ANALYSIS OF FUKUSHIMA S ACCIDENT BY FRENCH NATIONAL DATA CENTER

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1 ANALYSIS OF FUKUSHIMA S ACCIDENT BY FRENCH NATIONAL DATA CENTER G. LE PETIT, P. ACHIM, P. GROSS, G. DOUYSSET, M. MONFORT C. JUTIER, T. TAFFARY, X. BLANCHARD, C. MOULIN, T. HERITIER Commissariat à l Energie Atomique French Atomic Energy Commission CEA, DAM, DIF, F Arpajon, France

2 CEA (hosting French NDC) was relying on the CTBT IMS network data in order to: Assess the severity of damages of Fukushima s reactor cores Validate the atmospheric transport modeling for predicting the time evolution of the contaminated air masses over the globe Estimate the potential radiological impact Fukushima nuclear power plant 200 km Takasaki site (IMS stations JPP38 & JPX38) NOP CAP15 49 USP76 CAP16 ISP34 SEP63 RUP55 RUP57 RUP54 RUP59 RUP56 RUP60 USP71 CAP14 CAP17 DIF DEP33 RUP61 MNP45 CNP20 RUP58 USP70 USP74 USP75 PTP53 IRP36 CNP21 JPP38 USP78 MXP44 USP72 LYP41 KWP40 MRP CNP22 JPP37 USP79 FRP28 USP77 43 NEP48 THP65 PHP52 PAP50 USP80 FRP31 CMP13 ETP25 KIP39 ELP24 GBP66 MYP42 TZP64 PGP51 BRP12 AUP08 AUP09 FJP26 GBP67 FRP27 ARP02 AUP06 CKP23 BRP11 FRP29 CLP19 ARP01 AUP10 NZP47 GBP68 AUP04 NZP46 ARP03 ZAP62 FRP30 CLP18 AUP07 USP73 AUP05 FRP32 GBP69 Summary Information got from IMS RN stations detections Estimation of the Fukushima s source terms Assessment of the radiological impact due to 131 I (major contributor) Particulate network availability during Fukushima event: 80% International Monitoring System of the CTBTO (radionuclide particulate station network)

3 FRENCH NATIONAL DATA CENTER LOCATED AT BRUYERES-LE-CHATEL (40 KM SOUTH OF PARIS) Geophysical data analysis room Radionuclide data analysis

4 IMS Data Source (Raw spectral data input) -Noble Gas stations CTBTO network -Particulate stations CTBTO network -National Means (particulates and noble gas stations) Other data sources European Radionuclide particulate stations, CTBTO products -Particulate Radionuclide stations (ARR/RRR) -Laboratory CTBTO network Source terms analysis External data, calculations Global Analysis and forecasts (whole globe, 0.5 resolution, 6hr) European data: ECMWF US NCEP data: GFS, FNL Automated /Interactive Analyses CEA Data Base Data fusion processing Screening events Global coherence Analyses Radiological impact calculations Reporting: maps, interpreted data French National Data Center

5 IMS particulate station current sampling-measurement cycle 24 hours 24 hours 22 hours Sampling Volume sampled: up to m 3 (filter traps atmospheric dusts) Sample decay (after compression of the filter) Gamma standard source measurement (Checking of the detection chain) 1 h The sample is analyzed by gamma spectrometry (one spectrum sent each 2 hours) IDC-Vienna NDC s

6 Fukushima s contaminated air masses arrival at the Takasaki IMS particulate station (JPP38 about 200 km from Fukushima site) Contaminated air masses originated from Fukishima nuclear power plant reached the Takasaki IMS stations during the measurement of the sample collected on 2011/03/12 Cycle: 24 hours Contaminated air masses get into the station premises /03/12 06H55 UTC 2011/03/12 13H55 UTC 2011/03/12 18H55 UTC 2011/03/13 01H55 UTC 2011/03/13 06H55 UTC 2011/03/13 13H55 UTC 2011/03/13 18H55 UTC 2011/03/14 01H55 UTC 2011/03/14 06H55 UTC 2011/03/14 13H55 UTC 2011/03/15 01H55 UTC 2011/03/15 05H00 UTC 2011/03/15 06H30 UTC 2011/03/16 00H50 UTC 2011/03/16 06H30 UTC Unit 1 explosion: 2011/03/12 06H30 UTC Unit 3 explosion: 2011/03/14 02H30 UTC Unit 2 explosion: 2011/03/14 21H00 UTC

7 Takasaki station (JPP38) : First IMS station detecting Fukushima s contaminated air masses (in the station premises) Fission products were detected during the gamma spectrometry measurement of sampling collected on March 12 starting 06H55 UTC Acquisition time: 20 hours Acquisition time: 22 hours 132 Te 131 I Resolution was improved by operators Spectrum with poor resolution 15 March h00 UTC No fission product detected At that time the sampling contains only natural radionuclides 22 hours 2 hours Fission products detected in the station premises (difficulty for the measurement)

8 Second spectrum with fission products at IMS Takasaki station (JPP38): collection on March 13, /03/13 06H55 UTC (collection start) Optimal spectrum resolution 1001 kev 234m Pa 238 U? 234m Pa 238 U venting at Takasaki? Volatile and semi volatile fission products are first detected from the spectrum acquired at the station: 131 I, 132 I, 133 I, 134 Cs, 136 Cs, 137 Cs, 129 Te, 129m Te, 99m Tc, 99 Mo, 140 La Our concern at that time: what about 234m Pa ( 238 U)? Again it was supposed that air contaminated got into the station premises (order of 131 I concentration activity: ~10 Bq/m 3 )

9 CTBT Laboratories measurements on sampling collected at Takasaki (JPP38) following a major release (collection on March 22 06h55 to March 23 06h55 UTC) Volatiles isotopes detected at the station are confirmed and quantified: 131 I, 132 I, 133 I, 134 Cs, 136 Cs, 137 Cs, 129 Te, 129m Te, 99m Tc, 99 Mo, 140 La (major isotope: 131 I, 2 Bq/m 3 ) In addition, other isotopes were quantified: 110m Ag, 125 Sb, 86 Rb, 140 Ba, 95 Nb, 103 Ru FIL Ru (497 kev) 95 Nb (766 kev) FRL08 FIL07 Several late measurements have confirmed this isotope FRL08 Laboratory results provide valuable information on the reactor damages: detection of 103 Ru ( Bq/m 3 ) and 95 Nb ( Bq/m 3 ) Lesson learned: in case of high activity, useful to measure a sample several times

10 Atmospheric activity concentrations at Takasaki versus estimate core reactor activities (normalized to Cs-137), 10 days after the shutdown of the reactors Cesium and Rubidium (same behavior) Good coherence between activity concentrations Cs-137 Cs-134 Cs-136 Rb-86 Te-129m Te-132 I-131 Mo-99 Sb-125 Ag-110m Xe-133 Ba-140 La-140 Nb-95 Ru ~ measured in air and initial core inventory Volatile isotopes Tellurium Good coherence between the two isotopes Volatile isotopes Iodine High volatility in transportation Antimony, molybdenum and silver Semi-volatile isotopes Xenon Very high ratio complete absence of retention Baryum, lanthanum, niobium and ruthenium Detection of the refractory isotopes involves a high temperature in the reactor core and very probable core nuclear meltdown Information available on April , following the analysis of the JPP38 filter by laboratories

11 Isotopic ratios comments: example of USP71 station (Sand Point USA) estimates core reactor activity ratio: ~0.8 (on March 11, 2011) estimates core reactor activity ratio: ~3 (on March 11, 2011) Isotopic ratios given on March Isotopic ratios given on March estimates core reactor activity ratio: ~7 (on March 11, 2011) estimates core reactor activity ratio: ~12 (on March 11, 2011) Isotopic ratios given on March Isotopic ratios given on March Reasonable agreement with ratios calculated from the inventory of Fukushima reactor cores (for isotopes with same physical-chemical behaviour) Poor agreement is achieved for isotopes with different physical-chemical behaviour (due to difference on volatility, case of I/Cs) Certain trends are currently not completely explained: more works needed

12 Fukushima s contaminated air masses arrival at the Takasaki IMS Noble Gas station (JPX38 about 200 km from Fukushima site) blank acquisition sample acquisition JPX38_002 (Detector N 1) blank acquisition sample collection 2011/03/12 Sauna system β γ coïncidence mode sample acquisition blank acquisition sample collection 2011/03/13 Cycle: 12 hours Only a part of the sampling (2h/12h) on March 14, 2011 is concerned by the Fukushima releases sample acquisition blank acquisition sample collection 2011/03/ /03/16 00H50 UTC sample acquisition Radioxenons coming from Fukushima site detected sample collection 2011/03/15 blank acquisition JPX38_001 (Detector N 2) sample collection 2011/03/12 blank acquisition sample acquisition Blank acquisition sample collection 2011/03/12 sample acquisition sample collection 2011/03/ /03/15 01H55 UTC 2011/03/15 05H00 UTC Dating by Particulates only

13 Detection of 133 Xe at Takasaki (JPX38) Raw gamma signals Raw beta signals beta-gamma signal Normal sample, small amount of radioxenon beta-gamma signal usable (Average 133 Xe air concentration (2010) for JPX38 Takasaki-Japan : Bq/m 3 ) Collection: March , 18:43 March , 06:43 (UTC), Takasaki (Japan) sample Background (detector and gas) The Net gamma signal was analyzed by French NDC to give a rough estimate of 133 Xe air concentration at Tagasaki (JPX38 station) Usual analysis is NOT POSSIBLE (Out of the dynamic range of the system) BUT GAMMA SIGNALS REMAIN OF INTEREST!

14 Very soon, it was clear that due to high activity concentrations of the first samplings (out of the dynamic range of the detection system), major corrections or/and specific procedures have to be applied to achieve reliable results 133 Xe activity concentration (Bq/m 3 ) at Takasaki Japan (JPP38) 1500 Bq/m 3 on March (French NDC rough estimate) IDC and NDC automated analysis March (before Fukushima impact) Bq/m 3 (conventional value for Takaski site) French NDC has concentrated its effort on particulates data analysis as xenon level activity measured in air did not imply significant radiological impact

15 133 Xe/ 131m Xe isotopic ratio /03/2011 Radioxenon isotopic signature of Fukushima (independent from the time transportation) 02/04/ /04/ /04/ /04/ /04/2011 IMS station CAX16 French non IMS station IMS station MNX45 The evolution of the ratio over time suggests that no criticality step occurred after the reactor shutdowns 07/05/ /05/2011 Fukushima signature still observable (from Likelihood method used by French NDC on Spalax systems data) 21/05/ /05/2011 From Mid-April 2011, only the ratio 131m Xe/ 133 Xe could be detected by IMS stations; this information is valuable to assess performance monitoring capabilities following Fukushima s accident

16 Air masses atmospheric transport and radiological impact assessment 3D Modelling have been carried out at meso-scale and at global scale Only results at global scale will be presented (using meteorological GFS data (0.5 x0.5 ) and Flexpart 8.2 Lagrangian Dispersion model) March 15, 2011 March 20, 2011 March 25, 2011 April 3, 2011

17 What about source terms: Puffs and continuous releases? Gamma measurements Unit 1 Gamma measurements Main gate Western gate 1.1 km Unit 3 Unit km Unit 4 unit1 Unit4 (f) Unit4 (f) Unit3 (p) Unit2 (s) unit3 unit2 Unit3 (s) Unit3 (s)

18 2.5E E E E E E+00 Atmospheric dusts were daily collected on the Fukushima site by a mobile equipment (car) and measured using gamma spectrometry March March P time time I-131 Cs /16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00:00 05/15 00:00 05/17 00:00 05/19 00:00 P Main Gate I131 Western Gate I131 Main Gate Cs137 Western Gate Cs137 Décroissance I131 Activity concentration (Bq/m 3 ) Reactor shutdown Continuous leakage? From 22 March to 15 May (~2 month) 131 I (decay constant: 8 days) 137 Cs (decay constant: 30 years) Decay with 131 I half-life The decay of 131 I activity strongly suggests a continuous release from March 22, 2011 Before 22 March: 3 puffs following the reactor explosions Source terms profile

19 /03 00:00 14/03 00:00 16/03 00:00 18/03 00:00 20/03 00:00 22/03 00:00 24/03 00:00 26/03 00:00 28/03 00:00 30/03 00:00 01/04 00:00 03/04 00:00 05/04 00:00 07/04 00:00 09/04 00:00 11/04 00:00 13/04 00:00 15/04 00:00 17/04 00:00 19/04 00:00 21/04 00:00 23/04 00:00 25/04 00:00 27/04 00:00 29/04 00:00 01/05 00:00 03/05 00:00 05/05 00:00 07/05 00:00 09/05 00:00 11/05 00:00 13/05 00:00 15/05 00:00 2.5E E E E E E I decay curve fitted on Western Gate TEPCO measurements From 22 March to 15 May (~2 month) Rough estimate of the 131 I source term from the continuous leakage using a Gaussian model = Bq = Bq Weak wind diffusion: 2m/s = Bq Average value used for first step 3D modeling Normal wind diffusion: 5m/s Release at 20m/ ground level 12/03 00:00 14/03 00:00 16/03 00:00 18/03 00:00 20/03 00:00 22/03 00:00 24/03 00:00 26/03 00:00 28/03 00:00 30/03 00:00 01/04 00:00 03/04 00:00 05/04 00:00 07/04 00:00 09/04 00:00 11/04 00:00 13/04 00:00 15/04 00:00 17/04 00:00 19/04 00:00 21/04 00:00 23/04 00:00 25/04 00:00 27/04 00:00 29/04 00:00 01/05 00:00 03/05 00:00 05/05 00:00 07/05 00:00 09/05 00:00 11/05 00:00 13/05 00:00 15/05 00:00

20 Isotope 131 I: comparison simulations/measurements (hypothesis: puffs following explosion and continuous releases) Modelling Measurement 05/13 00:00 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00: USP70 Sacramento USA) USP74 (Ashland USA) Bq Bq Bq Bq Bq Bq Kinetic of releases used for modelling Modelling Measurements Kinetic of releases used for modelling 0 05/13 00:00 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 Activity concentration (µbq/m 3 ) Activity concentration [µbq/m 3 ] Activity concentration (µbq/m 3 )

21 Isotope 137 Cs: comparison simulations/measurements (hypothesis: puffs following explosion and continuous releases) Modelling Measurements 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 Activity concentration [µbq/m 3 ] USP70 Sacramento USA) Bq Bq Bq USP74 (Ashland USA) Bq Bq Bq Kinetic of releases used for modelling Modelling Measurements Kinetic of releases used for modelling 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 Activity concentration [µbq/m 3 ]

22 Atmospheric Transport Modelling at global scale - Far away the source: Reasonable agreement between activity concentrations measured at the stations and those determined from ATM - closed to the source: Poor agreement (case of IMS station JPP38) Size of particles in air is probably very different from a station close to source (coarse particles) compared to a remote station (fine particles have a behaviour quite similar to gas) Regarding iodine calculations, no distinction between vapor and solid (aerosols) phases was taken into account More generally, none physical effects which could impact dust transportation were including in our calculations: Dry deposition over time during the air masses transport (settling,..) Wet deposition (scavenging, washout, ) Consequently it appears that the source terms used for our simulations are probably slightly under-estimated Next step: introduce in the ATM model several physical parameters (dry deposition, washout ) on going work

23 Radiological impact assessment at global scale Integrated dose inhalation (in Sievert) for children related to iodine 131 (major contributor to the dose effect) Weak radiological impact far away from Japan area (in average every human being receives an annual dose of ~4 msv)

24 Isotope 133 Xe comparison simulations/measurements Modelling Measurements Modelling Measurements USX USX74 DEX /12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00:00 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00:00 03/11 00:00 03/13 00:00 03/15 00:00 03/17 00:00 03/19 00:00 03/21 00:00 03/23 00:00 03/25 00:00 03/27 00:00 03/29 00:00 03/31 00:00 04/02 00:00 04/04 00:00 04/06 00:00 04/08 00:00 04/10 00:00 04/12 00:00 04/14 00:00 04/16 00:00 04/18 00:00 04/20 00:00 04/22 00:00 04/24 00:00 04/26 00:00 04/28 00:00 04/30 00:00 05/02 00:00 05/04 00:00 05/06 00:00 05/08 00:00 05/10 00:00 05/12 00:00 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00: Modelling Modelling Measurements Measurements CAX NOX MNX45 Modelling Measurements /12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00:00 03/12 00:00 03/14 00:00 03/16 00:00 03/18 00:00 03/20 00:00 03/22 00:00 03/24 00:00 03/26 00:00 03/28 00:00 03/30 00:00 04/01 00:00 04/03 00:00 04/05 00:00 04/07 00:00 04/09 00:00 04/11 00:00 04/13 00:00 04/15 00:00 04/17 00:00 04/19 00:00 04/21 00:00 04/23 00:00 04/25 00:00 04/27 00:00 04/29 00:00 05/01 00:00 05/03 00:00 05/05 00:00 05/07 00:00 05/09 00:00 05/11 00:00 05/13 00: (3 puffs of Bq, between March 12 and March 16, 2011) Modelling Measurements

25 Three 133Xe releases of Bq between March 12 and March 16, Mar Apr Apr May 2011 CTBT Science and Technology 2011 June 8 to 10 Vienna Austria

26 Conclusion The International Monitoring System (IMS) of the CTBTO including particulates, noble gas systems and additional analysis conducted by the radionuclide Laboratories provides to States Parties through their NDCs unique information in case of major events such as the one that occurred at Fukushima nuclear power plant. IMS data analysis and ATM were used to roughly estimate the source terms and provide an estimate of the radiological impact. Relying on IMS data (especially radionuclide particulates), CEA was able to provide detailed interpretation overtime of the evolution of the Fukushima s event as requested by to the relevant National Authorities. However a lot of work remain to be performed by the scientific community in order to interpret more in depth data collected by the IMS, consolidate results of the atmospheric transport modeling and finalize the radiological impact calculation (especially close to the source). So that IMS potential contribution to crisis management can be properly assessed as it was done in the past following December 2004 tsunami in Indonesian

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