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Impacts of the Fukushima Nuclear Power Plants on Marine Radioactivity

Impacts of the Fukushima Nuclear Power Plants on Marine Radioactivity

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Published by Troy Livingston
Impacts of the Fukushima Nuclear Power Plants on Marine Radioactivity
This is proof a melt-through took place in 2011.
Impacts of the Fukushima Nuclear Power Plants on Marine Radioactivity
This is proof a melt-through took place in 2011.

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Published by: Troy Livingston on Mar 10, 2013
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Published:
October 20, 2011
r
2011 American Chemical Society
9931
dx.doi.org/10.1021/es202816c
|
Environ. Sci. Technol.
2011, 45, 9931
9935
ARTICLEpubs.acs.org/est
Impacts of the Fukushima Nuclear Power Plants onMarine Radioactivity
Ken Buesseler,
 ,
* Michio Aoyama,
and Masao Fukasawa
§
 Woods Hole Oceanographic Institution, Woods Hole, Massachusetts, United States
Meteorological Research Institute, Tsukuba, 305-0052, Japan
§
 Japan Agency for Marine-Earth Science and Technology, Yokosuka, 237-0061 Japan
b
S
Supporting Information
INTRODUCTION
 As a result of the earthquake on March 11, 2011, and sub-sequent tsunami, water as high as 15 m inundated the Dai-ichinuclear power plants (NPPs) causing loss of power and hencedisruption of controls and failed cooling systems shortly after theearthquake.Ventingofgases,hydrogenexplosions,andthe
reinthespentfuelpondofUnit4resultedintheprimaryatmosphericreleases of Fukushima radionuclide contaminants, peakingaround March 15, with a relatively high atmospheric release ratethrough March 24.
2
In addition to these atmospheric falloutpathways, the cooling of the reactors with fresh water andseawater, and release of highly contaminated water from thedamaged reactor buildings led to radioactive discharges directly to the sea. Some of this was intentional (to leave space for morehighly contaminated waters); some was unconstrained and likely resulted from contaminated groundwater discharges as well asdirect runo
ff 
to the sea. Unlike Chernobyl, there was no largeexplosive release of core reactor material, so most of the isotopesreported to have spread thus far via atmospheric fallout areprimarily the radioactive gases plus
ssion products such ascesium, which are volatilized at the high temperatures in thereactor core, or during explosions and
res. However, somenonvolatile activation products and fuel rod materials may have beenreleasedwhenthecorrosivebrinesandacidicwatersusedtocool the reactors interacted with the ruptured fuel rods, carryingradioactive materials into the ground and ocean. The fullmagnitude of the release has not been well documented, nor isthere data on many of the possible isotopes released, but we dohave signi
cant information on the concentration of severalisotopes of Cs and I in the ocean near the release point whichhave been publically available since shortly after the accidentstarted.
DATA SOURCES
 We present a comparison of selected data made publicly available from a Japanese company and agencies and comparethese to prior published radionuclide concentrations in theoceans. The primary sources included TEPCO (Tokyo ElectricPower Company), which reported data in regular press releases
3
and are compiled here (Supporting Information Table S1). TheseTEPCO data were obtained by initially sampling 500 mL surfaceocean water from shore and direct counting on high-purity germanium gamma detectors for 15 min at laboratories at the
Received:
August 12, 2011
 Accepted:
October 20, 2011
Revised:
October 19, 2011
 ABSTRACT:
The impacts on the ocean of releases of radionuclidesfrom the Fukushima Dai-ichi nuclear power plants remain unclear.However, information has been made public regarding the concentra-tions of radioactive isotopes of iodine and cesium in ocean water nearthe discharge point. These data allow us to draw some basic conclu-sions about the relative levels of radionuclides released which can becompared to prior ocean studies and be used to address doseconsequences as discussed by Garnier-Laplace et al. in this journal.
1
The data show peak ocean discharges in early April, one month afterthe earthquake and a factor of 1000 decrease in the month following.Interestingly,theconcentrationsthroughtheendofJulyremainhigherthan expected implying continued releases from the reactors or othercontaminated sources, such as groundwater or coastal sediments. By  July, levels of 
137
Cs are still more than 10000 times higher than levels measured in 2010 in the coastal waters o
ff 
Japan. Althoughsome radionuclides are signi
cantly elevated, dose calculations suggest minimal impact on marine biota or humans due to directexposure in surrounding ocean waters, though considerations for biological uptake and consumption of seafood are discussed andfurther study is warranted.
 
9932
dx.doi.org/10.1021/es202816c |
Environ. Sci. Technol.
2011, 45,
9931–9935
Environmental Science & Technology
ARTICLE
Fukushima Dai-ni NPPs. They reported initially results for
131
I (
1/2
= 8.02 days),
134
Cs (
1/2
= 2.065 years) and
137
Cs(
1/2
= 30.07 years). Data from MEXT (Ministry of Education,Culture, Sports, Science and Technology 
 Japan) were alsoreleased on a public Web site
4
and are based on similar directcounting methods. In general MEXT data were obtained by sampling 2000 mL seawater and direct counting on high-purity germanium gamma detectors for 1 h in a 2 L Marinelli beaker atlaboratories in the Japan Atomic Energy Agency. The detectionlimit of 
137
Cs measurements are about 20000 Bq m
À
3
forTEPCO data and 10000 Bq m
À
3
for MEXT data, respectively.These measurements were conducted based on a guidelinedescribed by MEXT.
5
Both sources are considered reliable giventhe common activity ratios and prior studies and expertiseevident by several Japanese groups involved in making thesemeasurements. The purpose of these early monitoring activities was out of concern for immediate health e
ff 
ects, and thus wereoften reported relative to statutory limits adopted by Japaneseauthorities, and thus not in concentration units (reported asscaling factors above
normal
). Here we convert values from both sources to radionuclide activity units common to priorocean studies of fallout in the ocean (Bq m
À
3
) for ease of comparison to previously published data.
RESULTS AND DISCUSSION
 We focus on the most complete time-series records from thenorth and south discharge channels at the Dai-ichi NPPs, andtwo sites to the south that were not considered sources, namely the north Discharge channels at the Dai-ni NPPs about 10 km tothesouthandIwasawabeachwhichis16kmsouthoftheDai-ichiNPPs (Figure 1). The levels at the discharge point are exceed-ingly high, with a peak 
137
Cs 68 million Bq m
À
3
on April 6(Figure 2). What are signi
cant are not just the elevatedconcentrations, but the timing of peak release approximately one month after to the earthquake. This delayed release ispresumably due to the complicated pattern of discharge of seawater and fresh water used to cool the reactors and spentfuel rods, interactions with groundwater, and intentional andunintentional releases of mixed radioactive material from thereactor facility.During the
rst month of release data,
134
Cs/
137
Cs activity ratios were one (0.99
(
0.03 for Dai-ichi north and southdischarge channels) and extremely uniform (Supporting Infor-mation Figure S1). This makes the tracking of Fukushimaderived radionuclides in the ocean quite straightforward, sincegivenitsrelativelyshort2yearhalf-life,theonlysourceof 
134
Csinthe North Paci
c at this time would be the Dai-ichi NPPs. Hencein addition to the elevated Cs activities, the presence of 
134
Cs is aunique isotopic signature for tracking these waters and calculat-ing mixing ratios. This ratio of Cs isotopes is determined by reactor design and fuel cycle and age. Interestingly a
134
Cs/
137
Csratio of 1.0 here is considerably higher than 25 years ago when aratio of 0.54
(
0.04 was reported in Chernobyl fallout.
6
In theoceans,thebehaviorofcesiumisthoughttobeconservative,i.e.itis soluble (<1% attached to marine particles) and is carriedprimarily with ocean waters and as such has been used as a tracerof water mass mixing and transport.
7
À
9
That being said, even asmall fraction at such a high activity release point is a largenumber, thus the concentrations of Cs in sediments and biotanear the NPPs may be quite large, and will continue to remainso for at least 30
À
100 years due to the longer half-life of 
Figure 1.
Map of Fukushima sampling locations at the Dai-ichi NPP(1F- yellow dot as indicated). Red dots N and S of the Dai-ichi NPP aredischarge channels where samples were collected. Samples were alsocollected by TEPCO at the Dai-ni NPP (2F- yellow dot as indicated) withsamplingindicatedfromshorenearDai-niNPPandIwasawaBeach(blue triangles). Also shown are sampling locations by MEXT 30 kmo
ff 
shore (green squares). For scale, 30 km radius around Fukushima isshown on land. More detailed sampling maps available at TEPCO andMEXT Web sites.
3,4
Figure 2.
Surface ocean concentrations from March 21 to July 31, 2011of 
137
Cs in Becquerels per cubic meter (Bq m
À
3
) for two sites near theFukushima Dai-ichi nuclear power plant (red circles, north (
lled) andsouth (open) discharge channels
3
), Dai-ni NPPs (10 km to the south of Dai-ichi, blue
lled triangles
3
), Iwasawa Beach near Dai-ni (16 km southof Dai-ichi, blue open triangles
3
), and 30km o
ff 
-shore (green squares,stations1
À
8inoriginalMEXTdata
4
).Thesearecomparedonthelower
 X 
-axis(1960
À
2010)tothehistoricalrecordof 
137
Cso
ff 
theeastcoastof  Japan(browncircles) andtoChernobyl in
uencedwatersin1986 intheBaltic and Black Seas.
13,14
 
9933
dx.doi.org/10.1021/es202816c |
Environ. Sci. Technol.
2011, 45,
9931–9935
Environmental Science & Technology
ARTICLE
137
Cs which is still detected in marine and lake sediments from1960s fallout sources.There was considerable attention given to
131
I releases due toits relatively high activities and tendency to accumulate in thehuman thyroid if ingested via land-based food supply orif bioconcentrated by seaweeds and consumed as part of the Japanese diet. We can see that the ocean release ratio of 
131
I/
134
Cs must have been relatively constant, with the highestmeasured activity ratios near 20
À
30 on March 22 followed by apredictabledecreaseduetotheradioactivedecayof 
131
Iwithits8day half-life (which would plot as straight line in Figure 3). Assuming the source ratios of Cs and I were
 xed when the
ssion process stopped on March 13, the initial source ratio would have been a factor of 2 higher. Reported atmospheric
131
I/
137
Cs ratios showed somewhat higher variability early in thereleases, ranging from around 10
À
80 during the period of maxi-mum atmospheric release between March 15 and 24
2
. Some of the ocean data fall o
ff 
of this ocean decay trend, indicatingperhapsdi
ff 
erentsources(e.g.,highervaluesaroundApril19
À
23at Dai-ichi NPPs, Figure 3), but the general consistency of thisdecay pattern in waters both at Dai-ichi NPPs and further southindicates that overall the I and Cs sources can be considereduniform even if several reactors and events contributed to thereleases.Ocean currents o
ff 
Japan would lead to both southwardtransport of water along the coast via the Oyashio current, andnorthward driven diversions due to surface wind shifts.
10,11
Clearly the waters 10 km south along the shore at the Dai-niNPPs were initially lower in overall activity, but rapidly reachedactivities more similar to the source at Dai-ichi. Coastal waterconcentrations decreased by close to a factor of 1000 in themonth following peak releases (Figure 2). This is a consequenceof ocean mixing and a primary radionuclide source that hasdramatically abated. Unlike contamination of soils on land, vertical and horizontal mixing rates in the ocean are fast, dilutingthe primary contaminant signal quite rapidly, particularly in theenergetic coastal waters o
ff 
Japan where the Oyashio watersmove south and interact with the rapidly 
owing and o
ff 
shoremeandering of the Kuroshio Current. These currents, tidalforces, and eddies mix the waters quite rapidly o
ff 
shore. Suchphysicaltransportandmixingprocessescanbemodeled,butthusfar there are no published models that include Fukushima oceandata for comparison (see for example Fukushima fallout predic-tions in ref 12).Sampling immediately o
ff 
shore was sponsored by MEXT in Japan, and we have summarized here the
rst month
s data ateightstationsalongatransect30kmo
ff 
shorefromtheFukushimaNPPs (along 141
°
24
0
E. Longitude between 37
°
00
0
and 37
°
40
0
N Latitude; Figure 1). From the
rst measurements onMarch 22 until about March 28, activities decreased. Thisdecrease can be explained if the initial data re
ect elevated
137
CsfromdirectFukushimafalloutdepositionearlierinMarch,
2
followed by dilution. The waters 30 km o
ff 
shore increased afterMarch 28 in parallel with the coastal waters at Dai-ni. Theo
ff 
shore waters have roughly 1000 times lower activities duringthe period of peak discharge in early April and remain at least10timeslowerlaterinApril.ThegridsampledbyMEXTexpandedconsiderably in April to include additional stations between thecoast and 30 km, but after about April 20, the reported MEXTdata fall largely below their minimum detectable limit, which was10000 Bq m
À
3
for
137
Cs.If the source at Fukushima had stopped abruptly and oceanmixing processes continued at the same rates, one would haveexpected that the
137
Cs activities would have decreased anadditional factor of 1000 from May to June but that was notobserved. The break in slope in early May implies that a steady,albeit lower, sourceof 
137
Cs continues to discharge to the oceansat least through the end of July at this site. With reports of highly contaminated cooling waters at the NPPs and complete meltthroughofatleastoneofthereactors,thisisnotsurprising.Aswehave no reason to expect a change in mixing rates of the ocean whichwouldalso impact this dilution rate, this change inslope of 
137
Cs in early May is clear evidence that the Dai-ichi NPPsremainasigni
cantsourceofcontaminationtothecoastalwaterso
ff 
Japan. There is currently no data that allow us to distinguish between several possible sources of continued releases, but thesemost likely include some combination of direct releases from thereactors or storage tanks, or indirect releases from groundwater beneaththereactorsorcoastalsediments,bothofwhicharelikely contaminated from the period of maximum releases.Itisprudenttopointoutthoughwhatismeantby 
signi
cant
to both ocean waters and marine biota. With respect to priorconcentrations in the waters o
ff 
Japan, all of these values areelevated many orders of magnitude.
137
Cs has been tracked quiteextensively o
ff 
Japan since the peak weapons testing fallout yearsin the early 1960s.
13
Levels in the region east of Japan havedecreased from a few 10s of Bq m
À
3
in 1960 to 1.5 Bq m
À
3
onaverage in 2010 (Figure 2; second
x
-axis). The decrease in
137
Csover this 50 year record re
ects both radioactive decay of 
137
Cs with a 30 year half-life and continued mixing in the global oceanof 
137
Cs to depth. These data are characteristic of other global water masses.
14
Typical ocean surface
137
Cs activities range from<1 Bq m
À
3
in surface waters in the Southern Hemisphere, whichare lower due to lower weapons testing inputs south of the
Figure 3.
Activity ratio of 
131
I/
137
Cs at the same four sites at Dai-ichi,Dai-ni and Iwasawa Beach as in Figure 2 plotted on a log activity ratio(
 y
-axis) vs time through May 30 (
x
-axis). Solid blackline is the decay trendexpected for the activity of an isotope with 8 day half-life such as
131
I.

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