This short blog summarizes an open access paper published today reporting results from a Canadian monitoring program tasked with documenting the arrival of ocean borne Fukushima contamination along the North American Pacific coast. This diary is part of an ongoing effort to communicate the best science available on the impacts of the Fukushima Dai-ichi meltdowns on the environment. High quality measurements to look for Fukushima derived radiocesium were made in seawater in the North Pacific and Arctic Oceans from 2011 to early 2014. The authors concluded that:
Fukushima derived radiocesium was first detected 1500 km west of British Columbia Canada in June 2012
Contamination was detected on the continental shelf (near coastal waters) in June 2013
By February 2014 Fukushima radiocesium was present at levels similar to preexisting weapons testing derived 137-Cs
These same models predict that total radiocesium levels from weapons testing fallout and Fukushima will likely reach maximum values of ~3-5 Becquerel per cubic meter (Bq m-3 of seawater in 2015-2016 and then decline to fallout background level of ~1 Bq m-3 by 2021
Fukushima will increase northeastern Pacific water to levels last seen in the 1980’s but does not represent a threat to environmental or human health
The purpose of this post is to address an error in a recently published review of current release estimates from the Fukushima Dai-ichi nuclear power plant disaster that began in March 2011. The post is part of an ongoing effort to communicate results of scientific studies aimed at understanding the impact of Fukushima on the health of the North Pacific and residents of the west coast of North America. In a recent review paper published in Progress in Nuclear Energy by Koo and colleagues this July, compiled estimates of atmospheric and ocean releases from Fukushima were presented. Due to an error in interpretation they suggest that direct ocean releases were a factor of 4 greater than atmospheric releases of radiologically significant isotopes like 131-I (~8 day half life) and 137-Cs (~30 year half life). This error inflates release estimates and has been reported on to suggest Fukushima releases exceed Chernobyl’s. Accurate estimates of releases from Fukushima suggest that they are about an order of magnitude less than those from Chernobyl in 1986.
The study of Koo and others (link to a ResearchGate upload) estimated atmospheric releases of 131-I, 137-Cs and the noble gas 133-Xe (half life ~ 5 days) from the Fukushima Dai-ichii nuclear power plant. Their estimates compared with previously published estimates are reported in the following table (Table 2 from paper):
Similar to previous work, for example, they estimate the atmospheric release of 137-Cs from the plant to be 10-50 PBq or somewhere between 3 and 17 kg of the isotope. Given the core inventories of reactors 1-3 this release represents about 4% of the inventory at the time of the meltdowns in March 2011.
The authors make a significant error when they begin their estimate of direct releases from Fukushima to the ocean when they state the following in section 2.2.2. Release from the primary system into the sea:
It is reported that, of the total radioactivity released from the units 1–3 into the environment, more than 80% of it flowed into the sea (Hoeve and Jacobson, 2012 and Christoudias and Lelieveld, 2013), implying that 4 times more radioactivity was released to the sea than to the atmosphere.
Bolds are mine. In stating that 80% of the total radioisotope releases flowed into the sea they fundamentally misinterpret the studies they cite. What the study of Christoudias and Lelieveld (2013), and other studies not referenced here in the diary, actually show and establish is that (quoting from the Christoudias and Lelieveld work):
We calculated that about 80% of the radioactivity from Fukushima which was released to the atmosphere deposited into the Pacific Ocean.
This is a fundamentally different than the interpretation Koo and colleagues use in their study. By wrongly interpreting that atmospheric releases represent 20% of the total release they assume that direct ocean releases are 4 fold greater than the 4% of core inventories (10-50 PBq) or 16% of core inventories of 137-Cs in March 2011. This error greatly increases the estimated total releases from the plant (atmosphere + direct ocean).
It is very likely that this incorrect approach will lead others to conclude that total releases from Fukushima are greater than those from Chernobyl. For example a back of the envelope calculation assuming the 4% of the total core inventory of 137-Cs (760-820 PBq according to the table above) was released to the atmosphere and 16% to the ocean would lead to a total release of ~152-164 PBq. Such a calculation was done by a popular news aggregator and editorial site that has a history of misinterpreting and misinformation the public about Fukushima. This estimate, not surprisingly, is at great odds with existing estimates based on measurements and modeling.
Best estimates to date suggest that:
1. atmospheric releases of 137-Cs were 19.4 +- 3.0 PBq through the end of March 2011
2. direct ocean discharge of 137-Cs to the Pacific in addition to atmospheric deposition are in the range 2.3 to 26.9 PBq
3. About 19.5 +- 5% of releases were deposited to land while about 80% ended up in the Pacific Ocean
A report reviewing the most recent peer reviewed studies which reaches these conclusions was summarized in a post here.
Releases of isotopes that represent potential radiological health threats given their respective total activities and/or their significant half lives (e.g. 131-I and 137-Cs) were about an order of magnitude (factor of 10 times) lower than the releases from the Chernobyl disaster in 1986 (see reports here and here for example). More and more observations are being made globally by the international scientific community which will help to improve source term and release estimates. I will report on these studies as the data becomes available.
I have contacted the authors to bring their attention to this problem with their study.
This post is part of an ongoing series that represents an effort to communicate peer-reviewed scientific studies of the impact of the Fukushima nuclear disaster on the North Pacific Ocean and residents of the west coast of North America. A frequently asked question of those involved in monitoring the health of the North Pacific is why more measurements of the long lived, alpha-emitting isotopes of plutonium (239-Pu half-life 24,100 years; 240-Pu 6,570 years) are not being made given the potential for these isotopes to pose radiological health risks. Measurements of air, soil and water indicate that Pu was released and broadcast into the environment as a result of the triple reactor meltdowns with estimates of the source on the order of 2.3×10^9 Bq of 239,240-Pu or 580 milligrams of the isotopes. Measurements of isotope composition and activity of Pu in seawater and sediments off the coast of Japan indicate that there was no detectable change resulting from the nuclear disaster (behind pay wall). Given that the Fukushima signal is not detectable in the ocean off Japan relative to legacy sources from atmospheric weapons testing in the 20th century there is likely little information in making the same measurements in the eastern Pacific off of North America.
Members of the public are concerned about the presence of the alpha-emitting isotopes of Pu and have been asking why measuring for these elements in seawater and marine biota is not a priority of the InFORM network. The purpose of this diary is to explain why such measurements are less likely to provide information about the plume and its impacts.
A recently published paper by Bu and colleagues in the peer-reviewed Journal of Chromotography A reports the development of a new method to determine Pu isotopes in small (20 – 60 liters) samples of seawater and measurements made of these isotopes off the coast of Japan from July 2011 to January 2013 until the present. Locations where samples were collected are shown in the figure below:
For all the seawater samples analyzed by Bu and colleagues, the 239-,240-Pu activities and 240-Pu/239-Pu atom ratios where found to be 0.00043 to 0.0056 Bq m^-3 and from 0.227 to 0.284, respectively. The results are summarized in Table 4 of the paper and are shown below:
Before the Fukushima accident in March 2011, Pu isotopes were being monitored off the coast of Japan to assess the radiological impact of the nuclear plants on the marine environment. The 239-,240-Pu activities before the meltdowns were below 0.0083 Bq m^−3 and 0.022 Bq m^−3 respectively, with 240-Pu/239-Pu atom ratios between 0.173 and 0.322. These ratios represent the influence of the Pacific Proving Ground nuclear weapon test site, which was characterized by a high 240-Pu/239-Pu atom ratio (0.30–0.36). Results after the Fukushima disaster were typically in the background data range, suggesting no detectable Pu contamination from the accident in the marine environment ~30 km offshore of the Fukushima Dai-ichi reactor complex. This conclusion is consistent with findings from previous studies of Pu isotopes in marine sediments in the western North Pacific after the Fukushima accident.
Given the absence of isotopic and concentration anomalies thus far in the western Pacific resulting from the Fukushima meltdowns there is not very much information to be gained about the evolution of the contaminated seawater plume in time and space. Similarly, the impact of the Fukushima disaster on the health of marine ecosystem with respect to Pu isotopes will be difficult to quantify relative to weapons testing background levels that persist in the environment.
On the Methodology Used to Make the Measurements (If You are Interested, IYI)
The approach used by Bu and colleagues to measure Pu isotopes at such low concentrations and activities involves applying sector field high resolution inductively coupled mass spectrometry. The instrument is able to separate chemical species by their respective mass to charge ratios using a strong electromagnetic field downstream of the plasma ionization source. Great pains were taken maximize the instruments sensitivity to measure the isotopes of interest 238-U, 239-Pu, 240-Pu, and 242-Pu. To remove the seawater matrix (cations and anions that would reduce instrument sensitivity) and elements with mass to charge ratios that would interfere with Pu detection like 238-U the seawater samples were purified using ion selective resins held in columns by passing them through successive loading and elution steps. This process is summarized in the following flow diagram from the paper:
The preconcentration and sensitivity of SF-ICP-MS allows for the very low detection limits required to quantify Pu in relatively small (20 – 60 L) volumes of seawater.
In addition to the citizen scientist sampling network that is under construction the other pillar of the InFORM project is the collection of samples in the open North Pacific and Arctic Oceans. The first samples for radionuclide analyses were collected by University of Victoria undergraduate student Kathryn Purdon on the first leg of the icebreaker CCGS Sir Wilfrid Laurier’s annual operations in Canada’s far North.
The goal of our sampling program was to obtain a detailed information about the location and intensity of the Fukushima contaminated plume of seawater by collecting seawater across the northeast Pacific from Victoria to Dutch Harbor, Alaska and up through the Bering Strait in the Chukchi Sea in the Arctic Ocean.
60 litres of seawater was collected for each sample and processed to concentrate radioactive elements for subsequent detection by gamma spectometry.