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Journal of NUCLEAR SCIENCE and TECHNOLOGY, Vol. 48, No. 7, p.

1129–1134 (2011)

RAPID COMMUNICATION Fukushima NPP Accident Related

Preliminary Estimation of Release Amounts of 131 I and 137 Cs Accidentally


Discharged from the Fukushima Daiichi Nuclear Power Plant
into the Atmosphere
Masamichi CHINO1; , Hiromasa NAKAYAMA1 , Haruyasu NAGAI1 ,
Hiroaki TERADA1 , Genki KATATA1 and Hiromi YAMAZAWA2
1
Japan Atomic Energy Agency, 2-4 Shirane, Shirakata, Tokai-mura, Naka-gun, Ibaraki 319-1195, Japan
2
Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Japan
(Received April 27, 2011 and accepted in revised form May 2, 2011)

KEYWORDS: Release amounts, 131 I, 137 Cs, atmosphere, Fukushima Daiichi nuclear power plant,
accident, monitoring data, air concentrations, atmospheric dispersion simulation, SPEEDI,
WSPEEDI-II

I. Introduction ing unit release rate (1 Bq h1 ). Release rates are obtained by
dividing measured air concentrations of 131 I and 137 Cs into
The Fukushima Daiichi nuclear power plant accident in calculated ones at sampling points as follows:
Japan triggered by a magnitude 9.0 earthquake and resulting
Qi ¼ Mi =Ci ; ð1Þ
tsunami on March 11, 2011 caused the month-long discharge
of radioactive materials into the atmosphere. It is urgent to where Qi is the release rate (Bq h1 ) of nuclide i when
assess the radiological dose to the public resulting from this discharged into the atmosphere, Mi the measured air con-
release, using both environmental monitoring data and com- centration (Bq m3 ) of nuclide i, and Ci the dilution
puter simulation based on atmospheric dispersion modeling factor (h m3 ) of nuclide i, which is equal to the air con-
of radioactive materials. However, the source term essential centration calculated under the assumption of unit release
to computer simulations, e.g., nuclides, release rates, and rate.
duration, was not available, although it was expected to be Even when air concentration data are not available, the
provided from a stack monitor and/or a reactor behavior release rates can also be estimated by comparing measured
analysis. Thus, in cooperation with the Nuclear Safety air dose rates due to radionuclides in plume and/or on the
Commission of Japan (NSC), the Japan Atomic Energy ground surface with calculated ones derived from simula-
Agency (JAEA) has been trying to estimate the source term tions with unit release rate, assuming the composition of
of iodine and cesium discharged from the Fukushima Daiichi iodine and cesium.
nuclear power plant into the atmosphere. The method ap- Total release amounts are estimated by the time integra-
plied in this estimation is a reverse estimation of source term tion of release rates as follows:
by coupling environmental monitoring data with atmos- X
Si ¼ ½Qi; j  Tj ; ð2Þ
pheric dispersion simulations under the assumption of unit
release rate (1 Bq h1 ). The authors have already applied this where Si is the total release amount (Bq) of nuclide i, Qi; j the
method to the Chernobyl accident,1) JCO accident,2) and release rate (Bq h1 ) of nuclide i at time j, the duration of
other incidents, and have considerable experience. This which is Tj (h).
paper estimated the release rates and total amounts of 131 I
and 137 Cs discharged into the atmosphere from March 12 to 1. Environmental Monitoring Data
April 5, 2011. For the source term estimation, environmental monitoring
data on air concentrations of iodine and cesium (hereafter,
dust sampling data) were mainly used. Gaseous and partic-
II. Reverse Estimation Method
ulate forms of iodine were expected to be sampled according
The reverse estimation method calculates the release rates to the guideline for environmental radiation monitoring from
of radionuclides (Bq h1 ) by coupling environmental mon- NSC,3) which recommends the use of dust samplers with
itoring data with atmospheric dispersion simulations, assum- charcoal cartridge for gaseous iodine. The data used in the
estimation are from the web sites of the Ministry of Educa-

tion, Culture, Sports, Science and Technology (MEXT),4)
Corresponding author, E-mail: chino.masamichi@jaea.go.jp the Japan Chemical Analysis Center (JCAC),5) and JAEA.
Ó 2011 Atomic Energy Society of Japan, All Rights Reserved.
1129
1130 M. CHINO et al.

Data No. Sampling date and time Sampling point


1 2011/3/15 06:00-07:00 a
2 2011/3/15 06:55-07:15 b
3 2011/3/16 06:05-06:25 b
i f 4 2011/3/18 10:50-11:18 c
g
j 5 2011/3/21 04:45-05:05 b
d h 6 2011/3/21 10:50-11:08 d
7 2011/3/22 14:17-14:31 c
c,e*
8 2011/3/23 13:15-15:10 e
Tokai-mura 9 2011/3/24 14:55-15:15 f
10 2011/3/25 15:05-15:22 g
b 11 2011/3/27 11:45- h
12 2011/3/29 11:17-12:15 f
13 2011/3/30 15:11-15:32 g
Chiba-city
14 2011/3/31 12:22-13:12 e
a 15 2011/4/1 12:00-12:20 i
16 2011/4/3 11:04- j
17 2011/4/5 13:07-13:27 f
*Points c and e are almost overlapped.

Fig. 1 Dust sampling points and sampling periods (in JST) used for estimating the release rates. The symbol (1F)
indicates the Fukushima Daiichi nuclear power plant and the square by a dotted line is SPEEDI’s calculation domain.

Figure 1 shows the locations of the dust sampling and sam- 3. Comparison of Measurement with Calculation
pling period, which are thought to capture plumes. Note that (1) Dust Sampling Data
the Japanese Standard Time (JST ¼ UTC þ 9 h) is used in Two types of dust sampling data, e.g., time trend data
this paper. from short-time samplings and time-integrated data, were
Air dose monitoring data from MEXT indicate that the available. Sampling data of each type were compared with
atmospheric release of radionuclides in the daytime of atmospheric dispersion simulation results as follows:
March 15 caused a large amount of ground deposition and  For the time trend data, peak values from both measure-
resulting high dose rates in the sector to the northwest of the ment and calculation were adopted to Eq. (1). An example of
plant. However, because no dust monitoring data were avail- the comparison at JAEA, Tokai-mura is shown in Fig. 2.
able in the daytime of March 15, the release rates of 131 I and Concentration peaks of measurement and calculation ap-
137
Cs in this period were estimated from the comparison of peared at around 7–9 JST on March 15.
measured air dose rate pattern due to ground shine with  For time-integrated data, calculated air concentrations
the calculated one, after the plume moved away from this averaged for the sampling period were adopted to Eq. (1).
region. Although the simulation results were generally in good
agreement with the measured concentrations as shown in
2. Atmospheric Dispersion Simulation Fig. 2, there were slight discrepancies in arrival time and
The System for Prediction of Environmental Emergency location of plume. In addition, the measured dust sampling
Dose Information (SPEEDI) network system6) operated by data were far insufficiently available in time and space to
MEXT was used for calculating air concentrations and dose precisely locate plumes. To cope with these limitations in
rates. The simulation results were furnished from NSC for the urgent situation, the following simplified methods were
the purpose of the source term estimation. In addition, to used.
utilize dust sampling data obtained beyond SPEEDI’s cal-  If multiple concentration data were available from differ-
culation domain as points a (Chiba City) and b (Tokai-mura) ent locations for a time, only a maximum value was adopted
in Fig. 1, Worldwide version of SPEEDI (WSPEEDI-II)7) to characterize the plume of the time to avoid errors caused
developed by JAEA was also used. by data obtained at edges of the plume.
Atmospheric dispersions of radionuclides were simulated  Discrepancies in arrival time and plume location were
by successive uses of the meteorological prediction model subjectively adjusted by comparing patterns.
PHYSIC and the atmospheric dispersion model PRWDA21 (2) Air Dose Rate Data
in SPEEDI, and MM5 and GEARN in WSPEEDI-II. One of the major releases occurred on March 15.
Because detailed descriptions of these models are given According to the atmospheric dispersion simulation by
in the literature,8,9) only an outline of the models and the SPEEDI, the plume of high concentration moved to the
computational conditions are summarized in Table 1. northwest direction, caused high-level deposition there by

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY


Preliminary Estimation of Release Amounts of 131 I and 137 Cs Accidentally Discharged from the Fukushima NPP 1131

Table 1 Summary of atmospheric dispersion simulation by SPEEDI and WSPEEDI-II

SPEEDI WSPEEDI-II
a)
Meteorological data GPV (GSM-Japan) by the Japan Meteorological Agency
(3-hourly and 0:25 deg.  0:2 deg. resolution)
Topographical data Digital National Land Global 2-min. resolution data
Information by Geospatial by the U.S. Geological Survey
Information Authority of Japan
Computational grid 100  100  30 130  190  30
(2-km horizontal resolution) (3-km horizontal resolution)
Computational domain 100 km  100 km  4 km area 390 km  570 km  10 km area
including the east side of including the Tohoku and
Fukushima Pref. Kanto regions
Meteorological PHYSIC: Atmospheric dynamic MM5b) : Atmospheric dynamic
prediction model model by JAEA model
Atmospheric dispersion PRWDA21: Lagrangian particle GEARN: Lagrangian particle
model random-walk model by JAEA random-walk model by JAEA
a)
GPV: Grid Point Value
b)
Atmospheric dynamic model by Pennsylvania State University and the National Center for Atmospheric Research (NCAR)

precipitation, then moved back to the Pacific Ocean on


March 16. This specific event brought the lasting air dose
rate due to ground shine. Thus, to estimate the release rates
of 131 I and 137 Cs on March 15, the air dose rates due to
ground shine from measurement and calculation on March
17 were compared. The calculation assumed the radioactiv-
ity ratio of 131 I:132 I:134 Cs:137 Cs to be 1:1:0.1:0.1 based on the
concentration measurements of iodine and cesium in rain,
snow, and vegetations in the area.4) This assumption may
result in an overestimation of release rates of the above-
mentioned nuclides because the contributions from other
short-lived nuclides are not taken into account in the calcu-
lation. The precipitations in the simulation were inter- and
extrapolated from observation data, e.g., the precipitations
of 0.5–1.5 mm/h were observed in the evening of March 15
to the morning of 16 at Iitate-mura in the area. Figure 3
depicts the air dose rate distribution from SPEEDI and
measurement. This figure indicates that SPEEDI reproduces
the spatial dose pattern well and, by multiplying 1016 to
contour values, the absolute values of calculation become
similar to the measurement. It is noted that the estimation
of release rates from air dose rates could not be used except
for March 15, because, before March 15, no large amount
of deposition appeared and the uncertainty caused by the
existence of short-lived nuclides may become serious. It is
also one of the reasons that, after March 15, the background
values of air dose rate became too high to distinguish addi-
tional air dose rates.

III. Results
The estimation result of release rates of 131 I is summarized
Fig. 2 Comparison of temporal variation of air concentration of in Table 2. The ‘Released time of sampled air’ is deter-
131
I between measurement and calculation at JAEA, Tokai-mura mined reversely from the sampling period, considering
(above), and wind and air concentration distributions at the the calculated movement of continuously released plume,
ground level at 7 JST on March 15 (below) observed wind speeds, and discrepancy of arrival time of

VOL. 48, NO. 7, JULY 2011


1132 M. CHINO et al.

16 The Fukushima
20 Daiichi nuclear
15 power plant
88
39 165
Measurements [µGy/h]
60
> 100
50 - 100
10 - 50
< 10

Calculation [µGy/h]
1 × 10 -14
5 × 10 -15
1 × 10 -15
The Pacific Ocean

Fig. 3 Comparison of air dose rate between measurement and calculation in the northwest area of the plant on March 17

131 131
Table 2 Preliminary estimated release rates of I, radioactivity ratio of I/137 Cs, and duration times

Dust sampling data Calculations Release rate 131 Released time


I/137 Cs Duration
No. [Bq m3 ] [Bq m3 ] [Bq h1 ] of sampled air
1 6.8 3:0  1013 2:3  1013 10 3/14 21:00 3/12 10 to 3/14 23
2 2,800 8:0  1012 3:5  1014 8.8 3/15 1:00 3/14 23 to 3/15 09
— Estimated from air dose rate 1:0  1016 10 3/15 13:00 3/15 09 to 3/15 15
3 830 4:0  1012 2:1  1014 70 3/16 4:00 3/15 15 to 3/17 06
4 33 8:0  1014 4:1  1014 41b) 3/18 8:00 3/17 06 to 3/19 15
5 1,900 5:0  1012 3:8  1014 11 3/20 22:00 3/19 15 to 3/21 03
6 1,420 1:0  1011 1:4  1014 131c) 3/21 8:00 3/21 03 to 3/21 21
7 410 1:0  1012 4:1  1014 87c) 3/22 9:00 3/21 21 to 3/22 23
8 355a) 5:0  1013 7:1  1014 80 3/23 12:00 3/22 23 to 3/24 00
9 193 1:0  1012 1:9  1014 66 3/24 12:00 3/24 00 to 3/25 00
10 555 1:0  1011 5:6  1013 45 3/25 12:00 3/25 00 to 3/26 11
11 20 5:0  1012 4:0  1012 23 3/27 9:00 3/26 11 to 3/28 10
12 75 1:0  1011 7:5  1012 1.6 3/29 10:30 3/28 10 to 3/30 00
13 180 1:0  1012 1:8  1014 1.3 3/30 14:00 3/30 00 to 3/31 00
14 24 1:0  1012 2:4  1013 5.3 3/31 9:30 3/31 00 to 3/31 22
15 1.78 1:0  1012 1:8  1012 1.1 4/1 9:30 3/31 22 to 4/02 09
16 8.84 5:0  1012 1:8  1012 3.1 4/3 8:00 4/02 09 to 4/04 09
17 6.99 1:0  1011 7:0  1011 4.9 4/5 10:00 4/04 09 to 4/06 00
a)
Two hourly data, 530 and 180 Bq m3 , were averaged.
b)
Interpolated from the ratios of Nos. 3 and 5 because only 131 I was measured.
c)
Applied the 131 I/137 Cs ratio measured at other points because only 131 I was measured.

plume between measurement and calculation. To estimate the period from about 12 to 15 JST on March 15 flowed
the total amounts of 131 I and 137 Cs discharged into the northwestward and resulted in the high dose rates due to wet
atmosphere, the ‘Duration’ is roughly estimated by assuming deposition in the nighttime of the day. However, it does not
that the release with a certain release rate continued from/to mean that the release with the release rate of 1016 Bq h1 of
131
the middle times between released times of sampled air. I started from 12 JST. It is because, even if the release
Here, the release rate firstly estimated is assumed to continue continued from the morning, the plume discharged in the
from the occurrence of release from Unit 1 due to the morning did not encounter the precipitations in the northwest
accident, 10 JST on March 12 to 23 JST on March 14. area of the plant due to the difference in wind directions and
Concerning the duration for the release rate of 1016 Bq h1 left no environmental data effective to the source term esti-
of 131 I in the daytime of March 15, which is critical to mation. There is not clear evidence to determine the release
the total release amounts, several trial simulations of atmos- starting time but an explosive sound around the suppression
pheric dispersion were carried out with various release chamber of Unit 2 of the plant at 6:10 JST was reported,
durations. They indicated that the plume released during and the dose rates measured at the main gate of the plant

JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY


Preliminary Estimation of Release Amounts of 131 I and 137 Cs Accidentally Discharged from the Fukushima NPP 1133

131 137 131


Fig. 4 Preliminary estimated temporal variation of release rates of I and Cs. Lateral bars on plots for I show
estimated release durations.

extremely increased from 9 JST. Thus, we estimated con- additional releases due to the hydrogen explosions might
servatively that a 6-hour release from 9 to 15 JST with the have taken place. The significant increase to 1016 Bq h1 of
release rate of 1016 Bq h1 of 131 I occurred. 131
I was probably caused by the damage of the suppression
Figure 4 shows the temporal variation in release rates of chamber of Unit 2 on March 15. From March 16 to 24, the
131
I and 137 Cs shown in Table 2, where the release rates of release rates of 131 I were on the order of 1014 Bq h1 and,
137
Cs are derived based on the radioactivity ratios of 131 I to after March 24, declined to the order of 1011 –1012 Bq h1 in
137
Cs from dust sampling data. In Fig. 4, the 18 plots with the beginning of April. This trend implies that, after March
lateral bars are the release rates and durations estimated from 24, the damaged reactors became stable and the atmospheric
the 17 dust sampling data and one air dose rate distribution. release of radioactive materials was reduced.
Some periods without data mean that the dust sampling
missed to capture plumes. When several dust sampling data 2. Further Tasks
are available for the estimation in the same day, the highest The uncertainty of estimated release rates is mainly
release rate in the day is plotted. The temporal variation caused by the accuracy of atmospheric dispersion calcula-
indicates that the significant release, 1016 Bq h1 of 131 I, tions and the limited coverage of monitoring in time and
occurred on March 15, following relatively small releases, space. Although the discrepancies of the distribution patterns
1013 –1014 Bq h1 , but the release rates from March 16 were and arrival times of calculated plumes to the observations
estimated to be rather constant on the order of 1014 Bq h1 were simply adjusted, the estimated release rates are consid-
until March 24. The release rates have decreased with small ered to still have the error of at least factor 5. For the
day-to-day variations to the order of 1011 –1012 Bq h1 of estimation of the total amount of nuclides discharged into
131
I in the beginning of April. The release rate of 137 Cs the atmosphere, the release rates for the periods when no
had a similar trend with fluctuations of the 131 I/137 Cs ratio dust sampling data were available are inter- or extrapolated.
in the range from 1 to 100. This may cause uncertainty that cannot be assessed from the
According to Eq. (2), the total amounts of 131 I and 137 Cs presently available data. In particular, the instantaneous ad-
discharged into the atmosphere from 10 JST on March 12 to ditional releases from March 12 to 14 may have possibly
0 JST on April 6 are estimated to be approximately 1:5  happened, but there was no trace in the environment, which
1017 and 1:3  1016 Bq, respectively. could be used for the estimation of the source term.
On April 12, 2011, the Nuclear Safety Commission of It is a preliminary assessment and the uncertainty is still
Japan disclosed that the total amounts of 131 I and 137 Cs large. To estimate the total amount of release accurately,
discharged into the atmosphere in the same period were further investigation of environmental data and technical
1:5  1017 and 1:2  1016 Bq, respectively, as preliminary evaluation are required by specialists from the reactor analy-
values10) based on our research. The slight difference in the sis and environmental fields.
total amount of 137 Cs from this paper is due to the revision of
the composition of iodine to cesium based on additional
Acknowledgements
environmental data.
The authors wish to thank the members of the Nuclear
Safety Commission of Japan for their invaluable advices, the
IV. Discussion
Ministry of Education, Culture, Sports, Science and Tech-
1. Comparison with Plant Events nology and the Nuclear Safety Technology Center for the
Because the estimation is based on the environmental contributions associated with SPEEDI operations.
monitoring, the temporal variation of estimated release rates
reflects all the releases from the damaged reactors and pos-
sible releases from the spent fuel in the pools. The release References
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probably corresponds to the wetwell venting at Units 1 and SPEEDI System to the Chernobyl Reactor Accident, JAERI-M
3 before March 14. As mentioned before, instantaneous 86-142, Japan Atomic Energy Research Institute (JAERI)

VOL. 48, NO. 7, JULY 2011


1134 M. CHINO et al.

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