CHARACTERISTICS OF SPHERICAL Cs-BEARING PARTICLES COLLECTED DURING THE EARLY STAGE OF FDNPP ACCIDENT
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1 CHARACTERISTICS OF SPHERICAL Cs-BEARING PARTICLES COLLECTED DURING THE EARLY STAGE OF FDNPP ACCIDENT Yasuhito Igarashi, Kouji Adachi, Mizuo Kajino & Yuji Zaizen Atmospheric Environment and Applied Meteorology, Meteorological Research Institute 1-1 Nagamine, Tsukuba, Ibaraki , Japan Corresponding author:
2 Talk outline Research backgrounds, aims of the present study and so forth Radioactive aerosol sampling at the Meteorological Research Institute (MRI), methodologies for analysis of Cs-bearing particles with state-of-the-art instruments including scanning electron microscope (SEM) Characteristics of spherical Cs-bearing particles including morphology, size and major components Modeling approach with state-of-the-art aerosol transport simulation considering the present spherical Cs-bearing particles Summary
3 Radioactivity deposition (mbq/m 2 /month) Research Background: Temporal change in atmospheric deposition of radionuclides at MRI, Japan Cs 90 Sr Koenji, Tokyo Max. 137 Cs depo.: 550 Bq/m 2 in June 1963 Tsukuba Chernobyl Accident 137 Cs depo.: (23±0.9) 10 3 Bq/m 2 in March 2011 Fukushima Accident Nuclear tests by former USSR, USA, etc. Max. 90 Sr depo.: 170 Bq/m 2 in June, 1963 Nuclear tests by China 90 Sr depo.: 4.4±0.1 Bq/m 2 in March Year
4 Fukushima radioactivity emission inventory Just a few kgs in weight Nuclear and Industrial Safety Agency Estimate Emission in mass Nuclide Half life Emission/g Nuclide Half life Emission/PBq Xe ｄ 1590 Kr y Xe d Te-129m 33.6d 3.0states Investigation is needed regarding mixed Te-129m 33.6d 3.3 Te ｄ 7.8the Te-132with 3.26dnot only 88 the radionuclide but also I d 160 I d 35 atmospheric aerosol. I d general 42 I h 1.0 Cs y 18 Most of radionuclides occurred in the380 aerosol Cs d Cs y Cs-137form, 30.0y which 15 floated and transported in the Cs y 4660 Sr d 2 atmosphere. Sr y 0.14 Sr d 1.9 Pu ,065y Sr ｙ 28 Pu-240 6,537y Pu ｙ 1.4 Conversion Pu ｙ 0.4 Cf. Daily SO2 emission in Japan g EAGrid2000
5 Hygroscopicity Deposition of aerosols in environ. and humans Dry depo. onto forest Inhalation Radioactive Aerosols Aerosol size=physical and hygroscopicity=chemical information are very Deposition important! rate From Petroff et al. (2008) Wet depo.: CCN activity Kajino, Igarash & Fujitani, Jpn. Soc. Atmos. Environ., 2014 (in press) Particle size
6 POLLUTION MAP Tsukuba Result of aircraft monitoring made by the Ministry of Education, Culture, Sports, Science and Technology (MEXT) (Total of cumulative 134,137 Cs pollution of the surface (kbq/m 2 ) in the range that the survey completed up to fall, 2011) Nov. 11, 2011 Announcement
7 Sampling, sample preparations and radionuclides measurements HV filter sampling 8" 10 Quartz fiber filter Until March 2011 Total = Wet and dry deposition sampling 4 m 2 deposition sampler Stocked samples Punched out 33 mmφ For Sr analysis For γ-measurement For γ-measurement Hydraulic press machine Rotary evaporator
8 Activity concentration (Bq/m 3 ) Radioactivity in aerosol samples at MRI in March Mo 132Te 131I 129Te 129mTe 133I 134Cs 137Cs 136Cs In logarithmic scale 10-4 ND levels /11 3/15 3/19 3/23 3/27 3/31 Date Igarashi et al., ICAS2011
9 Event 1 Event 2 Imaging plate picture of HV filter sample The BG image with homogeneous distribution vs Hot spots with irregular distributions like Japanese sesame senbei. = Strong radioactive particle was seen. However, the black spot in the image doesn't show the size of the particle directly. Digital radiography with courtesy of Dr. Osada, Nagoya Univ. #5 March/14-15 (700 m 3 ) #6 March/15a (253 m 3 ) #7 March/15b (233 m 3 ) In April 2011 (more than a month later the accident) images were taken. HV filter samples collected at MRI #8 March/15-16 (498 m 3 ) #14 March/20-21 (487 m 3 ) #15 March/21-22 (1011 m 3 )
10 Exploit for strong radioactive particle Providing position data SEM image of quartz fiber filter IP imager Micro-manipulator Low vacuum-low acceleration bias SEM with EDS mapping Pick up Extraction of the particle Nano-XRF Activity measurement with Ge detector
11 Exploit for strong radioactive particle Adachi et al., Sci. Rep., 2013; doi: /srep02554 Particle1 2.6 µm 3 cm 1 cm 1 mm 100 μm Downsize 2 μm
12 SEM image of particle µm Cs-ball Detected elements by EDS: O, Na, Si, Cl, Fe, Mn, Zn, Cs Adachi et al., Sci. Rep., 2013; doi: /srep µm
13 Intensity (a.u.) Adachi et al., Sci. Rep., 2013; doi: /srep02554 EDS Cs Cs Fe spectrum of d) Particle 1 Mn Zn 5 10 kev Si C O Na S Ca K Cs Fe Zn Pb Pb Substrate (back g round) kev
14 Elemental mapping by EDS analysis Particle 1
15 Gamma-spectrum of Cs-ball from Mar HV filter Measurement: 50,000 sec Particle Cs: 3.27 ± 0.04Bq 134 Cs: 3.31 ± 0.06 Bq ~6 Wt% within the particle Particle Cs: 0.66 ± 0.02 Bq 134 Cs: 0.78 ± 0.04 Bq ~3 Wt% within the particle Photo peaks with * are from the background or the glass substrate. Adachi et al., Sci. Rep., 2013; doi: /srep02554
16 Collection of Cs-ball Particle 4 Particle 2 O, Si,Cl, K, Fe, Zn, Rb, Sn, Cs Fe, Zn, Cs 137 Cs: 1.4±0.1 Bq, 0.13 TBq/g 3.0 µm 3.3±0.2 Bq, 0.06 TBq/g 1.7 µm Particle 5 Specific activity calc. assume density of 2 g/cm 3 Particle 3 O, Na, Cl, K, Fe, Mn, Zn, Cs Particle 6 from Tsukuba Univ. 1.3 µm 1.0±0.1 Bq, 0.2 TBq/g C, O, Na, Cl, Fe, Zn, Rb, Sn, Cs 2.1 µm 2.2 µm 1.4±0.1 Bq, 0.1 TBq/g O, Cl, Fe, Zn, Rb, Sn, Cs
17 Cesium isotopic composition of Csball (In total 7 particles) 134 Cs/Bq y = x R² = Decay corrected as of March 14, Cs /Bq *One data was not yet subjected to SEM analysis.
18 Particle number in which corresponding element was found Elements identified in Cs-ball by SEM-EDS (In total 6 particles) C O Si Na Cl K Mn Fe Zn Rb Sn Cs
19 Normalized intensity Cs-L Fe-Kα Fe-Kβ Mo-Kα Mo-Kβ Pb-Lβ Rb-Kα Rb-Kβ Zr-Kα Sb-Kα Te-Kα Ba-Kα Zn-Kα Zn-Kβ Pb-Lα Sn-Kα Cs-Kα Thom. Scat. (37.5 kev) Results of synchrotron radiation-μ-xrf analyses (vs. Thom. Scat.) Particle - Background (carbon tape) Sn-Kβ 1,3 Sn-Kβ 2 Cs-Kβ 1,3 Cs-Kβ Energy /kev Comparison of XRF spectra of the particle and background (37.5 kev-excited). Ba-Kα Cs-Kα Te-Kα Sb-Kα Sn-Kα Mo-Kα Zr-Kα Rb-Kα 2 μm Pb-Lα Zn-Kα Fe-Kα SEM image Results of μ-xrf imaging analysis (37.5 kev-excited) and SEM image of the particle. Elements in particle: Ba, Cs, Te, Sb, Sn, Mo, Zr, Rb, Zn, Fe (Pb : derived from an attached fragment of the filter) Unpublished data: Courtesy of Prof. Nakai and Dr. Abe, Tokyo Univ. Sci.
20 Extraction efficiency of 137 Cs from HV filter samples Mar sample contained insoluble materials not only in water but hot nitric acid! Characteristics of Mar.20 plume and particles seem to be different from those of
21 SEM image of a remained particle on HV filter after nitric acid extraction Mar. 15 sample IP exposed for 24h. Particle µm Similar type of Cs-ball was found! 0.3±0.03 Bq Detected elements by EDS: O, Si, Na, Ca, Mg, Fe, K, Al, Cl, Zn, Cs
22 Coagulation Wet deposition (Rain, Snow) Dry deposition MANAL-NHM-PM/r (Δx=4km) (Passive-tracers Model for radioactivity, off-line coupled with NHM) Aerosols Dissolution Hydrometeors Gas Condensation/ Evaporation ATK PRI CCN activation CLD RNW ACM SS Cloud microphysics SNW DU POL IN activation ICE GRW Coalescence ATK (Aitken mode), PRI (primary radionuclides), ACM (accumulation mode),du (dust), SS (sea salt), POL (pollen)
23 Difference in simulated depo. due to difference in aerosol characteristics March 11 to 22, 2011 Total depo.(kbq m -2 ) Cs depo. emitted on March 14 only (kbq m -2 ) Submicron hygroscopic (CMD = 102 nm, κ=0.4) CMD= 2μm, κ=0 Dry depo. velocity becomes about 4 times. No CCN activity. Removal by only rain drops encounter (scavenging).
24 SUMMARY 1 We have found spherical Cs-bearing particles (Cs-ball) from HV filter samples collected during Mar , 2011, when the first radioactive plume arrived from the FDNPP accident at the MRI as well as Univ. Tsukuba, Japan So far seven Cs-balls were found from any given black dot on IP image of the filter sample. They have basically spherical morphology, characterized composition of Fe, Zn, Mn, O, etc. with an appreciable amount of elemental Cs. They are a few microns in diameter (corresponding to PM2.5) with a few Bq activity but as high specific activity as sub-terra Bq/g. They are insoluble; even refractory to conc. nitric acid. Also, the extraction experiments showed that the Cs-ball occupied major part in the Mar Fukushima plume. They would persist for a long time in the environment as well as in living organisms.
25 SUMMARY 2 While the investigation on radioactive aerosol during the second plume arrival gave no such Cs-ball. Aerosol model simulation gave the results that nonhygroscopic super-micron Cs-ball could be removed more by the dry deposition and below-cloud scavenging than conventional sulfate-hosted particles. A few Cs-balls have been subjected to the analysis of synchorotron X-ray analyses by using Spring-8 (Prof. Nakai and Dr. Abe, Tokyo Univ. Sci.). The finding should be a key to understand the processes of the FDNPP accident, to accurately evaluate the health and environmental impacts and to improve efficiency of the decontamination of the polluted area. Further studies are recommended for the present Cs-ball in more detail!
26 ACKNOWLEDGMENT Y. Igarashi acknowledge the following people for their support and collaboration; Prof. I. Nakai, Dr. Y. Abe and Mr. Iizawa (Tokyo Univ. Sci.) for their advanced analysis by using Spring-8. Prof. Sueki and Mr. Sato (Univ. Tsukuba) for providing a filter sample Dr. M. Mikami (MRI) for general support and Dr. M. Aoyama (MRI) for helping HV sampling Mayama, Hida, Kimura, Sako, Inukai, Kamioka, Iwai, Kamiya, Yanagida, Nabeshima, and Takeda (Part-time & temporary staffs at MRI) Prof. K. Osada (Nagoya University), Prof. Y. Oki and Dr. Osada (Kyoto Univ. Res. Reactor Inst.) Prof. Y. Onda (Univ. Tsukuba), Prof. T. Nakajima (Tokyo Univ.), Prof. M. Ebihara (Tokyo Metro. Univ.), Prof. A. Shinohara (Osaka Univ.) and others
A n earthquake with a magnitude of 9.0 occurred in Japan on March 11, In addition to the earthquake
OPEN SUBJECT AREAS: ENVIRONMENTAL SCIENCES ENVIRONMENTAL MONITORING ATMOSPHERIC CHEMISTRY GEOCHEMISTRY Received 12 June 2013 Accepted 15 August 2013 Published 30 August 2013 Correspondence and requests
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