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Contamination of soil with
radiocesium emitted from
Fukushima Daiichi Power Plant
Katsutoshi Seki (C’est qui?)
Toyo University, Japan
University of Strasbourg
Joint seminar of JSPS - Maison Universitaire France-Japonais
Strasbourg, France
25 November, 2013
1
Hydrology and soil physics
2
Figure cited from http://www.usask.ca/hydrology/CHOverview.php
Movement of water in
unsaturated zone (vadose zone)
My background
• The University of Tokyo (1989 – 2008)
Laboratory of soil physics and soil hydrology
Ph.D. “Effect of microorganisms on soil
physical properties” (1998)
• Toyo University (2008 - present)
Faculty of Business Administration
Teaching environmental science (liberal
education)
• University of Strasbourg (2013.4 – 2014.3)
Numerical simulation of soil water 3
My works related to radioisotopes
• Yamaguchi, Seki, Komamura and Kurishima
(2007) Long-term mobility of fallout 90Sr in
ploughed soil, and 90Sr uptake by wheat grain.
Science of the Total Environment, 372(2-3):
595-604.
• Seki (2011) Remediation of soil contaminated
with radionuclides derived from the
Fukushima Nuclear Plant accident. Journal of
Business Administraion, Toyo University 77:
13-26, in Japanese.
4
Deposition of Cs-137 and Sr-90
5
Tsukuba is 150 km away from Fukushima NPP. Until several months after the accident.
PTBT = Partial Test Ban Treaty
(Meteorological Research Institute, 2011)
1963: PTBT
Yamaguchi et al. (2007)
• Environmental decay factor was calculated.
• CEC was correlated with environmental decay factor and
transfer coefficient to wheat grain.
• I didn’t believe this research would be so useful, but … 6
Safety of 5 walls for NPP
• It was believed (or explained) that radionuclide will
not be emitted in the environment.
7
4: containment building
3: pressure vessel
5: concrete reactor building
1: pellet of nuclear fuel
2: zirconium alloy
Cooling
• After the accident, chain reaction was stopped safely,
as expected.
• The decay heat from fission products had to be
cooled down. However, the cooling system was
broken by earthquake and tsunami. Backup
electricity was also broken by tsunami.
• They poured water in nuclear reactors to cool down,
but TEPCO said the water level was not rising on TV
(14-15 March, 2011). I was scared …
8
Radiation at Isobe, 100 km from Fukushima
9
I was looking at this data on time, and understood that radionuclide was
actually emitted to environment, and traveled 100 km from Fukushima.
http://www.houshasen-pref-ibaraki.jp/present/result01.html
100 times increase !
10
Kyoto, May 15, 2011
Kinkaku-ji (Temple of the Golden Pavilion)
Explosion of 3rd reactor, 11am March 14
11
Actually it was not the only source of emission.
Radiation contour map of Cs-134 and Cs-137 at September 2011 (Yukio Hayakawa)
12
100 km
200 km
50 km
Decreased to 62 % in 2 years
13
Evacuation (20 km) Stay in door (20 - 30 km)
Iitate
Evacuation
14
 160,000 people are
evacuating (December
11, 2012, Fukushima
Minpo news)
 Warning region
 Hard to return region
> 50 mSv / year
 Residence restriction region
> 20 mSv / year
 Preparing for termination of
evacuation
20km
Iitate village
Seki (2011)
• Reviewed emission of radionuclides
• Reviewed soil contamination
• Reviewed remediation strategies
15
Emission of radionuclides from Fukushima Daiichi NPP
Leakage to groundwater
NPP
Emission to air
770 PBq (1015 Bq)
Water emitted
43 PBq
Groundwater
Sedimentation
Groundwater
movement
Plume
Air current
Rain
Fallout
Deposit on
Soil pollution
Direct pollution of plant
Indirect pollution
of plant from root
Livestock
(Remote place)
Ocean
.
(Seki, 2011)
16
(Chernobyl: 5200 PBq)
Converted to iodine
Radioisotopes
17
Radioisotope Half life
I-132 2 hr
Te-132 3 day
I-131 8 day
Sr-89 50 day
Cs-134 2 year
Sr-90 29 year
Cs-137 30 year
Radiocesium movement in soil
• Cs-137 concentration at Lithuania 17 years after
Chernobyl accident (Druteikiené et al., 2011)
0 25 50 75 // 300
Cs−137, Bq/kg
0 1 2 3 4 5
Sand Forest
18
Cs-134 and Cs-137 profile at paddy field at Fukushima
after 2 months from accident
(Shiozawa et al., 2011)
19
Soil in Fukushima
Ministry of Land, Infrastructure, Transport and Tourism, Japan
Mostly brown forest soil and lowland soil. Also volcanic ash soil (Andisol).
20
Cesium adsorption on Clay particle
(Yamaguchi et al., 2012)
21
Phyllosilicate (Sheet of SiO4 tetrahydra)
has siloxane ditrigonal cavity similar to
the size of Cs-
(1) Beidellite (2) Vermiculite, illite
Hydrated ions
ex. Ca2+
It can swell, but when Cs-
enters between sheets, it
shrinks and Cs- is trapped.
Frayed edge site
•Takes long time to access
•Once Cs- is trapped, no escape
•Small ratio to whole charge
•Main cause of Cs- entrapment
RIP (Radiocesium Interception Potential)
RIP
Andisol has small RIP
22
(Vandebroek et al., 2009)
Transfer coefficient (TC)
• Cs-137 in agricultural product
TC = ------------------------------------------
Cs-137 in soil
• TC of brown rice was set as 0.1 on April 8,
2011 by MAFF (Ministry of Agriculture, Forestry and
Fisheries, Japan)
• MAFF published transfer coefficient of
vegetables and fruits on May 27, 2011
http://www.maff.go.jp/j/press/syouan/nouan/110527.html
23
Rice in Fukushima
• Plantation of rice with soil more than 5000 Bq/kg
was prohibited. Temporal regulation was 500
Bq/kg, and TC of 0.1 was assumed.
• At first, most rice was below 500 Bq/kg, but some
rice exceeded 500 Bq/kg.
• Regulation changed to 100 Bq/kg on April 1, 2012,
based on the limit of radiation exposure of 1 mSv
/ year.
24
Radiocesium in soil and rice (2011)
25
(Fukushima Prefecture and MAFF, 2011)
Radiocesiuminbrownrice(Bq/kg)
Radiocesium in soil (Bq / kg)
Potassium in fertilizer (2011)
26
Radiocesiuminbrownrice(Bq/kg)
Exchangeable K2O concentration in soil (mg / 100g)
(Fukushima Prefecture and MAFF, 2011)
Radiocesium in soil and rice (2012)
27
(Fukushima Prefecture and MAFF, 2013)
Radiocesium in soil (Bq/kg DW)
Radiocesiuminbrownrice(Bq/kgFW)
Much better than 2011
Countermeasures (Seki, 2011)
• Stripping of surface soil
• Turn over surface soil with subsoil
• Application of K fertilizer
• Change to crops of low transfer coefficient
• Phytoremediation
• Chemical remediation
28
29
(Twitter @seki, March 25, 2011)
Identify the contaminated area,
remove soil of several cm at the
surface, and discard it as radioactive
waste. Does it work ?
Stripping of surface soil
• As long as radiocesium is in a few centimeters,
it can be removed.
• Planned for paddy field uncutivated after 2011
(> 5000 Bq/kg, ex. Iitate). Once cultivated, it is
ieffective.
• Depth of contamination should be examined.
• Massive amount of soil as radioactive waste
disposal.
30
Radioactive waste disposal site
• Final disposal site is not determined.
• Not enough temporal storage site.
31
Temporal temporal
storage site at Iitate
village
Osamu Ieda
http://www.kyoten.org/top_seminar12.html
Stabilizer of soil
• Difficult to remove surface
soil of paddy field.
• Stabilizer with magnesium
can be used before removal.
• Contaminated soil can be
easily identified.
http://www.s.affrc.go.jp/docs/press/110914.htm
32
Turn over
(Seki, 2011)
33
Change crops
• Change to crops with lower transfer
coefficient.
34
Phytoremediation
• Make plant absorb contamination.
• Experiment with sunflower showed that it is
not very effective.
• Plant should be safely disposed.
• Depth of root and depth of contamination
should be examined.
35
Chemical remediation
• No efficient way of chemical remediation now.
• Cesium is too strongly adsorbed on clay.
• Besides, concentration is less than 10000 times
lower than cadmium contamination.
– 100 Bq/kg of radiocesium = 0.032 ppb
– 400 ppb for Cd
36
Problem for decontamination
• High cost – 100 trillion yen or more, to attain <
1mSv / year.
• Final disposal site is not determined.
37
Battle of soil scientists in Fukushima, Japan
ASA, CSSA and SSSA Annual Meeting, Tampa, Florida, November 4, 2013
• Enhancing vertical transport with artificial macropore
• Device to measure radiocesium concentration
• Cooperation of NGO with researchers to resurrect Fukushima
• Field monitoring system for sediment and radiocesium runoff
• Colloid facilitated transport of radioactive cesium
• Role of clay mineral in radioactive Cs transport
• Recovering soil fertility after stripping
• Burial experiment of soil contaminated by radiocesium
• http://www.iai.ga.a.u-tokyo.ac.jp/mizo/edrp/fukushima/ASA13/
38
Still long way for safeguarding Fukushima
• Nuclear fuel is melt down, how can we take out? We
have no plan yet.
• Nuclear fuels in the pool of 4th reactor are now
transported to safer place.
• Stop the leakage of contaminated water
• Water cleanup system of ALPS (France) – until the
end of 2014
• 40 years is enough?
39
Problems
• Many workers get limit radiation 100 mSv /
year and cannot work any more. They work in
very bad condition.
• Earthquake probability is always high in Japan.
If “unpredicted” accident happens again, who
can do the recovery work ?
• Risk for big earthquake is always large in
Japan.
40
Energy in future
• In Japan, all NPP is stopped now for regular
maintenance. They are waiting for safety
judging.
• Government still wants to promote nuke, but
strong movement of anti-nuke in citizens.
• We need to seek for transition to other energy
sources.
• How about in France ?
41
Final remark
• We are still in the process of recovering from
the disaster.
• This talk focused on soil contamination and
remediation. I would like to contribute
something in this field as a soil scientist.
• France and Japan can share our knowledge
and techniques for better future of our
countries.
42
43
Merci

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Contamination of soil with radiocesium emmited from Fukushima Daiichi Power Plant

  • 1. Contamination of soil with radiocesium emitted from Fukushima Daiichi Power Plant Katsutoshi Seki (C’est qui?) Toyo University, Japan University of Strasbourg Joint seminar of JSPS - Maison Universitaire France-Japonais Strasbourg, France 25 November, 2013 1
  • 2. Hydrology and soil physics 2 Figure cited from http://www.usask.ca/hydrology/CHOverview.php Movement of water in unsaturated zone (vadose zone)
  • 3. My background • The University of Tokyo (1989 – 2008) Laboratory of soil physics and soil hydrology Ph.D. “Effect of microorganisms on soil physical properties” (1998) • Toyo University (2008 - present) Faculty of Business Administration Teaching environmental science (liberal education) • University of Strasbourg (2013.4 – 2014.3) Numerical simulation of soil water 3
  • 4. My works related to radioisotopes • Yamaguchi, Seki, Komamura and Kurishima (2007) Long-term mobility of fallout 90Sr in ploughed soil, and 90Sr uptake by wheat grain. Science of the Total Environment, 372(2-3): 595-604. • Seki (2011) Remediation of soil contaminated with radionuclides derived from the Fukushima Nuclear Plant accident. Journal of Business Administraion, Toyo University 77: 13-26, in Japanese. 4
  • 5. Deposition of Cs-137 and Sr-90 5 Tsukuba is 150 km away from Fukushima NPP. Until several months after the accident. PTBT = Partial Test Ban Treaty (Meteorological Research Institute, 2011) 1963: PTBT
  • 6. Yamaguchi et al. (2007) • Environmental decay factor was calculated. • CEC was correlated with environmental decay factor and transfer coefficient to wheat grain. • I didn’t believe this research would be so useful, but … 6
  • 7. Safety of 5 walls for NPP • It was believed (or explained) that radionuclide will not be emitted in the environment. 7 4: containment building 3: pressure vessel 5: concrete reactor building 1: pellet of nuclear fuel 2: zirconium alloy
  • 8. Cooling • After the accident, chain reaction was stopped safely, as expected. • The decay heat from fission products had to be cooled down. However, the cooling system was broken by earthquake and tsunami. Backup electricity was also broken by tsunami. • They poured water in nuclear reactors to cool down, but TEPCO said the water level was not rising on TV (14-15 March, 2011). I was scared … 8
  • 9. Radiation at Isobe, 100 km from Fukushima 9 I was looking at this data on time, and understood that radionuclide was actually emitted to environment, and traveled 100 km from Fukushima. http://www.houshasen-pref-ibaraki.jp/present/result01.html 100 times increase !
  • 10. 10 Kyoto, May 15, 2011 Kinkaku-ji (Temple of the Golden Pavilion)
  • 11. Explosion of 3rd reactor, 11am March 14 11 Actually it was not the only source of emission.
  • 12. Radiation contour map of Cs-134 and Cs-137 at September 2011 (Yukio Hayakawa) 12 100 km 200 km 50 km Decreased to 62 % in 2 years
  • 13. 13 Evacuation (20 km) Stay in door (20 - 30 km) Iitate
  • 14. Evacuation 14  160,000 people are evacuating (December 11, 2012, Fukushima Minpo news)  Warning region  Hard to return region > 50 mSv / year  Residence restriction region > 20 mSv / year  Preparing for termination of evacuation 20km Iitate village
  • 15. Seki (2011) • Reviewed emission of radionuclides • Reviewed soil contamination • Reviewed remediation strategies 15
  • 16. Emission of radionuclides from Fukushima Daiichi NPP Leakage to groundwater NPP Emission to air 770 PBq (1015 Bq) Water emitted 43 PBq Groundwater Sedimentation Groundwater movement Plume Air current Rain Fallout Deposit on Soil pollution Direct pollution of plant Indirect pollution of plant from root Livestock (Remote place) Ocean . (Seki, 2011) 16 (Chernobyl: 5200 PBq) Converted to iodine
  • 17. Radioisotopes 17 Radioisotope Half life I-132 2 hr Te-132 3 day I-131 8 day Sr-89 50 day Cs-134 2 year Sr-90 29 year Cs-137 30 year
  • 18. Radiocesium movement in soil • Cs-137 concentration at Lithuania 17 years after Chernobyl accident (Druteikiené et al., 2011) 0 25 50 75 // 300 Cs−137, Bq/kg 0 1 2 3 4 5 Sand Forest 18
  • 19. Cs-134 and Cs-137 profile at paddy field at Fukushima after 2 months from accident (Shiozawa et al., 2011) 19
  • 20. Soil in Fukushima Ministry of Land, Infrastructure, Transport and Tourism, Japan Mostly brown forest soil and lowland soil. Also volcanic ash soil (Andisol). 20
  • 21. Cesium adsorption on Clay particle (Yamaguchi et al., 2012) 21 Phyllosilicate (Sheet of SiO4 tetrahydra) has siloxane ditrigonal cavity similar to the size of Cs- (1) Beidellite (2) Vermiculite, illite Hydrated ions ex. Ca2+ It can swell, but when Cs- enters between sheets, it shrinks and Cs- is trapped. Frayed edge site •Takes long time to access •Once Cs- is trapped, no escape •Small ratio to whole charge •Main cause of Cs- entrapment
  • 22. RIP (Radiocesium Interception Potential) RIP Andisol has small RIP 22 (Vandebroek et al., 2009)
  • 23. Transfer coefficient (TC) • Cs-137 in agricultural product TC = ------------------------------------------ Cs-137 in soil • TC of brown rice was set as 0.1 on April 8, 2011 by MAFF (Ministry of Agriculture, Forestry and Fisheries, Japan) • MAFF published transfer coefficient of vegetables and fruits on May 27, 2011 http://www.maff.go.jp/j/press/syouan/nouan/110527.html 23
  • 24. Rice in Fukushima • Plantation of rice with soil more than 5000 Bq/kg was prohibited. Temporal regulation was 500 Bq/kg, and TC of 0.1 was assumed. • At first, most rice was below 500 Bq/kg, but some rice exceeded 500 Bq/kg. • Regulation changed to 100 Bq/kg on April 1, 2012, based on the limit of radiation exposure of 1 mSv / year. 24
  • 25. Radiocesium in soil and rice (2011) 25 (Fukushima Prefecture and MAFF, 2011) Radiocesiuminbrownrice(Bq/kg) Radiocesium in soil (Bq / kg)
  • 26. Potassium in fertilizer (2011) 26 Radiocesiuminbrownrice(Bq/kg) Exchangeable K2O concentration in soil (mg / 100g) (Fukushima Prefecture and MAFF, 2011)
  • 27. Radiocesium in soil and rice (2012) 27 (Fukushima Prefecture and MAFF, 2013) Radiocesium in soil (Bq/kg DW) Radiocesiuminbrownrice(Bq/kgFW) Much better than 2011
  • 28. Countermeasures (Seki, 2011) • Stripping of surface soil • Turn over surface soil with subsoil • Application of K fertilizer • Change to crops of low transfer coefficient • Phytoremediation • Chemical remediation 28
  • 29. 29 (Twitter @seki, March 25, 2011) Identify the contaminated area, remove soil of several cm at the surface, and discard it as radioactive waste. Does it work ?
  • 30. Stripping of surface soil • As long as radiocesium is in a few centimeters, it can be removed. • Planned for paddy field uncutivated after 2011 (> 5000 Bq/kg, ex. Iitate). Once cultivated, it is ieffective. • Depth of contamination should be examined. • Massive amount of soil as radioactive waste disposal. 30
  • 31. Radioactive waste disposal site • Final disposal site is not determined. • Not enough temporal storage site. 31 Temporal temporal storage site at Iitate village Osamu Ieda http://www.kyoten.org/top_seminar12.html
  • 32. Stabilizer of soil • Difficult to remove surface soil of paddy field. • Stabilizer with magnesium can be used before removal. • Contaminated soil can be easily identified. http://www.s.affrc.go.jp/docs/press/110914.htm 32
  • 34. Change crops • Change to crops with lower transfer coefficient. 34
  • 35. Phytoremediation • Make plant absorb contamination. • Experiment with sunflower showed that it is not very effective. • Plant should be safely disposed. • Depth of root and depth of contamination should be examined. 35
  • 36. Chemical remediation • No efficient way of chemical remediation now. • Cesium is too strongly adsorbed on clay. • Besides, concentration is less than 10000 times lower than cadmium contamination. – 100 Bq/kg of radiocesium = 0.032 ppb – 400 ppb for Cd 36
  • 37. Problem for decontamination • High cost – 100 trillion yen or more, to attain < 1mSv / year. • Final disposal site is not determined. 37
  • 38. Battle of soil scientists in Fukushima, Japan ASA, CSSA and SSSA Annual Meeting, Tampa, Florida, November 4, 2013 • Enhancing vertical transport with artificial macropore • Device to measure radiocesium concentration • Cooperation of NGO with researchers to resurrect Fukushima • Field monitoring system for sediment and radiocesium runoff • Colloid facilitated transport of radioactive cesium • Role of clay mineral in radioactive Cs transport • Recovering soil fertility after stripping • Burial experiment of soil contaminated by radiocesium • http://www.iai.ga.a.u-tokyo.ac.jp/mizo/edrp/fukushima/ASA13/ 38
  • 39. Still long way for safeguarding Fukushima • Nuclear fuel is melt down, how can we take out? We have no plan yet. • Nuclear fuels in the pool of 4th reactor are now transported to safer place. • Stop the leakage of contaminated water • Water cleanup system of ALPS (France) – until the end of 2014 • 40 years is enough? 39
  • 40. Problems • Many workers get limit radiation 100 mSv / year and cannot work any more. They work in very bad condition. • Earthquake probability is always high in Japan. If “unpredicted” accident happens again, who can do the recovery work ? • Risk for big earthquake is always large in Japan. 40
  • 41. Energy in future • In Japan, all NPP is stopped now for regular maintenance. They are waiting for safety judging. • Government still wants to promote nuke, but strong movement of anti-nuke in citizens. • We need to seek for transition to other energy sources. • How about in France ? 41
  • 42. Final remark • We are still in the process of recovering from the disaster. • This talk focused on soil contamination and remediation. I would like to contribute something in this field as a soil scientist. • France and Japan can share our knowledge and techniques for better future of our countries. 42