesiculosus Rock Weed Ascophyllum nodosum " " Laminaria~Tongi cruris Kelp B. Red_A1^3ae Chondrus crispus Irish Moss Mixture: Ceramium rubrum Irhipflv '^°"^ Spermothamnion lurner)^ '''^^'-y " Phycodrus rubens )cnmo " Phyllophora brodiaei )^°^^ Animals A. AnneHda^ Worms Nereis virens Sandworm; Clamworm B- Mgllyscs 2 Shellfish Bivalves ^ Crassostrea virginiana Oyster Spisula soTidissima Surf Clam Mytilus edul is Blue Mussel G?!k2P9Ls ' Snails Lunatia heros Moon snail Buccinum undatum Waved Whelk Littorina littorea Common Periwinkle C. Crustacea^ Balanus balanoides Barnacle Homarus americanus Lobster D. Echinodermata 2 Stronqyl ocentrotu s drobachiensis Green Sea-urchin E. Birds ' Somateria mollissima Common Eider duck Notes : ' - Taxonomy from Kingsbury, 1969. ^ - Taxonomy from Smith, 1964. ^ - Taxonomy from Robbins, et al , 1966. 50 REFERENCES CITED Beasley, T. K. and S. Fowler, 1976a. Plutonium isotope ratios in polychaete worms. Nature 262:813-814. Beasley, T. M. and S. Fowler, 1976b. Plutonium and Ameri- cium: uptake from contaminated sediments. Marine Biology ^S: 95-100. Fowler, S., K. Heyrand, and T. M. Beasley, 1975. Experi- mental studies on plutonium kinetics in marine biota. In Impacts of Nuclear Releases into the Aquatic Environ- ment. (IAEA, Vienna) pp 157-177. Fukai, R., S. Ballestra, and C. N. Murraj/, 1973. Inter- calibration of methods for measuring fission products in seawater samples. In Radioactive Contamination of the Marine Environment~TlAEA , Vienna) pp 3-27. Goldberg, E. D., V. T. Bowen, J. W. J. H. Martin, P. L. Parker, R. W. son, E. Schneider, and E. Gamble, Watch, Environmental Conservation Farrington, G. Harvey, Risebrough, W. Robert- 1978. The Mussel 5, 101-125. Hetherington, J. A., 1976. The behaviour of plutonium nuclides in the Irish Sea. j_n Environmental Toxicity of Aquatic Radionuclides; Models and Mechanisms, M. W. Miller and J. N. Stannard, Eds. (Ann Arbor Sci., Ann Arbor) pp 81-106. Joseph, A. B., P. F. Gustafson, I. R. Russel , E. A. Schuert, H. L. Volchok, and A. Tamplin, 1971. Sources of radioactivity and their characteristics. In Radio- activity in the Marine Environment (US NAS-NRUT Wash- ington) pp 6-41. Kingsbury, I si ands , J. M., 1969. Seaweeds of Cape Cod and the Chatham Press, Mass., 212 p. 51 Krishnaswami , S., D. Lai, B. S. Amin, and A. Soutar, 1973. Geochronol ogical studies in Santa Barbara Basin: Fe^S as an unique tracer for particle settling, Limnol. Oceanogr. 18, 763-770. Labeyrie, L. D., H. D. Livingston, Measurement of SSpe from nuclear ments and seawater. Nucl . Instr and A. G. Gordon, 1975 fallout in marine sedi- Methods 128: 575-580. Livingston, H. D., and V. T. tween the marine and fresh of Plutonium and americium Admin., Health Safety Lab. HASL-315, pp 1-157-174. Bowen, 1976. Contrasts be- water biological interactions U S Energy Res . Devel . Environm. Quarterly, Rept. Livingston, H. C, and V. T. Bowen, 1979. Pu and 137Cs in coastal sediments. Earth and Planet. Sci. Lett. 43 : 29-45. Livingston, H. D., D. R. Mann, and V. T. Bowen, 1975. Analytical procedures for transuranic elements in sea- water and marine sediments. j_n_ Analytical Methods in Oceanography, Adv. in Chem. No. 147 (ACS, New York) pp 124-138. Nelson, D. M. and M. B. Lovett, 1978. Oxidation state of Plutonium in the Irish Sea. Nature 176: 599-601. Noshkin, V. E., V. T. Bowen, K. M. Wong, and J. C. Burke, 1971. Plutonium in North Atlantic Ocean organisms; ecological relationships. In Proc. Third Natl. Sympo- sium on Radioecol ogy , vol. T7 D. I. Nelson, Ed, U S Dept. Commerce NTIS, Springfield, Va.) pp 681-688. Noyce, J. R. J. M. R. Hutchinson, W. B. Mann, and P. A. Mullen, 1976. Development of a National Bureau of Standards environmental radioactivity standard: river sediment. Xn P<^oc. Intntl . Conf. Environmental Sensing and Assessment (Inst. Electrical Electronic Engineers, N. Y.) paper 19-5. 52 Robbins, Chandler, B. Brown, H. Zim, North America, Golden Press, N. Y. 1966. Birds of 340 p. Smith, R. I., Ed., 1964. Keys to Marine Invertebrates the Woods Hole Region, Spaulding Co., Boston, 108 p. of Volchok, H. L., and M. Feiner, 1979. Laboratory Intercompar i son Exercise. Energy, Rept. EML-366, 43 pp. Radioanalytical U S Dept. of Wong, K. M., V. E. Noshkin, and V. T. Bowen , 1970. Radio- chemical procedures for the analysis of strontium, anti- mony, rare earths, cesium and plutonium in sea-water samples. Xn Reference Methods for Marine Radioactivity Studies, Y. Nishiwaki and R. Fukai, Eds. (IAEA, Vienna) pp 119-127. 53 NRC FORM 335 (7 77) US. NUCLEAR REGULATORY COMMISSION BIBLIOGRAPHIC DATA SHEET 4 TITLE AMD SUBTITLE lAdd Volume No , li appropriate) The Environmental Behavior of Transuranic Nuclides Released from Water Cooled Nuclear Power Plants 1. REPORT NUMBER (Assigned by DDCI NUREG/CR-1658 2 (Leave blank) 3 RECIPIENT'S ACCESSION NO. 7 AUTHOR(S) 5. DATE REPORT COMPLETED Vaughan T. Bowen MONTH September 1980 9 PERFORMING ORGANIZATION NAME AND MAILING ADDRESS (Include Zip Code) Woods Hole Oceanographic Institution Redfield 3, Water Street Woods Hole, MA 02543 DATE REPORT ISSUED MONTH March 1981 6 (Leave blank) 8. (Leave blank) 12 SPONSORING ORGANIZATION NAME AND MAILING ADDRESS (Include Zip Code) Division of Safeguards, Fuel Cycle and Environmental Researcl)i Office of Nuclear Regulatory Research U. S. Nuclear Regulatory Commission Washington, DC 20555 10. PROJECT/TASK/WORK UNIT NO. 11 CONTRACT NO FIN B6153 13 TYPE OF REPORT Final PERIOD COVERED (Inclusive dates) 1 August 1977 - 31 December 1978 15 SUPPLEMENTARY NOTES 1 4 (Leave olankj 16. ABSTRACT (200 words or less) Release data are reported for three coastal water-cooled nuclear reactors: Millstone Point No. 1 and No. 2 (for the period January 1977 through April 1978), and Maine Yankee (for the period 20 June 1977 through 25 March 1978); release samples were analyzed for 55Fe, 60Co, 134Cs, 137Cs, 238Pu, 239,240Pu, 24lAm, 242Cm, and 244cm, but not all nuclides on every sample. Radioiron is a major component of the releases measured; the transuranium nuclides are less significant components than was expected, but levels have occasionally reached microcuries per month. Pulses of this size are adequate for tracer studies. Environmental samples (water, sediments, and biota) have been analyzed from about the two reactor sites noted, and that of the Pilgrim No. 1 reactor. No water samples remote from reactor outflows have unequivocally shown reactor contamination. No sediment samples from near Millstone Point or Pilgrim 1 have shown reactor contamination; this has been clearly evident in several sediment collections from near Maine Yankee. Biota so far measured from near Millstone Point show reactor contamination only when taken from the effluent canal. From the Maine Yankee and Plymouth areas, however, biota samples fre- quently prove to show slight, but definite, reactor contamination. In these two areas biogeochemical studies of the fates of long-lived waste radionuclides could easily be carried out, and would be very profitable. 17 KEY WORDS AND DOCUMENT ANALYSIS water-cooled reactors reactor effluents environmental radioactivity iron-55 cobalt-60 radiocesium Plutonium americium 17a DESCRIPTORS 17b. IDENTIFIERS/OPEN-ENDED TERMS 18 AVAILABILITY STATEMENT Unlimited 19 SECURITY CLASS IThis report) Unclassified 20 SECURITY CLASS ITh,s page) Unclassified 21 NO OF PAGES 22 PRICE S N RC FORM 335 17 77) UNITED STATES NUCLEAR REGULATORY COMMISSION WASHINGTON. O. C. 20555 OFFICIAL BUSINESS PENALTY FOR PRIVATE USE. $300 POSTAGC ANO FEES PAID U.S. NUCLEAR REGULATORY COMMISSION 2 C 33 m c X o o o f- m D Z c o l- m > 33 o Crt