Fukushima

Tracking the Fallout and Fate of Fukushima Iodine-129 in Rain and Groundwater

Matt Herod December 21, 2015

A recently published paper (by myself and colleagues from uOttawa and Environment Canada) investigates the environmental fate of the long lived radioisotope of iodine, 129I, which was released by the Fukushima-Daichii Nuclear Accident (FDNA). Within 6 days of the FDNA 129I concentrations in Vancouver precipitation increased 5-15 times above pre-Fukushima concentrations and then rapidly returned to background. The concentrations of 129I reached were never remotely close to being dangerous, however they were sufficient to distinguish the impact of the FDNA on the region.

Subsequent sampling of groundwater revealed slight increases in 129I concentration that were coincident with the expected recharge times. This suggests that a small fraction of the FDNA-derived 129I may have been transported into local groundwater after infiltrating through soils.

Sample map showing location of all three precipitation sampling locations as well as the location of both wells used for groundwater sampling. The surface expression of the Abbotsford-Sumas Aquifer is shaded.

What is iodine-129 and where does it come from?

Iodine-129 is the longest lived isotope of iodine with a half-life of 15.7 million years. It is radioactive and occurs everywhere throughout the environment. It is produced in three ways. The first two are natural and the third is by the nuclear industry.

The natural production of 129I occurs in the atmosphere and in soil/rocks. The atmospheric production happens when a cosmic ray proton hits a xenon-129 nucleus and removes a neutron, replacing it and creating an iodine-129 nucleus. The production in soil and rocks happens when a uranium-238 nucleus spontaneously fissions and one of the halves it releases has a mass of 129 ala, iodine-129.

The anthropogenic production occurs because when uranium fissions in a nuclear reactor sometimes one of the parts is 129I. This anthropogenic production is by far the largest source in the environment as substantial amounts have been released by nuclear fuel reprocessing. This 129I that has been released can trace a host of environmental processes and inform us about what happens to 129I or the much more dangerous, 131I. The current levels of 129I are much too low to pose a health threat to humans or the environment, but do allow 129I to be used as an environmental tracer.

129I from Fukushima is present in Vancouver, B.C. rain

The purpose of this research was to discover the fate of 129I in the released by Fukushima, which although a small amount, was isolated in time and space. We measured the 129I deposition in rain and its subsequent movement though soils and see if it reached groundwater. The results tell us about the impact of Fukushima, how 129I moves, where it is attenuated, and how quickly contaminants in this aquifer move from the ground surface to the water table. This knowledge can then be applied to understand 129I behavior in other settings such as nuclear waste repositories and watersheds or it can be used to learn about the behavior of other types of contaminant in this aquifer and how vulnerable it is to contamination.

The results in rain show an increase in 129I concentrations of up to 220 million atoms/L*. This increase was seen ~6-10 days after the emission from Fukushima began and are 5-15 times higher than rain samples collected before Fukushima. Following this increase 129I concentrations returned to background with a few weeks. This agrees with other studies monitoring the fallout of Fukushima derived radioisotopes [Wetherbee et al., 2012]. Furthermore, atmospheric back trajectory modelling shows trajectories for air parcels arriving in Vancouver from over the Pacific ocean and Japan.

Variation in the concentration of 129I and the 129I/127I ratio in precipitation from Vancouver, Saturna Island and NADP site WA19 over time. The time range that each NADP sample integrates is displayed using horizontal error bars. 1σ error is contained within data points if not visible. The dashed vertical line shows the date of the FDNA relative to samples.

We also calculated the mass flux of 129I from Fukushima. That is the actual quantity of 129I that was deposited on the region in grams, or in this case in atoms/m2. This was calculated by simply multiplying the concentration of 129I in rain by the amount of rain that fell. We found that only about 15% of the annual 129I deposition in the Vancouver region could be directly linked to Fukushima affected rain events. The total mass deposited by Fukushima was ~0.0000000000002 (2 x 10^-13) grams. This is a negligibly small quantity with respect to radioactive risk.

Despite the fact that the deposition of 129I from Fukushima was infinitesimally small it was still measurable. Therefore, the question became where did it go and can we learn about local groundwater resources using 129I as a tracer?

129I variation in groundwater may be due to Fukushima

The results in groundwater show very small 129I concentration increases. Two different wells were sampled. The first had a recharge time, which is the time it takes for water to move from the water table to the well screen, where it is sampled, of 0.9 years and the second had a recharge time of 1.2 years [Wassenaar et al., 2006]. The exact time it takes for water and dissolved contaminants to travel through the unsaturated zone was unknown. However, the sediments of this aquifer are very coarse and are known for their ability to rapidly transport contaminants, such as nitrate [Chesnaux and Allen, 2007]. Therefore, if we were going to see 129I from Fukushima this was an ideal location.

The increases in groundwater 129I concentrations were seen in two different wells (ABB03 and PB20) located close to one another. The two wells also had slightly different recharge times. The first was 0.9 years and the second was 1.2 years. The 129I anomaly in the first well occurred at 0.9 years and in the second well at 1.2 years. These 129I anomalies, which occurred exactly when the recharge age predicted they would, suggests that some of the 129I deposited by Fukushima was reaching the wells and causing these increases.

Temporal variation in the concentration of 129I in groundwater in ABB03 and PB20. The solid vertical line shows the date of the Fukushima accident and the dashed horizontal line shows the median of each dataset respectively. The 3H/3He ages from [Wassenaar et al., 2006] of groundwater in each well and their uncertainty is pictured as the solid arrow which is aligned with the 129I anomaly possibly caused by the FDNA. The dashed arrow covers a 40 day (0.11 year) time span and represents a possible vadose zone transport time.

In order to verify if it was possible for 129I to travel from the ground surface to the water table in the time required to produce the variations observed we modelled its transport time and attenuation through the unsaturated zone.

The time it took for 129I to reach the water table in the model was then added to the previously dated recharge time to get an estimate for how long it might take 129I from Fukushima to reach the wells we sampled. The results show that it is indeed possible for 129I deposited in rain to infiltrate through the unsaturated zone and reach the wells in time for us to detect it. However, this rapid transport assumes that certain flow paths exist to rapidly conduct 129I due to the heterogeneous lithology of the unsaturated zone. There is evidence of such flow paths [McArthur et al., 2010].

To summarize,

Within a week of the FDNPP accident elevated 129I concentrations were observed in precipitation. This agrees very well with work on other radionuclides in air filters and rain.

129I concentrations in rain returned to background within a few weeks. However, discrete pulses of elevated 129I occurred for another several months.

Elevated 129I concentrations were measured in two wells and corresponded with the expected recharge times indicating that 129I from Fukushima can be traced into groundwater.

Vadose zone modeling has shown that 129I can be rapidly transported to the water table and reach the well screen in accordance with groundwater ages.

We propose 129I transport is enhanced by preferential dispersion of 129I that exists due to the heterogeneous nature of the vadose zone.

This results in variability in groundwater 129I concentrations that preserve the variability in the input of 129I via washout with some dampening of the signal due to attenuation and dilution.

Conceptual model showing the possible transport pathways of Fukushima derived 129I which was deposited via precipitation. A fraction of this 129I was rapidly transported through a heterogeneous vadose zone via preferential flowpaths to groundwater where minor 129I variation was detected. The remainder was retarded or attenuated in the vadose zone during transport.

Thanks for reading, if you have any questions or concerns please leave a comment or send me an email to discuss further!

*Note: 100 million atoms/L of 129I is equivalent to an activity of 0.00000014 (1.4 x 10^-7) Bq/L. These quantities are extremely low level and only the most sensitive analytical methods in the world can detect them. This amount of radioactivity is several orders of magnitude lower than the natural background radiation produced by naturally occurring radionuclides in soil and the atmosphere. For more on naturally occurring radioactivity see here. Even a clean rainfall has about 1 Bq/L of tritium (radioactive hydrogen), which remains from atmospheric weapons testing in the 1960’s

Access the full paper here: http://onlinelibrary.wiley.com/doi/10.1002/2015WR017325/abstract

References

Chesnaux, R., and D. M. Allen (2007), Simulating Nitrate Leaching Profiles in a Highly Permeable Vadose Zone, Environ. Model. Assess., 13(4), 527–539, doi:10.1007/s10666-007-9116-4.

McArthur, S. A. Q., D. M. Allen, and R. D. Luzitano (2010), Resolving scales of aquifer heterogeneity using ground penetrating radar and borehole geophysical logging, Environ. Earth Sci., 63(3), 581–593, doi:10.1007/s12665-010-0726-9.

Wassenaar, L. I., M. J. Hendry, and N. Harrington (2006), Decadal geochemical and isotopic trends for nitrate in a transboundary aquifer and implications for agricultural beneficial management practices., Environ. Sci. Technol., 40(15), 4626–32.

Wetherbee, G. A., D. A. Gay, T. M. Debey, C. M. B. Lehmann, and M. A. Nilles (2012), Wet Deposition of Fission-Product Isotopes to North America from the Fukushima Dai-ichi Incident, March 2011, Environ. Sci. Technol., 46(5), 2574–2582.

My EGU2013 (Tuesday)

Matt Herod April 11, 2013

Firstly, I am not actually attending EGU 2013 this year. However, that does not mean I can’t participate. In fact, it has been incredibly easy for to me join in, although I have had to wake up very early in the morning to make up for the time difference between Vienna and Ottawa.

I took part in two press conferences on Tuesday. The first called: The consequences of nuclear accidents: Fukushima and Europe and promised to be extremely interesting especially from my point of view as a researcher of environmental radionuclides. In fact, I was tuned in for more than just the EGU blogging part since I am in the midst of a project investigating the effects of Fukushima here in Canada and the transport of radionuclides from the accident. I intend to present the work at Goldschmidt later this year and write a publication on it which will comprise a part of my thesis.

The session was started by Dr. Yuichi Onda from the Centre for Research in Isotopes and Environmental Dynamics at the University of Tsukuba.

Dr. Onda and his group are studying the transfer and fallout of Fukushima radionuclides in every aspect of the environment. This is an incredibly daunting task. The infrastructure required to sample so many different environmental reservoirs is mind-boggling and Dr. Onda showed in several of his slides how tough it could be. The group sampled trees, soil, soil water, soil erosion, water in both cultivated and non cultivated environments, sediment in rivers and lakes as well as transport between these reservoirs and then finally the transport to the ocean from all of these sources. Basically, they set up one bad-a$$ monitoring network!

The conclusions from this network were that the deposition process of the radionuclides began by falling on trees but then over time washes off and between .2 and 3.5% of the fallout washes into streams and rivers where it is then transported to the oceans. In a very basic way it kind of looked like this:

Source: Wikipedia

The next speaker was Dr. Kazuyuki Kita from Ibaraki University. He was explaining one step earlier in the whole transport process than Dr. Onda since Dr. Kita’s focus is on the atmospheric transport and dispersion of radionuclides from Fuksuhima. Basically, once the accident occured tons of radionuclides were released into the atmosphere and blown hither and yon until they are eventually deposited in rain or adsorbed onto aerosols and settle because of gravity’s relentless nature. They can also be re-suspended after the fact. This is particularly common with iodine (I know about this one…) Dr. Kita then went on to show a picture of the fallout of cesium-137 over Japan, which is pictured below. Furthermore, the measured concentrations agreed very well with the predictions made by atmospheric modelling, which is a tricky business at the best of time, but must be even more so when the entire world is breathing down your neck asking where will the radionuclides go? The difference were due to rainout, which is difficult to predict.

Slide from Dr. Kita’s talk showing the actual fallout vs. the modelled fallout.

Dr. Kita then went on to talk about the variation of radionuclides in the atmosphere over time following the accident and the influence of re-suspension on radionuclides sitting on the land surface. He showed this graph which illustrates very clearly how 137Cs and 134Cs concentrations spiked following the accident and then declined over time. However, if you look in October you can see that the levels start to rise again, which Dr. Kita attributes to re-suspension. Furthermore, these peaks were coincident with the transport of air parcels from Fukushima as well making it certain that this was the source of the radionuclides. Another source of radionuclides since the disaster has been the re-emission of iodine and cesium from the ocean surface as well.

A slide from Dr. Kita’s talk showing the temporal trend in cesium fallout from Fukushima.

The final talk of the press conference was by Dr. Petra Seibert from the University of Vienna. Dr. Seibert, a meteorologist, gave a truly fascinating, yet somewhat scary talk about how prepared (or not) Europe is for nuclear accidents and the consequences they have with context from both Fukushima and Chernobyl. Dr. Seibert makes the point that despite ample opportunity to learn from our nuclear mistakes we have not addressed all of the deficiencies that exist.

Concerning Fukushima, Dr. Seibert points out that the dispersion of radionuclides from the nuclear plant is not simple and results in contamination outside of predicted zones. This means that the evacuation pattern of simply evacuating people in concentric circles depending on the distance from the plant is not a very effective way of ensuring that people are not affected since the atmospheric spread of radionuclides is not circular. Therefore, in order to be prepared for potential disasters a predictive model of dispersion is needed. Dr. Seibert has developed such a model and shows some of the incredibly variable, and somewhat artistic, results in the following image. The blank space shows a movie of a very complex dispersion.

A slide from Dr. Seibert’s talk showing the incredibly variable nature of radionuclide dispersion from a point source.

Dr. Seibert’s ultimate point is that despite what we have learned from Fukushima and Chernobyl we are not yet prepared enough to handle another large nuclear disaster. Indeed, she makes the point that one in Europe could result in continental scale contamination and that in order to prepare for this proactive measures like iodine tablets should be widely distributed. Furthermore, data distribution and communication between organizations and nations is not adequate as well, which would only serve to exacerbate the seriousness of a nuclear accident should one occur.

In my opinion to keys to avoiding another Chernobyl or Fukushima lies in open communication and learning everything we can from these two disasters. However, I put it to you, what do we still need to learn? What are our shortcomings when if comes to disaster preparedness. Do you agree with measures like iodine distribution in order to mitigate the risk from another accident or should we just cease nuclear energy production entirely?

I also tuned into the fantastic press conference on the Chelyabinsk meteorite fall, but Jon has covered it excellently so head over to his blog a for a summary of it. If you would like to watch the livestream of the press conference for yourself it can be found here: http://streams.h82.eu/EGU2013/index.php?modid=18&a=show&pid=206

Research Highlight – Variations of 129I in the atmospheric fallout of Tokyo, Japan: 1963-2003

Matt Herod December 13, 2012

I occasionally like to focus in on what I view as a key paper either in my particular field of iodine geochemistry or in the geochemical world at large. In this instance I have decided to highlight a paper in my field that releases a fantastic wealth of data that is matched nowhere else in the literature I have seen. This paper also reflects incredible dedication and planning to answer a scientific question that far exceeds that of most papers in terms of patience and structure. The reason I say this is because most datasets in papers today may reflect a few years of sampling. In my opinion the average is around 2-5 years of data for papers that concern modern processes. This is great, however, datasets such as this only represent a small snapshot of these processes and do not allow one to observe long term trends with much confidence. Indeed, most of these papers finish by saying more data is needed to reach conclusions about long term changes. The reason for this is usually money, grad students wanting to finish, etc. These are good reasons, particularly the latter, which I can really empathize with, however, the problem is that such short time periods are not really long enough to make robust conclusions about changes in the environment or that factors that are causing such changes. Most researchers overcome their piddly datasets by adding in the work of others to broaden their time periods. Obviously, there are problems with doing this such as differences in sampling location, sampling techniques, lab practices…the list goes on and on with reasons why two datasets from different researchers may not be exactly comparable. This practice is very common nonetheless. However, rarely papers come out that present many years worth of data all analysed by the same person, in the same place, and collected the same way. Such datasets are invaluable in the geochemistry world! The paper I review here is such a paper. In fact, it presents data for a 40 year period!!

The paper is by the AMS research group in the department of chemistry at Gakushin University in Tokyo, Japan. The authors are: Chiaki Toyama, Yasuyuki Muramatsu, Yuka Uchida, Yasuhito Igarashi, Michio Aoyama, and Hiroyuki Matsuzaki.

Why 129I

I thought this might be a good introductory section to add in order to bring everyone up to speed on what the value of researching 129I is. The main reason is that 129I levels are continually increasing globally and it is an emerging contaminant which we don’t want our environment, particularly 129I, which we don’t understand very well. The next reason is that we are still learning how iodine and 129I behave in the environment. They are tricky little elements that just won’t stay put no matter what the chemical conditions. Therefore, we need to better understand how they move and over what time scales. Lastly, 129I is produced by nuclear reactors and is present in large amounts in radioactive waste. This means that when we dispose of it and store it there is a very mobile isotope in there with a 16 million year half life. It is essential that we understand how it behaves and where it comes from.

Purpose

The purpose of this paper, that is to say the research questions that they authors are attempting to answer is:

1. What variations exist in the fallout rate of iodine-129 over time in Tokyo and what factors influence this fallout?

2. What are the sources of 129I in Tokyo?

3. How have nuclear accidents, such as Chernobyl, affected 129I concentrations in Tokyo?

4. What is the background concentration of 129I in Tokyo?

Sampling Methods

The samples were collected by the Japanese Meteorological Research Institute. Precipitation and particulate fallout samples were collected on a monthly basis from 1963 to 2003 and iodine was extracted as silver iodide and analyzed using accelerator mass spectrometry. Total iodine was analyzed with ICP-MS.

Results and Discussion

Unfortunately I cannot reproduce any figures from the paper…even though it has a graphical abstract…since Elsevier wants to charge me $20/figure to use them.

Anyway, I’ll make do without and try and describe the results without being too long winded.

– The 129I/127I ratio increased drastically during the 70’s and 80’s. It peaked at 4 orders of magnitude, or 10,000 times higher than the pre-anthropogenic ratio of 1.5 x 10^12. This increase is likely initially due to bomb testing, but the steady increase through the 80’s, which post dates most bomb testing means there is another cause.

– The deposition of 129I initially mimics the deposition of strontium-90 and cesium-137, both produced exclusively by bomb testing and nuclear reactor accidents. However, over time the 90Sr and 137Cs inputs decrease while the 129I remains steady. Also, there is a visible Chernobyl pulse for 90Sr and 137Cs, but not for 129I, although this is mainly since very little 129I was released from Chernobyl.

– The authors then compare the 129I deposition to the releases of 129I from the nearby Tokai Reprocessing Plant. The correlation is excellent. In order to guage the influence of European reprocessing plants the authors compared their results to another study looking at 129I in ice cores from the Alps, which found that there was a strong relationship to reprocessing releases. The Japanese deposition fluxes did not match the European very well. The suggests that 129I deposition in Tokyo is mainly from the Tokai plant.

– There was a consistent seasonal variation in 129I deposition in Tokyo. Indeed, the deposition of 129I was about 2 times higher in the spring than in the fall. This is consistent with other studies that have noticed a “spring peak” in radioactive fallout in mid-latitude regions. This is explained by a change in stratosphere-troposphere mixing in the spring (I have the reference if you want it). However, the authors also note that the air mass above Tokyo in the spring comes from Europe the higher levels could represent an influence of the European or Russian fuel reprocessing plants.

Conclusions

The principle conclusions of this article are:

1. The current ratio of 129I/I in atmospheric fallout is 10,000 times higher than the pre-anthropogenic, natural 129I/I ratio. This is primarily due to atmospheric weapons testing in the 1950’s and 60’s.

2. There is no detectable influence of the Chernobyl accident in atmospheric fallout in Tokyo. This is likely because the signal is hidden rather than not present.

3. The high deposition of 129I in the 1980’s is due to the influence of the nearby Tokai Nuclear Fuel Reprocessing Plant. There is no correlation between 129I and 137Cs and 90Sr, which indicates the recent rise in 129I concentrations are not due to bomb testing.

4. There is also a possibility of distant transport of 129I from overseas reprocessing facilities in Europe, Russia and China and the authors intend to assess this by carrying out further sampling in places throughout Japan.

These conclusions are not especially novel. Many other papers have clearly demonstrated the impact of nuclear fuel reprocessing on 129I fallout and the ease with which 129I can be transported atmospherically. Indeed, I have published a paper demonstrating this in the Yukon Territory. However, most papers, mine included, do not present the quantity of data to verify this conclusion that this one does. This makes this paper a fantastic addition to the body of 129I literature as well as provides an excellent starting point for future conclusions about changes in 129I fallout with time and the factors responsible for them. It also provides excellent context for future work. It is difficult to put 129I deposition fluxes in context over time and this data set opens that door.

Some Speculation

So many papers come out every day in the research community. I have often wondered what each one represents financially. I mean, how much does it cost to produce all this research? How much do the analyses cost, the sampling, the preparation, the time, the analytical equipment? None of these components is cheap, except maybe the grad student hours, and therefore, every paper that comes out represents a substantial financial investment on the part of the supervisor and the funding agencies. So I thought it might be an interesting thought experiment to guess what this paper may have cost to produce. I have no actual knowledge regarding what this paper cost to produce, but I can speculate a bit since I am familiar with the cost of AMS analysis and lab work. So here is my very, very rough cost breakdown. It is likely on the low side though since I am not going to factor in human labour hours, the cost of sampling, or the cost of using the lab equipment besides the AMS.

# of Samples: 80

AMS sample prep: ~$75/sample = $6000

Cost of AMS analysis per sample: ~$250/sample = $20,000

Cost of ICP-MS per samples: ~$25 x 80 = $2000

Grand Total: $28,000

I believe that the paper is sadly trapped behind a paywall. Therefore, if you would like to read the paper in full let me know in the comments below and leave me your email so I can pass it on to you.

Thanks for reading! If you have any questions or concerns I’d love to hear from you. Also, if you have an opinion on the paper or dataset I’d love to hear it as well

Citation

Toyama, C., Muramatsu, Y., Uchida, Y., Igarashi, Y., Aoyama, M., & Matsuzaki, H. (2012). Variations of 129I in the atmospheric fallout of Tokyo, Japan: 1963–2003 Journal of Environmental Radioactivity, 113, 116-122 DOI: 10.1016/j.jenvrad.2012.04.014

Matt

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