Detection of Fukushima Daiichi nuclear power plant accident radioactive traces in Monaco

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    Fukushima DaiichiAir masses

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    fallout collection were started daily on the 18th of March on theroof of NAEL-Monaco premises. It allowed determining the quan-tity of detectable radionuclides in aerosol samples as well as inprecipitation (dry or wet) samples, to follow the variation of theiractivity concentration and their deposition rates with time.

    sampled air volumewas between 2000 and 6500m3. The ISAP 2000air lter system used was not equipped with charcoal trap, inconsequence only particulate radionuclides (especially hereparticulate 131I) was collected. The air sampler was protected witha locked cover to avoid direct input of rain. The lters were pressedand analysed for gammaemitting radionuclides bymeans of gammaspectrometry in calibrated geometry.

    The precipitation sample was collected using a 2 2 m2 stain-less steel funnel collector, which was installed 15 m above the

    * Corresponding author. Tel.: 377 97 97 72 27; fax: 377 97 97 72 73.

    Contents lists available at

    Journal of Environm

    els

    Journal of Environmental Radioactivity 114 (2012) 131e137E-mail address: m.pham@iaea.org (M.K. Pham).nent and around the northern hemisphere (CTBTO, 2011; Takemuraet al., 2011; Qiao et al., 2011). Traces of contaminated air masseswere detected in most of European countries despite dispersionandwashout along the trip of the contaminated air masses (Massonet al., 2011; Pittauerov et al., 2011). In Europe, the rst signs of thereleases arrived in Iceland seven days after the release while therst peak of activity level was observed between March 28th and30th. The starting of plume was in the northwest and movedtowards southeast with a maximum observed in Central Europe. InMonaco (43730N, 7430E) sampling of aerosols and the rain or dry

    High-Volume Aerosol Sampling Device, produced by INGENIEUR-RO SCHULZE AUTOMATISIERUNGSTECHNIK, Germany). Thedeviceworked with a high precision volumetric ow rate controllerwith linear ow sensor, scaled by controlling temperature andpressure STP (standard temperature and pressure). The samplingwas done daily (starting from 9 am for one cycle of 24 h for eachlter) from 18th March to 4th April and then every two-three daysuntil 7th May 2011. One lter magazine contained 30 lters. Quartzmicrober lters of 0.8 mm pore size and dimensions of 150 mmwere used. The typical air ow rate was 100 m3 per hour. The totalScavengingRadionuclides

    1. Introduction

    Radioactive releases to the atmFukushima Daiichi reactors startedvolatile and/or particulate bound isotransported across the Pacic towar0265-931X/$ e see front matter 2012 Elsevier Ltd.doi:10.1016/j.jenvrad.2012.01.010tively) were observed. The signicant input of Cs and Cs into the Mediterranean seawater column(30 m depth) was detected later, on the 24th of May. Radioisotopes of caesium and iodine were found farabove the applied detection limits, but still with no concern for harmful radiation exposure and publichealth. The contamination gradually decreased in air and activity concentrations returned to backgroundvalues after one or two months.

    2012 Elsevier Ltd. All rights reserved.

    re from the crippledarch 12th, 2011. Moreand radionuclides wereNorth American conti-

    2. Material and methods

    The sampling station was located on the roof of the IAEA-NAELbuilding of the Principality of Monaco (43500 N, 7300 E), which is15 m above the ground level, north-western of Mediterranean Sea.The airltering systemusedwasmodel ISAP 2000 (Fully AutomatedKeywords:Atmosphere(around 0.54). Up to 95% of caesium isotopes were washed out by wet scavenging during 27e28th ofMarch, where the maximum deposition rates of 134Cs and 137Cs (13.7 and 19.1 mBq m2 day1, respec-

    134 137to 137Cs activity ratio was close to 1, which is different from that one observed after the Chernobyl accidentDetection of Fukushima Daiichi nucleartraces in Monaco

    M.K. Pham*, M. Eriksson, I. Levy, H. Nies, I. OsvathEnvironment Laboratories, International Atomic Energy Agency, 4 Quai Antoine 1er, MC

    a r t i c l e i n f o

    Article history:Received 10 August 2011Received in revised form4 January 2012Accepted 16 January 2012Available online 29 February 2012

    a b s t r a c t

    Daily air monitoring of radDaiichi nuclear power plaand 137Cs) were detected. T5th, meanwhile both peaks4th. Their maximum activ

    journal homepage: www.All rights reserved.ower plant accident radioactive

    . Betti00, Monaco

    clides in the Principality of Monaco (43730N, 7430E) after the Fukushimaccident showed that only Iodine-131 (131I) and Caesium isotopes (134Cseak of 131I varied and reached its maximum betweenMarch 29th and April34Cs and 137Cs arrived later and attained amaximum between April 1st andoncentrations in air were 354, 30, and 37 mBq m3 respectively. The 134Cs

    SciVerse ScienceDirect

    ental Radioactivity

    evier .com/locate/ jenvrad

  • this paper wewill treat only radionuclides issued from the accident,which were detected during the period 23rd of March until 8th of

    ental Radioactivity 114 (2012) 131e137ground level with the wall height of the sampler as high as 2.5 m.This collector, designed to prevent evaporation of rainfall, consistedof 3 parallel polyethylene containers (capacity of 200 L each).During rain periods the acidied samples (20e40 L) were takenfrom homogenous bulk samples to determine the activityconcentration for the total (wet dry) deposition. If it was notraining during this period, the samplewas collected by cleaning thesurface of the collector system with diluted HCl (pH 2) todetermine the dry fallout deposition. In cases of low rain deposi-tion, the sample was collected by cleaning the surface of thecollector system with acidied distilled water, combined withwhatever rainfall was collected. The samples were then concen-trated by evaporation to 100 mL and analysed by gamma spec-trometry in well-dened and calibrated geometry.

    Further investigation on the input of 134Cs and 137Cs to theseawater column was studied. The activity ratios, 134Cs/137Cs (i.e.the Fukushima contribution, assuming no 134Cs from other sources)were determined in large volume samples (up to 5000 m3) ofMediterranean Sea sampled near the Oceanographic Museum inMonaco at a water depth of 30 m (4343.080N, 0725.060E). Thewater sampling was performed in-situ by pumping ltered (1 mm)seawater through copper ferrocyanide-impregnated cotton-woundcartridge lters (Roos et al., 1994), i.e. in this case no Cs radio-chemical yield determination by 134Cs tracer was used. Thesesamples were taken twice a month, starting from mid-April. Inaddition to the in-situ seawater samples, a separate sample wastaken where the radiochemical yield determination with 134Cs wasadded for the determination of the 137Cs activity concentration. Thecotton-wound cartridge lters were ashed in the furnace (to 400 Cmaximum) and analysed in the very low-background level anti-Compton underground gamma spectrometry.

    2.1. Determination of the activity concentrations of gamma emitters

    Activities of the samples collected were measured by gammaspectrometry using coaxial HPGe detectors (Canberra IndustriesInc. USA), which were located in the IAEA-NAEL undergroundlaboratory. Details of the low-background gamma-ray detectionsystem and calibration procedures are described elsewhere(Povinec et al., 2004, 2005). The uncertainties reported are propa-gated errors arising from the one sigma counting error due todetector efciency calibration and background correction, using theformulae of uncertainty calculation previously described (Dovleteand Povinec, 2004). The calculated activities were corrected forradioactive decay to the mid-collection period. Typical propagateduncertainties were from 2 to 10%, depending on the activity levelsof different radionuclides detected. Meteorological data for thesampling station for each sampling period were obtained usingKIMO system (which contains software named KILOG which allowsquerying, retrieving and processing the data recorded by temper-ature, humidity and pressure recorders. Recorders and KILOG aredeveloped by the KIMO company, France) directly located at thesampling site.

    3. Results and discussions

    The analysis of gamma spectra of aerosol and precipitationsamples showed that only 131I, 134Cs and 137Cs were detected inMonaco air after the Fukushima Daiichi accident. The gamma linesfromnatural origin radionuclides such as 7Be, 40K, 210Pb and radiumdaughters (214Bi, 214Pb.) were of course also observed in thesegamma spectra. The temporal changes of 7Be, 137Cs and 210Pbactivity concentrations in surface air at Monaco for a long period(1997e2010) and their correlation with meteorological parameters

    M.K. Pham et al. / Journal of Environm132have been discussed in a previous publication (Pham et al., 2011). InMay 2011. Two different origin radionuclides 7Be (cosmic) and 210Pb(terrestrial) were used to interpret the data together with localmeteorological parameters.

    The arrival and the diffusion of these radionuclides over allEuropean countries after Fukushima events as well as back-trackingtrajectory were described elsewhere (Masson et al., 2011, http://www.zamg.ac.at/; http://www.irsn.fr/FR/popup/Pages/irsn-meteo-france_Film-Global_8avril.aspx; http://www.kantei.go.jp/foreign/kan/topics/201106/iaea_houkokusho_e.html; http://www.nisa.meti.go.jp/english/les/en20110412-4.pdf, etc.).

    In this paper we will discuss only the activity concentrations ofthese radionuclides in aerosol and precipitation samples and theirevolution with time. More investigation of the fate of these radio-nuclides in soil after deposition will be done later for 134Cs and137Cs. The 131I was no longer detectable after one or two monthsdue to its short life time.

    3.1. Radionuclides in aerosol samples

    Following the Chernobyl accident on the 1ste3rd of May 1986,more than 28 radionuclides (long and short half-lives) mainlyssion products after the nuclear disaster were detected in Monacoair (Ballestra et al., 1987; Whitehead et al., 1988). This abundance ofradionuclides was due to the proximity of Monaco with the acci-dent site in Ukraine and to the occasional EasteWest air circulation.The gamma spectra of aerosol samples taken inMarch 2011 showedonly signicantly peaks of 131I (364.5 keV, T1/2 8.02 days), 134Cs(604, 795 keV, T1/2 2.07 years) and 137Cs (661.5 keV, T1/2 30years) that were attributable to Fukushima, and 7Be (477.6 keV),210Pb (46.5 keV) that were attributed to the cosmic and naturalterrestrial origin, respectively. The activity concentrations of theseradionuclides as well as 7Be and 210Pb are shown in the Table 1. Thevariations of 131I, 134Cs and 137Cs activity concentrations (and theiractivity ratios) with time are in Fig. 1 and Fig. 3, respectively. Theother signicant peaks of 214Pb (352 keV) and 214Bi (609 keV)(radium daughters) were also observed but not subject to be dis-cussed in this paper.

    Many more volatile or non-volatile radionuclides were releasedfrom Fukushima Daiichi. Japanese data from the near-eld pub-lished by TEPCO1 and MEXT2 indicated high concentrations in theenvironment of Cs-isotopes and 131I, but signicantly lower activ-ities for others such as 90Sr and plutonium isotopes. However only131I, 134Cs and 137Cs could be detected inmost of European countriesbecause of dispersion and washout along the trip of the contami-nated air masses (Masson et al., 2011).

    There were several peaks of particulate 131I and it reached itsmaximum between March 29th and April 5th (Fig. 1, Table 1),meanwhile both peaks of 134Cs and 137Cs arrived later and attaineda maximum between April 1st and 4th (Fig. 3, Table 1). The uc-tuation of particulate 131I with peaks of 290, 270 and 354 mBq m3

    on the 29th of March, 2nd and 5th of April, respectively and witha lower magnitude (87 mBq m3) on the 19th of April allowed tosuggest that there were more than one wave/plume of radionu-clides that arrived over Monaco. It is interesting to notice that thesepeaks of 131I coincide with the maximum temperatures duringthese days (Fig. 1), when lower humidity and slightly higher pres-sure were observed (Table 1), although the variation of thesemeteorological parameters did not show much effect on the 7Beand 210Pb activity concentrations in air, as conrmed in our

    1 Tokyo Electric Power Company.2 Ministry of Education, Culture Sports, Science and Technology, Japan.

  • Table 1Activity concentration of radionuclides in Monaco air between 23rd March and 7th May 2011.

    Date I-131 mBq m3 Cs-134 mBq m3 Cs-137 mBq m3 Be-7 mBq m3 Pb-210 mBq m3 T C H % P mBar

    23-Mar-11 7.8 4.6 2.7 1.2 3.9 3.2 3390 260 780 50 17.5 35 96024-Mar-11 8.3 1.4 0.4 0.2 0.7 0.5 3520 260 790 50 16.8 55 102825-Mar-11 8.5 1.5 0.9 0.4 1.4 0.5 3220 240 780 50 15.6 64 102026-Mar-11 28 3 0.4 0.2 1.5 0.5 3160 240 910 50 16.0 65 101427-Mar-11 33 4 0.6 0.3 1.1 0.3 3200 240 740 40 13.8 83 101229-Mar-11 290 20 9.9 2.6 13 3 2440 190 410 40 17.1 66 101230-Mar-11 215 17 7.5 1.6 7.6 2.3 1660 130 620 40 15.1 74 101431-Mar-11 190 15 7.6 1.9 8.2 2.6 1800 140 750 40 17.5 67 101801-Apr-11 270 20 23 2 23 2 2070 160 580 40 17.8 72 102002-Apr-11 200 15 30 2 32 2 3420 260 815 50 17.4 72 101704-Apr-11 220 20 30 3 37 4 3920 300 830 50 17.1 73 101205-Apr-11 354 27 21 2 23 2 6590 490 580 40 19.7 52 101907-Apr-11 156 12 20 1 19 1.4 6600 490 870 50 19.4 63 100009-Apr-11 99 8 20 1 22 1 6140 460 1008 55 18.5 72 101811-Apr-11 48 4 9 1 12 1 5970 450 1266 70 21.1 63 101814-Apr-11 76 6 12 1 14 1 5690 420 320 20 20.0 65 101416-Apr-11 87 7 5.6 0.7 8.5 0.8 4650 350 540 30 21.6 35 101819-Apr-11 48 4 9.8 0.6 11.5 0.7 5400 400 740 40 20.7 41 100021-Apr-11 38 4 6.5 0.8 7.7 0.8 5740 430 905 60 19.9 43 101524-Apr-11 8.2 0.8 2.4 0.2 3.4 0.3 5020 370 624 30 18.1 69 101327-Apr-11 7.4 0.9 2.3 0.2 3.4 0.3 4920 370 860 50 20.6 57 100705-May-11 3.7 1.3 0.6 0.5 0.7 0.5 7620 570 835 50 20.9 49 101707-May-11 5 1 1.5 0.2 2.1 0.2 9790 730 940 60 21.5 40 1020

    M.K. Pham et al. / Journal of Environmental Radioactivity 114 (2012) 131e137 133previous observation (Pham et al., 2011). However, the variation of210Pb issued from radon emanation from the terrestrial crust seemsto coincidence with some peaks of 131I with a day or two delay(Fig. 2), showing that the radon emanationwas probably inuencedby higher temperatures during these days as well as this particulate131I, but the radon daughter (210Pb), which is not volatile, attainedits maximum activity concentration later.

    From the study of other groups in Europe, the average gaseous/total 131I ratio was 77.2% (Masson et al., 2011). This is the sameaverage value as the one found after Chernobyl (Cambray et al.,1987). According to the measurements taken on the FukushimaDaiichi NPP site from March 22nd to April 4th, the average partic-ulate/gaseous 131I ratio was 0.46 0.17, i.e. a gaseous/total ratio of71% 11%. This is roughly the same as the one observed in Europe,

    131leading to the assumption that I remains mainly in its gaseousform during transport. A rough estimate of the total 131I inventory

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    Fig. 1. Activity concentration of 131I in aerosol samples collected in Monaco (blue line) and thgure legend, the reader is referred to the web version of this article.)(around 1 PBq) that passed over Europe during this period is

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    M.K. Pham et al. / Journal of Environmental Radioactivity 114 (2012) 131e137134it would be relevant to notice that a slightly higher concentration of137Cs in comparison with 134Cs is due to the contribution of re-suspension of 137Cs from soil surface. This contribution is esti-mated around 20% if considering that 134Cs/137Cs ratio is equal to 1in aerosol sample. A rough estimate of the 137Cs inventory (around0.2 PBq) that passed over Europe during this period is around 1e3%of the released amount (6e12 PBq of 137Cs, NISA Japanese Agencyhttp://www.nisa.meti.go.jp/english/les/en20110412-4.pdf).

    In contrast to iodine behaviour, which was mainly found in

    Be-7 Bq/m3 I-131

    Fig. 2. Activity concentration of 131I (blue line), 7Be (red linegaseous form which then disappeared due to a short half-life (8.02days), caesium was rapidly bound to aerosols and thus highlysubject to washout removal by dry or wet deposition. Here we cansee the decrease of caesium isotope activities in air mainly due tothe heavy rain in 27e28th of March (Fig. 3) (see more detail below

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    Fig. 3. Activity concentration of 134Cs and 137Cs and their afor wet and dry deposition). Meteorological local conditions such astemperature, humidity and pressure seemed to have no effect onthe variation of caesium concentrations, conrming our previousstudy (Pham et al., 2011).

    3.2. Comparison of 137Cs activity concentration with other events

    The comparison of 137Cs activity concentration with otherevents such as Chernobyl in 1986 and Algeciras in 1998 are shown

    137

    q/m3 Pb-210 Bq/m3

    d 210Pb (green line) in aerosol samples collected in Monaco.in the Fig. 4. The peak of Cs observed in Monaco after theFukushima incident was much lower than the maximum observedfollowing the Chernobyl accident (2500 times lower) (Ballestraet al., 1987) or Algeciras accident (3 times) (Pham et al., 1999,2011). It is notable that the 134Cs to 137Cs activity ratio was about

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    M.K. Pham et al. / Journal of Environmental Radioactivity 114 (2012) 131e137 1350.54 after the Chernobyl accident (Whitehead et al., 1988), indi-cating a much longer burn-up of the nuclear fuel at Fukushimareactors. The Chernobyl accident occurred in connection witha long lasting graphite re with high temperatures, resulting in farreaching contamination also from less volatile radionuclides and intransport to higher atmosphere.

    3.3. Radionuclides in the precipitation or dry fallout samples

    The activity concentration of 134Cs and 137Cs in the washoutsamples (by dry and/or wet deposition) and their deposition rates,including the precipitation rates during period studied are in theTable 2 and Fig. 5. Some data of sample collection for January and

    Fig. 4. Comparison of 137Cs concentration in the Monaco air from the Fukushima accidenvertical axis).February andMay before and after Fukushima accident were addedto allow the determination of the important washout of theseradionuclides by precipitation scavenging. The activity concentra-tion is expressed in mBq L1 in precipitation case and the depositionrate of radionuclides is expressed in mBq m2 day1.

    The activity concentration of 134Cs was around its detection limit(10 mBq L1) in January, Februaryanduntil 26th ofMarch,meanwhilethe 137Cs activity concentration was observed at 200e590 mBq L1,which is equivalent with 480e2350 mBq m2 day1 (the conver-sion factor, gured in the last column in the Table 2, is done by takinginto account the precipitation rate). This 137Cs was due to local re-suspension as found in a previous study (Pham et al., Submitted forpublication). The 134Cs activity concentration in precipitationduring weekend 27e28th March reached 980 mBq L1 (100 times

    Table 2Activity concentration of caesium and their deposition rates in the precipitation of Mona

    Date Cs-134 mBq L1 Cs-134 mBq m2 day1 C

    January LLD LLDFebruary LLD LLD01e26-March LLD LLD27e28-March 980 60 13,740 790 128 Marche8 April 620 309 Aprile4 May 1220 50 730 30 104e31 May 570 100 270 50 1

    LLD: Lower Limit Detection.higher than detection limit), or equivalent of 13,700 mBq m2 day1,meanwhile the 137Cs activity concentration attained 1370 mBq L1, orequivalent of 19,100 mBq m2 day1. The difference of activityconcentrations between 134Cs and 137Cs is due to the contribution of137Cs re-suspension, which is estimated around 28% (i.e. the differ-ence between two values 980 and 1370 mBq L1 of 134Cs and 137Cs,respectively, divided by the 137Cs value of 1370 mBq L1). Thiscontributiontswellwith that found in the aerosol samples of above20%. From28thMarch to 8thApril therewas no precipitation and thedeposition rates of 134Cs and 137C were due to dry deposition andwere 620 and680 mBqm2 day1, respectively. Theseweremuch less(44e56 times) than the deposition rates due to the precipitationduring 27e28th of March. The deposition rates of 134Cs and 137Cs

    th the Chernobyl (note: 137Cs values of Algeciras and Fukushima events are on the rightwere rather constant from 9th of April to 11th of May(620e680 mBq m2 day1 for 134Cs and 730e940 mBq m2 day1 for137Cs, respectively) and became signicantly lower for 134Cs(270 mBq m2 day1) during the rest of May, where still littleprecipitation occurred. The important peak of 134Cs and 137Cs activityconcentrations or their important deposition rates during 27e28thof March shows that almost 90e95% of caesium radionuclideswere washed out by the precipitation (Fig. 5). The smaller peaks(5e10%) of both 134Cs and 137Cs deposition in the following days (28Marche08 April and 09 Aprile04 May, Fig. 5) would probably t tothe next received wave/plume of radionuclides (see above in theRadionuclides in aerosol samples section) or the re-suspension inaerosol samples, and theywere progressivelywashed out by dry andwet scavenging (08e31 May, Fig. 5).

    co.

    s-137 mBq L1 Cs-137 mBq m2 day1 Precipitation

    mm mm day1

    330 80 1130 280 95 3.4200 80 480 200 91 2.4590 150 2350 600 104 4370 50 19,100 700 28 14

    680 40 0 0570 80 940 50 15 0.6360 120 6300 60 12.5 0.5

  • 4

    in M

    ent3.4. Radionuclides in the seawater at 30 m depth

    Radio-caesium originated from the Fukushima NPP accidentwas rst detected in these seawater samples on the 24th of May2011, i.e. 54 days after the main plume passed Monaco. The reasonof the delay can be explained because the samples were taken fromthe 30m depth meaning that a lag time can be expected for verticalmixing. The seawater concentration of 137Cs was about1.8 0.1 mBq L1, of which 0.26% (0.06%) originating from theFukushima accident assuming a 134Cs/137Cs ratio is 1 in theFukushima fallout.

    4. Conclusion

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    Fig. 5. Deposition rate of 134Cs and 137Cs

    M.K. Pham et al. / Journal of Environm136The daily air monitoring of radionuclides originated from theFukushima Daiichi nuclear power plants accident in Monaco(43500N, 7350E) showed that only 131I, 134Cs and 137Cs weredetected. There were several peaks of 131I and reached itsmaximum between March 29th and April 5th, whereas the highestconcentration of 134Cs and 137Cs in air was between April 1st and4th. There might have been more than one plume of radioactivityreleased (at different concentrations level). Most of caesiumisotopes (up to 95%) were washed out by wet scavenging during27e28th of March, where the maximum deposition rates of 134Csand 137Cs were observed. On the 24th of May the seawaterconcentration of 137Cs was about 1.8 0.1 mBq L1, of which 0.26%(0.06%) originating from the Fukushima accident.

    A rough estimate of the total 131I inventory (around 1 PBq) thathad passed over Europe during this period was

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    M.K. Pham et al. / Journal of Environmental Radioactivity 114 (2012) 131e137 137

    Detection of Fukushima Daiichi nuclear power plant accident radioactive traces in Monaco1. Introduction2. Material and methods2.1. Determination of the activity concentrations of gamma emitters

    3. Results and discussions3.1. Radionuclides in aerosol samples3.2. Comparison of 137Cs activity concentration with other events3.3. Radionuclides in the precipitation or dry fallout samples3.4. Radionuclides in the seawater at 30 m depth

    4. ConclusionAcknowledgementsReferences

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