n

l -

Radionuclrdes and Heavy Metalsin Environment

edited by

Marina V. FrontasyevaFrank Laboratory of Neutron Physics,Joint Institute for Nuclear Research,Dubna, Russia

Vladimir P. PerelyginFlerov Laboratory of Nuclear Reactions,Joint Inst i tute for Nuclear Research.Dubna. Russia

and

Peter VaterKernchemie FB 15.Ph il ipps-Un iversitdt,Marburg, Germany

Kluwer Academic Publishers

Dordrecht / Boston / London ,J CC 1

Published in cooperation with NATO Scientific Affairs Division,1- l

i : i i \ i - ! i - i ,u.r ; i i r

e

) I

h,#

WW

'"sr AND "'cs AcrIvITy IN SURFACE soIL SAMpLES FROM soMEAREAS AFFECTED BY THE (MAYAK) PLUTONIUM PRODUCTIONASSOCLATION

M.V. FRONTASYEVA. L I SMIRNOVlirorrk Laborotor.t' of .\'eutron Ph.r,,sics, ./oinl In.slilule.fitr .\:ucleurIlcsearch, l.l 1980 Duhna. 1ia/,\Vl

S.A. ROMANOVIn.stituIt of Bioph.r,.;ic.t, ()zar.sk,1i a :\l\7-.I

V D CI.IERCHINTSEV,\lagnitogor:;k Slule '1'er:ltnic;al I init,er.sit.v, 155000 llognituryorsk, /ia,;\l\Z.l

E, STEINNESDeparlmenl of ('hcnrislry, .Nonresion ( tniyersit.y 6J Jc:icnc:a antl' l t: c: h n o I ogr.',,\ ' ( ) - 7 1 9 I ' l 'r o n t lh e i trt, i \ ' ( ) R II ' . I I

Abstract

This papcr conlains lhc rcsulls from mcasurcrnents ol 'e"Sr and rrics in s:unplcs ofsurlacc soil collccted in 1998 bc1 ond thc Eastcrn Ural Radioactivc Tracc (EURT) in 1hcnorlhcrn parl ol Chch'abinsk rcgion. Thc sarnpling sitcs u'crc thc sanrc as for lnosssaruplcs collcctcd to studl the deposition of hcarl ' nlclals in this part of Ural [ | Thcrcsulls obtained \\ 'erc conrbined rvith dala fronr a pro'ioush' published papcr bascd onsarnplcs col lectcd betu'een 1990:urd 1995 [2] * , i th in thc EURT, and GIS nups o[ thcpollution paltenrs of lhc abovc radionuclidcs ucre crcalcd on (he basis of thc conrbincddala.

l . Introduct ion

'l 'hc South Ural Moulrtains is atnong of t ltc rnosl scvcrcl) 'polluted rcgions in tlre uorld.*herc lhe huntan impact on thc cnvironnrent is practicall l irrcvcrsiblc. In sonrc areassuch us thc Chclr,abinsk rcgion the condition o[ thc cnvironurcnl has rcached (a slalc ofdccp ccological cr is is> [3] This is lhc rcsul t ofatnrosphcr ic cnr issions ofhcavv nrctalsfrom iuduslry and conlarnination of lhe arm bl' high lcvcls of r:rdioactive substancesfrorn l ltc <Nlavak> produclion association (PA) Thc <Mavak> production i lssocietionlocatcd nc\l to l lrc cit l 'of Ozersk. about 70 krn norlh of Chell 'abinsk is thc silc at lrhiclrRrrssi;t 's f irsl plutoniunt productiou rcaclor bcgan opemting in l9{9 Sincc thcn thcl\{arak sitc has also becn uscd for spcnl fucl proccssiug. \\aslc stoli lgc and uastcrrtri l lcalion. Substartt irrl cnrissions ol'radioactivc substauccs htrvc occurrcd in thc l jral

)9

, \1.V. f ' rontust t to ( t d l . ( tds.) . Rudionucl i t l t 's und I l tut t i l l t ' tu ls in I :nvintnntt 'nt . )9 16.(O l00l X/art ' r t \cudtnr i t I 'ubl i .shL'rs. I ' r in lu l in thc 'Nttht ' r lunds-

30

region as the result of firll-scale activities of the PA: the explosion of high-level wastetank storage in 1957; airborne debris from Lake Karachay in 1967; discharge to tlrcTecha river.

As the result of the explosion n 1957 a radioactive cloud appeared. It moved inthe north and north-western directions and involved radioactive contamination of theChelyabinsk, Sverdlovsk and Tumen regions (Figure l). Ilre area contaminated at alevel appreciably higher than the background was 23000 km'. The main components ofcontamination were short-lived radionuclides. However long-lived Sr, Cs, and Puisotopes were the most dangerous (Table l). Since l95l Lake Karachay has been themain reservoir for storage of liquid radioactive waste from Mayak. In 1967 windscarried about 600 Ci primarily associated with dust from the dried exposed shoreline ofLake Karachay up to 75 km from the site. Due to the highly uleven nature of the winds"hotspots" were formed having activities of up to 50 Ci/lsrn'. The contaminated areaconstituted 27001ffr'. Since 1949 the amount of contamination from Mayak has reached150 million Ci of radionuclides which covers an :uea about 26700 km' . The latter isreviewed in the report "Behind the Nuclear Cutain. Radioactive Waste Management inthe Former Soviet Union" of Battelle Memorial lnstitute, USA, 1997 [41.

Figure /. Fastern-Ural Radioaclive Trace(For orientation: 9enr6nrcx - Chelyabinsk, Exaraprcfypr - Ekatarinburg)

-1 I

l ' .Ul l - t i l . Radionucl idcs contr ihul ing to rhc long- l ived radioact iv i tv l5 l

Radionucl ide I lall--lil'e 'l rpc of-radiation

Contribution to thcactivitv ol' mixture. %oI

i

f.l

srfls

,d

isin

Sr-89Sr-90+Y-90

Zr-95+Nb-95I{u-106+Rh-106

Cs-l l7Ce- I4:l+Pr- I:14

I'tn- 1,17I iu-155

I)u (rnixtLre ol'isotopes)

5l d2ll 6 r,'65dl1

-10 v28,1 d2615v

0.vl i

0.v[], v0.r0.v0.v[J,r

trace

) .4

249

0 03666

tracctracetracc

In thc present rvork the impact of "Mavak" PA in areas adjaccnt to thoscdircctl l affected by the EURT *as studied. For this purpose. ! 'Sr and r37Cs actirit ieswerc mcasured in soil sarnples collccted in Chcly'abinsk rcgion in 1998.

Numerous invcstigators tluoughout the years (see. for example. [5-81) studiedspccific pcculiaritics of thc discharged radionuclidcs and their spatial and tcrnporaldistribution in that affected area. In the early l990s the Danish scientist A. Aukrog andhis colleag.res rvere the first western scientists who rvere able to participate inradionuclidc sludics in this uca bccausc lhc lwo contalnination events wcrc kept secretunlil lhc cold rvar cnded in thc latc l9tt0s In thcir papcr "Radioactive lnventorics frornthc K1sht1'nr and Karachay Accidcnts: Estimatcs Based on Soil Sarnplcs Collected inthc South Umls (1990-1995) I2 l the1,have est innted thc inr , 'entor ics of t " 'Sr. ' t 'Cs andrrerioPu from trr'o major conlanrirution evcnts in t-he Eastcnr Ural Rad.ioactir,'c Tracc.Thus rrc lud a possibil i t l ' to cornbinc our rcsults obtained in 1998 for thc arcas bcvondEURT u'ith thosc publishcd b1' Aarkrog ct al.

2. Mcthods

2.I . SAMPLING

The soil sarnples rvcrc collected in l99tt in the northem part of Chelvabinsk region(Figurc 2). Surfacc soil was sampledby means of a stecl corer. u'ith l0 crr diameterAfter removal of thc litler, the uppcrnlost 3 cnr of the soil prohle rvas sampled Eightsub-sanrples frorn each site. taken rvithin an area of about l0 x l0 nr, rvcrc joined loform a composite sarnplc. The rveight of the composile sarnplc may vary considerably.dcpending on the rntio of organic rnattcr/rnincral nlattcr. The total amount of samplervas about 2 5 L After sampling. the soil rvas dried and sieved bcforc analysis.

'&.tirniilil

tiiii}!.!.;,{$iii$til

I

.iiii'll. l

;i;j.it,i

;i',,.,tg,.1

ffiiitffi

Figure 2. SamPling sites

Sites marked as open circles are from the authors' sampling in 1998;

black circles denote sites from Aarkrog et al [2], sampling during 1990-

The total dry weight of the sample was recorded and speciflc weight of each

sample was determined in order to be able to express the amounts of contaminants on an

area basis. This part of work was perforrned in Dubna.

2.2. ANALYSIS

The radioactivity measurements were performed in the Institute of Biophysics in

Ozersk. The determination of eoSr in soil samples was based on measurement of the "T

daughter isotope after radiochemical sepantion, using the low-background installation

UMF-1500.The activity of r3?Cs in soil samples was measured by scintillation y-

spectrometry.

: : : : t :

'|',- ra' atr

3. Results

Thc results frour dctcnnir.ration of t"'Sr and lstCs in thc

Tablc 2. Data on ! ' 'Sr plottcd vcrstts 't-Cs arc shon'n

corrcsponding data lrom Aarkrog ct al. l2l iuc includcd'

'1 . \ l l l . l , 2. ' ' Sr:ur, i l i "C, i r t surfacc soi l samplts l iorn the Sotr lh I r ra ls

- lJ

prcscnl slmplcs rtre givcn ittin Figurc 3. u'hcrc also the

td!r"

cach0n all

lcs ln

hc q'Y

l lat ion

;^ . -^,lu l l r -

A'

,.i :r'"...il ip:=t:, ' ,t h"l

@(Da

i'oo(!

f

(!

:at

0,

<oo

x

$

lJ)od)

oo,(t)

i'ootf

34

1.E+(X

l.E+04 l.E+Gs CS

1.E+06

Figure 3. tttCs tzrsn.y ssr

Open circles are data from the present work, black circles are from [2]

Colored contour maps of eosr and r3?Cs pollution patterns were generated usingGlS-technology (Figure 4). It can be seen from Table 2 that in the entire sampling areathe values for sSr are 40-2000 times higher and the values for r3?Cs are 10-80 timeshigher than typical background level for corresponding soils in Aarkrog et al's snrdylssr - 1.6 kBq/m2, 'ttcs - 2.56 kBq/n2) in areas not appreciably affected by fallout fromthe accidents discussed above. Though the present levels of soil contamination withradioactive sSr and r3tCs exceed tlTicat background levels for the No(hern hemisphereby a factor of 2-5, the radiation doze from these radionuclides does not imply anyhazardous health impact on local residents. At the same time, fiuther investigations arenecessary to determine the plutonium impact, as well as the combined impact ofradionuclides and heavy metals on the environmental situation in this region.

Acknowledgements

The authors gratefully acknowledge cooperation and financial support for this study bythe International Atomic Energy Agency (Crp <Biomonitoring Air Pollution ThroughTrace Elements>, research contract No. 9939/Ro).

1.E+03

90S r

13 7cs

e ExarEfifrdlpr

s Exalagstrypr

35

kl3q/m'?

tu <23

tll zs -4.3

E$ 4..s -6 2

% 6.2 -a

W 'r- io

ffi 1{) 20

I 2a-4.r

I 40-1co

I ,1oo

kBq/m'z

l,'att1 < 5

ln'::f 5 -g

Hi3 a -11E$i

W 11 -14W

m 14 - ' t t :

I in21

I zt-24

I 24-4t)

l : ;4,r1

i,t,,*,,,|

; :,:,,ti;.j, ,i:ttj I :i..t,:i

,,ril

d: + l : l.A

n4*4, ,d , t * .

r ' r SontdhHcx

I

li:i::r : {::t !(sei.'. cps^tnxr

tr 9onqfHHcK

*T

ra

1: :

q he+:

, ,:1

Figure 4. eoSr and l37Cs pollution maps in the examined area of the Chelyabinsk region.

iFor orientation: gert6uHcK - Cheljabinslq Exarapnn6ypr - Ekatarinburg)

36

References

).

6.

7.

Cherchintsev, V.D., Frontasyev4 M.V., Lyapunov, S.M., Smimov, L.l. (1999) Biomonitoring AirPollution in Chelyabinsk Region (Ural Mountains, Russia) Through Trace-Elements and Radionuclides:Temporal and Spatial Trends. In Report on the First Research Co-ordination Meeting (RCM) <Co-ordinated Research Project on Validation and Application of Plants as Biomonitors of Trace ElementAtmospheric Pollution, Analysed by Nuclear and Related Techniques>, NAHRES-43, IAEA, Vienna,r36- I 54.Aarkrog A, Dahlgaar4 H., NielserL S.P., Trapeznikov, A.V., Molchanova, I.V., Pozolotina, V.N.,Karavaeva" 8.N., Yushkov, P.I., Polikarpov, G.G. (1997) Radioactive inventories from the Kyshtymand Karachay accidents: Estimates based on soil samples collected in the South Ural (1990-1995\, TheScience ofthe Total Enviroment 2Ol, 137-154.I. Linkov and R. Wilson (eds), (1998) Air Pollution in the Ural Mountains. Environmental, Health andPolicy Aspects. Kluwer Academic Publishers, Nato ASI Series 2, Environment 40, 450.Bradley, D.J. (1977) Behind the Nuclear Curtain. Radioactive Waste Management in the Former SovietUnion. Edited by David R. Payson" Battelle Press, Columbus Richland, 371-450.Romanov, G.N., Voronov, AS. (1990) Radiation situation after Kyshtym accident. Nature 5,50-52 (inRussian).Romanov, G.N., Spirin, D.A., Aleksahin, R.M.(1990) Radioactive substances in environment. Nature 5,53-58 (in Russian).Nifontova, M.G. (1995) Content of longJived radionuclides in the moss cover of the Eastem-UralRadioactive Trace region; Ru ssian Journal ofEcologlt 26,300-303.Nifontova" M.G. (1998) Accumulation of long-lived artificial radioactivity by moss and lichens in Ural-Siberia region; EcologSt 3, 196-200 (in Russian).