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Geoscience problems related to massive release of radioactive materials by nuclear accidents and other human activities

The session gathers geoscientific aspects such as dynamics, reactions, and environmental/health consequences of radioactive materials that are massively released accidentally (e.g., Chernobyl and Fukushima nuclear power plant accidents, wide fires, etc.) and by other human activities (e.g., nuclear tests).

The radioactive materials are known as polluting materials that are hazardous for human society, but are also ideal markers in understanding dynamics and physical/chemical/biological reactions chains in the environment. Thus, the radioactive contamination problem is multi-disciplinary. In fact, this topic involves regional and global transport and local reactions of radioactive materials through atmosphere, soil and water system, ocean, and organic and ecosystem, and its relations with human and non-human biota. The topic also involves hazard prediction and nowcast technology.

By combining 35 years (> halftime of Cesium 137) monitoring data after the Chernobyl Accident in 1986, 10 years dense measurement data by the most advanced instrumentation after the Fukushima Accident in 2011, and other events, we can improve our knowledgebase on the environmental behavior of radioactive materials and its environmental/biological impact. This should lead to improved monitoring systems in the future including emergency response systems, acute sampling/measurement methodology, and remediation schemes for any future nuclear accidents.

The following specific topics have traditionally been discussed:
(a) Atmospheric Science (emissions, transport, deposition, pollution);
(b) Hydrology (transport in surface and ground water system, soil-water interactions);
(c) Oceanology (transport, bio-system interaction);
(d) Soil System (transport, chemical interaction, transfer to organic system);
(e) Forestry;
(f) Natural Hazards (warning systems, health risk assessments, geophysical variability);
(g) Measurement Techniques (instrumentation, multipoint data measurements);
(h) Ecosystems (migration/decay of radionuclides).

The session consists of updated observations, new theoretical developments including simulations, and improved methods or tools which could improve observation and prediction capabilities during eventual future nuclear emergencies. New evaluations of existing tools, past nuclear contamination events and other data sets also welcome.

Co-organized by AS4/BG1/ERE1/ESSI4/GM12/NH8/OS4/SSS7
Convener: Daisuke Tsumune | Co-conveners: Yasunori IgarashiECSECS, Liudmila KolmykovaECSECS, Masatoshi Yamauchi
| Thu, 26 May, 08:30–11:05 (CEST)
Room 0.51

Thu, 26 May, 08:30–10:00

Chairperson: Masatoshi Yamauchi

On-site presentation
Yuichi Onda et al.

For the Fukushima region in Japan, the large-scale decontamination in the catchments needed to require more attention because of their possible consequence in altering particulate Cs-137 flux from the terrestrial environment to the ocean. Here, combining the high-resolution satellite dataset and concurrent river monitoring results, we quantitively assess the impacts of land cover changes in large-area decontaminated regions on river suspended sediment (SS) and particulate Cs-137 dynamics during 2013-2018. We find that the decontaminated regions’ erodibility dramatically enhanced during the decontamination stage but rapidly declined in the subsequent natural-restoration stage. River SS dynamics show linear response to these land cover changes, where annual SS load (normalized by water discharge) at the end of decontamination increased by over 300% than pre-decontamination and decreased about 48% at the beginning of natural restoration. Fluctuations in particulate Cs-137 concentrations well reflect the process of sediment source alternation due to land cover changes in decontaminated regions. The “Fukushima decontamination experiment” can reveal the dramatic impact of decontamination-natural restoration processes, which highlights the need for quantitatively assessing human impacts on land use and resultant alternation in sediment transfer patterns in large scale catchments. 

How to cite: Onda, Y., Bin, F., Wakiyama, Y., Taniguchi, K., Hashimoto, A., and Zhang, Y.: Decontamination and subsequent natural restoration processes impact on terrestrial systems in Niida River Catchment in Fukushima, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-10713, https://doi.org/10.5194/egusphere-egu22-10713, 2022.

Virtual presentation
Yasunori Igarashi et al.

The 2011 Fukushima Daiichi Nuclear Power Plant (FDNPP) accident released large amounts of radioactive materials into the environment. River systems play an important role in the terrestrial redistribution of FDNPP-derived 137Cs in association with water and sediment movement. We examined the seasonal fluctuations in dissolved and particulate 137Cs activity concentrations and clarified the biological and physicochemical factors controlling 137Cs in the Abukuma River’s middle course in the region affected by the FDNPP accident. The results showed the water temperature and K+ concentration dominated the seasonality of the dissolved 137Cs activity concentration. We concluded that the 137Cs in organic matter is not a source of dissolved 137Cs in river water. The study also revealed the temperature dependence of Kd in riverine environments from a Van ’t Hoff equation. The standard reaction enthalpy of 137Cs in the Abukuma River was calculated to be approximately −19.3 kJ/mol. This was the first study to clearly reveal the mechanisms by which the dissolved 137Cs activity concentration and Kd are influenced by chemical and thermodynamic processes in the middle course of a large river, and it is expected to lead to an improved model of 137Cs dynamics in rivers.

How to cite: Igarashi, Y., Kenji, N., Wada, T., Wakiyama, Y., Onda, Y., and Moritaka, S.: Factors controlling the dissolved 137Cs seasonal fluctuations in the Abukuma River under the influence of the Fukushima Nuclear Power Plant accident , EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-3340, https://doi.org/10.5194/egusphere-egu22-3340, 2022.

Virtual presentation
Yoshifumi Wakiyama et al.

This study presents the temporal variations in riverine 137Cs concentrations and fluxes to the ocean during high-flow events in three coastal river catchments contaminated by the Fukushima Daiichi Nuclear Power Plant accident. River water samples were collected at points downstream in the Niida, Ukedo, and Takase Rivers during three high-flow events that occurred in 2019–2020. Variations in both the dissolved 137Cs concentration and 137Cs concentration in suspended solids appeared to reflect the spatial pattern of the 137Cs inventory in the catchments, rather than variations in physico-chemical properties. Negative relationships between the 137Cs concentration and δ15N in suspended sediment were found in all rivers during the intense rainfall events, suggesting an increased contribution of sediment from forested areas to the elevated 137Cs concentration. The 137Cs flux ranged from 0.33 to 18 GBq, depending on the rainfall erosivity. The particulate 137Cs fluxes from the Ukedo River were relatively low compared with the other two rivers and were attributed to the effect of the Ogaki Dam reservoir upstream. The ratio of 137Cs desorbed in seawater to 137Cs in suspended solids ranged from 2.8% to 6.6% and tended to be higher with a higher fraction of exchangeable 137Cs. The estimated potential release of 137Cs from suspended solids to the ocean was 0.048–0.57 GBq, or 0.8–6.2 times higher than the direct flux of dissolved 137Cs from the river. Episodic sampling during high-flow events demonstrated that the particulate 137Cs flux depends on catchment characteristics and controls 137Cs transfer to the ocean. 

How to cite: Wakiyama, Y., Niida, T., Takata, H., Taniguchi, K., Kurosawa, H., Fujita, K., and Konoplev, A.: A comparative study of riverine 137Cs dynamics during high-flow events at three contaminated river catchments in Fukushima, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-3442, https://doi.org/10.5194/egusphere-egu22-3442, 2022.

Virtual presentation
Aleksei Konoplev et al.

Bottom sediments of lakes and dam reservoirs can provide an insight into understanding the dynamics of 137Cs strongly bound to sediment particles. On this premise, a number of cores of bottom sediments were collected in deep parts of lakes Glubokoe, Azbuchin, and Cooling Pond in close vicinity of the Chernobyl NPP in Ukraine, in Schekino reservoir (Upa River) in the Tula region of Russia (2018) and in Ogaki reservoir (Ukedo River) in Fukushima contaminated area (2019). Each layer of bottom sediments can be attributed to a certain time of suspended particles sedimentation. With 137Cs activity concentration in a given layer of bottom sediments corresponding to 137Cs concentration on suspended matter at that point in time, we were able to reconstruct the post-accidental dynamics of particulate 137Cs activity concentrations. Using experimental values of the distribution coefficient Kd, changes in the dissolved 137Cs activity concentrations were estimated. The annual mean particulate and dissolved 137Cs wash-off ratios were also calculated for the period after the accidents. Interestingly, the particulate 137Cs wash-off ratios for the Ukedo River at Ogaki dam were found to be similar to those for the Pripyat River at Chernobyl in the same time period after the accident, while the dissolved 137Cs wash-off ratios in the Ukedo River were an order of magnitude lower than the corresponding values in the Pripyat River. The estimates of particulate and dissolved 137Cs concentrations in Chernobyl cases were in reasonable agreement with monitoring data and predictions using the semi-empirical diffusional model. However, both the particulate and dissolved 137Cs activity concentrations and wash-off ratios in the Ukedo River declined faster during the first eight years after the FDNPP accident than predicted by the diffusional model, most likely, due to greater natural attenuation and, to some extent, remediation measures implemented on the catchments in Fukushima.

This research was supported by Science and Technology Research Partnership for Sustainable Development (SATREPS), Japan Science and Technology Agency (JST)/Japan International Cooperation Agency (JICA) (JPMJSA1603), by bilateral project No. 18-55-50002 of Russian Foundation for Basic Research (RFBR) and Japan Society for the Promotion of Science (JSPS), and JSPS Project KAKENHI (B) 18H03389.

How to cite: Konoplev, A., Wakiyama, Y., Wada, T., Igarashi, Y., Laptev, G., Golosov, V., Ivanov, M., Komissarov, M., and Nanba, K.: Vertical distribution of 137Cs in bottom sediments as representing the time changes of water contamination: Chernobyl and Fukushima, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-6698, https://doi.org/10.5194/egusphere-egu22-6698, 2022.

Virtual presentation
Taichi Kawano et al.

The Fukushima Daiichi Nuclear Power Plant (FDNPP) accident occurred on March 11, 2011, and a large amount of Cs-137 was released into the environment. It is important to clarify the behavior of radioactive cesium-137 in headwater catchments because most of the Cs-137 falls and is deposited in forest areas and is transported in the environment through river systems.

The purpose of this study was to clarify the influence of water quality composition and organic matter on the seasonal variation of dissolved Cs-137 concentrations in stream water based on long-term monitoring since 2011 at four headwaters catchments in Yamakiya district, Fukushima Prefecture (Iboishiyama, Ishidairayama, Koutaishiyama, Setohachiyama), located about 35 km northwest of FDNPP.

Water temperature, pH, and EC were measured in the field, and SS and coarse organic matter were collected using a time-integrated SS (suspended sediments) sampler and organic matter net. The Cs-137 concentrations was measured in the laboratory using a germanium detector. Concentrations of cations (Na⁺,K⁺,Ca²⁺,Mg²⁺,NH₄⁺) and anions (Cl⁻,SO₄²⁻,NO₃⁻,NO₂⁻,PO₄²⁻) were measured by ion chromatography after 0.45μm filtration. In addition, dissolved organic carbon (DOC) concentrations was measured using a total organic carbon analyzer.

The results showed that K⁺, which is highly competitive with Cs-137, was detected at Iboisiyama, Ishidairayama, and Koutaishiyama, while NH₄⁺ was only detected in some samples at Iboishiyama. There was no obvious relationship between dissolved ion concentration and water temperature, and between dissolved ion concentration and dissolved ¹³⁷Cs concentration at all sites. However, a positive correlation between dissolved cesium concentration and water temperature and DOC and water temperature was observed at all sites regardless of the presence of K⁺ and NH₄⁺. On the other hand, there was no clear relationship between the cesium concentrations in SS and organic matter and water temperature. These results suggest that the seasonal variation in dissolved Cs-137 concentrations in stream water with water temperature could be caused by the seasonality of microbial decomposition of organic matter.

How to cite: Kawano, T., Onda, Y., Takahishi, J., Makino, F., and Iwagami, S.: Seasonal variation of dissolved Cs-137 concentrations in headwater catchments in Yamakiya district, Fukushima Prefecture, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-7068, https://doi.org/10.5194/egusphere-egu22-7068, 2022.

Virtual presentation
Yuko Hatano et al.

Lake Onuma on Mt. Akagi (Gunma Prefecture, Japan) is a closed lake with an average water residence time of 2.3 years. The activity concentration of radioactive cesium in the lake was high shortly after the Fukushima accident. According to Suzuki et al. [1] and Watanabe [2], after a filtration process, Cs-137 are separated into two groups: particulate form and dissolved form. These two forms appears to have very different concentration profiles with each other,  when the Cs-137 concentration plotted against the sampled water depths. In the present study, we are going to model those behavior of particulate/dissolved forms with an emphasis on the depth dependency.

We consider a creation-annihilation process of plankton for the model of the particulate form, since diatom shells are found to be a major constituent of the particulate Cs-137 [2]. We set  ∂P/∂t = f(x,t)  and  f(x,t) = χ(x) cos(ωt) (0 ≤ x ≤ L(water column height), t > 0),  where P=P(x,t) is the activity concentration of the particulate form. The term f(x,t) is the rate of the net production of the plankton at a specific location x at a specific time t. Seasonal cycle is also taken into account by the cosine function (we neglect the phase shift here). The function χ(x), depends solely on water depth x, is responsible for dynamics or inhomogeneity of lake water, such as circulation, stratification or a thermocline. We assume that such a water structure relates to the production rate of plankton through the function χ(x). Thus, we may obtain the concentration of particulate Cs-137. For the dissolved concentration S(x,t), we use the classical diffusion equation with the diffusivity K being dependent on both space and time (i.e. K(x,t)), namely ∂S/∂t =  ∇•(K(x,t) ∇S). Here S=S(x,t) is the activity concentration of the dissolved form. The total activity concentration C(x,t) is the sum of P(x,t) and S(x,t). Using the pair of the equations, we can reproduce the followings. (1) depth profiles of each of the soluble- and particulate activity concentration and (2) depth profiles of the total Cs-137 concentration.

 [1] Suzuki, K. et al., Sci. Tot. Env. (2018)

 [2] Watanabe, S. et al.,  Proc. 20th Workshop on Environmental Radioactivity (2019)

How to cite: Hatano, Y., Akasaki, K., Suetomi, E., Okada, Y., Suzuki, K., and Watanabe, S.: Modeling the depth dependence of Cs-137 concentration in Lake Onuma , EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-1235, https://doi.org/10.5194/egusphere-egu22-1235, 2022.

On-site presentation
Hikaru Sato and Yuichi Onda

Radiocesium (137Cs) was one of the radioactive materials released from the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in March 2011. Highly 137Cs contaminated water from groundwater to the sea was reduced after installation of the sea-side impermeable wall as a countermeasure against contaminated water in October 2015. As a result, 137Cs contamination in water from other sources became more prominent and the levels of 137Cs concentration in seawater was correlated with rainfall fluctuation. To determine the source of contamination, we estimated the fluctuation patterns of 137Cs concentration in seawater, groundwater level, and discharge from the channels using the Antecedent Precipitation Index (Rw) method.
The results indicated that the fluctuation in seawater collected near the 1-4 Units had strong agreement with the 3 day half-life of Rw. The half-life is shorter than that estimated by groundwater level (7 to 30 day). Therefore, the 137Cs concentration in seawater was influenced by relatively faster runoff than the deep groundwater flow. We also made the spatial distribution map of 137Cs concentration in seawater to determine the sources of contamination. It showed that the 137Cs contaminated area was the highest at “south- inside the intake of 1-4 Units” where the outlets of the K and BC discharge channels are located. In particular, the concentration of 137Cs in the channel K was found to correlate with the concentration of 137Cs in seawater near the 1-4 Units (average of R2 = 0.5). These results indicate that the concentration of 137Cs in seawater inside the FDNPP port can be estimated by the Rw method and that the source of the contamination could be determined using the half-life.

How to cite: Sato, H. and Onda, Y.: Determining sources of the 137Cs concentration in seawater at Fukushima Daiichi Nuclear Power Plant using Antecedent Precipitation Index, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-9055, https://doi.org/10.5194/egusphere-egu22-9055, 2022.

Hiroaki Kato et al.

Radiocesium deposited in the forest canopy is transferred to the forest floor by rainwater and litterfall. Among them, stemflow likely increases the radiocesium inventory by concentrating rainwater around the trunk. However, the effects of stemflow on the influx of radiocesium into forest soil have not been evaluated quantitatively. In this study, the fluxes of rainwater via stemflow, throughfall, and soil infiltration water were observed. The concentration of dissolved 137Cs was measured in a cedar forest in Fukushima Prefecture, Japan. Soil infiltration water was collected at 5 cm and 20 cm depths at the distant point from the tree trunk (Bt), and the base of the tree trunk (Rd), where the influence of stemflow was strong. The observations were conducted during the period from September 2019 to November 2021. During the observation period, an experiment was conducted to intercept the inflow of rainwater via the throughfall or stemflow, and the change in soil infiltration water was observed. The observation results showed that the infiltration flux of radiocesium into the forest soil was significantly higher at the Rd site and about three times larger than at the Bt site. Particularly at the 20 cm depth at the Rd site, the soil infiltration water flux increased with the stemflow. The stemflow exclusion resulted in the dcrease of radiocesium flux by about 70% at all depths at the Rd site. These results suggest that the stemflow increases the input of radiocesium to the base of the tree trunk and facilitates its transfer to the deeper soil layers.

How to cite: Kato, H., Iida, H., Shinozuka, T., Niwano, Y., and Onda, Y.: Effects of stemflow on radiocesium infiltration into the forest soil, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-10817, https://doi.org/10.5194/egusphere-egu22-10817, 2022.

Valentyn Protsak et al.

Most of the territory of the Chernobyl Exclusion Zone (CEZ) is covered by forest. Forest of CEZ have accumulated a significant part of the radioactive release and for many years have served as a barrier to the non spreading of the radionuclide contamination outside the CEZ.

According to the classification of wildfire danger, the forests of CEZ belong to high, above average and medium classes, making cases of wildfires as quite common.

Poor, sod-podzolic soils of Ukrainian Polesye contribute to the entry the activity of 90Sr and 137Cs in plant biomass. During wildfires some of the radionuclides contained in combustion products of biomass are emitted into the atmosphere. Biologically important radionuclides such as 90Sr, 137Cs, plutonium isotopes and 241Am bound to fine aerosols - combustion products - can be transported with atmospheric flows over the long range, causing secondary radioactive fallout and forming additional inhalation dose loads on the population.

Lack of the actual information on the source term (rate of emission of radionuclides) does not allow reliable modeling of the radiological impact of wildfires. To address this issue, we have proposed a methodology that allows for operational assessments of the dynamics of radionuclide emissions into the atmosphere from wildfires in the CEZ.

The basic parameters for the calculations are

  • cartographic data on the density of radionuclide contamination of the territory of the CEZ;
  • classification of the territory of the CEZ according to the distributive features of forests and meadows;
  • classification of CEZ forests according to taxa characteristics to estimate amount of stored fuel biomass (kg/m2);
  • experimental data on the transfer of radionuclides from soil to the main components of biomass for the calculation of radionuclide inventory in fuel biomass (Bq/m2). Thus, for meadows the main fuel component is grass turf, while for forest these are litter, wood, bark and pine needles.
  • experimental data on emission factors of radionuclides from fuel biomass.

Implementation of the proposed algorithm in the form of GIS application makes it possible to assess the dynamics of radionuclide emission into the atmosphere by delineation the fire areas on the CEZ map. The NASA WorldView interactive mapping web application can be used to estimate the temporal and spatial characteristics of the wildfire while it is being developed. The contouring of the area affected by fire is carried out according to the analysis of the cluster of thermal points. Also, operational contouring of wildfire can be carried out using data delivered from unmanned aerial vehicles.

The application of the proposed algorithm for the analysis of the dynamics of 137Cs emissions into the atmosphere from the April 2020 wildfire showed a good agreement with the data reported by various authors who used the method of inverse simulation. Improving the accuracy of calculations according to the proposed algorithm can be done by rectifying radionuclide emission factors and taking into account fire intensity data, which in turn can affect both the radionuclide emission factor and the degree of burnout of plant biomass.

How to cite: Protsak, V., Laptev, G., Voitsekhovych, O., Hinchuk, T., and Korychenskyi, K.: Methodology for estimating the emission of radionuclides into the atmosphere from wildfires in the Chernobyl Exclusion Zone, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-11620, https://doi.org/10.5194/egusphere-egu22-11620, 2022.

Virtual presentation
Denis Dolgushin and Elena Korobova

A study of 137Cs distribution in a landscape cross-section characterizing the ELGS system (top-slope-closing depression) in the “Vyshkov-2” test site located in the Chernobyl abandoned zone, the Bryansk region, Russia, has been performed in 2015 and 2021. The test site (70×100 m) is located on the Iput’ river terrace in a pine forest characterized by the undisturbed soil-plant cover. Sod-podzolic sandy illuvial-ferruginous soils present the soil cover. The initial level of 137Cs contamination of the area varied from 1480 kBq/m2 to 1850 kBq/m2. Up to now, 89-99 % of the total 137Cs is fixed in the upper 20 cm soil layer with 70-96 % in the upper 8 cm. It allows field spectrometry data to study the structure of the 137Cs contamination field. The 137Cs activity was measured in the soil and moss cover along cross-sections with 1 m step by adapted gamma-spectrometer Violinist-III (USA). Cs-137 content in the soil cores’ and plant samples was determined in the laboratory by Canberra gamma-spectrometer with HPGe detector. It was shown that there is no unidirectional movement of 137Cs both in the soil and in the vegetation cover of the ELGS from the top to the closing depression. On the contrary, the data obtained allow us to state a pronounced cyclical variation of the 137Cs activity in ELGS, which can be traced in the soil and the vegetation. The variation appeared to be rather stable in space 29 and 35 years after the primary pollution. Cyclic fluctuation (variation) of 137Cs activity was described mathematically using Fourier-analysis, which was used to model the observed changes by the revealed three main harmonics. High and significant correlation coefficients obtained between the variation of 137Cs activity and the model for the soil-vegetation cover (r0,01= 0,868; n=17 - 2015; r0,01= 0,675; n=17 - 2021), soils (r0,01= 0,503-0,859; n=17) and moss samples (r0,01= 0,883; n=17 - 2015; r0,01= 0,678; n=17 - 2021) proved satisfactory fitting of models. The character of 137Cs variability in moss cover was generally similar to surface soil contamination, but the level of contamination and amplitude was specific.

The performed study confirmed specific features of 137Cs secondary migration in ELGS, which periodic functions describe. We infer that the observed cyclicity reflects elements’ migration in the ELGS system with water.

The reported study was funded by the Vernadsky Institute federal budget (research task #0137-2019-0006). The field works were supported partly by RFBR No 19-05-00816.

How to cite: Dolgushin, D. and Korobova, E.: Regularities of the 137Cs secondary distribution in the soil-moss cover of elementary landscape-geochemical systems and its dynamics within 6 years on the test site in the Chernobyl abandoned zone, Russia, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-8178, https://doi.org/10.5194/egusphere-egu22-8178, 2022.

Virtual presentation
Paballo Moshupya et al.

Human activities such as mining and processing of naturally occurring radioactive materials have a potential to result in enhanced radioactivity levels in the environment. In South Africa, there has been extensive mining of gold and uranium which produced large mine tailings dams that are highly concentrated with radioactive elements. The purpose of this study was to carry out a preliminary survey on a large scale to assess the activity concentrations of 238U, 232Th and 40K in mine tailings, soils and outcropping rocks in the West Rand District in South Africa. This was done to better understand the impact of the abandoned mine tailings on the surrounding soil. This study employed in-situ gamma spectrometry technique to measure the activity concentrations of 238U, 232Th and 40K. The portable BGO SUPER-SPEC (RS-230) spectrometer, with a 6.3 cubic inches Bismuth Germanate Oxide (BGO) detector was used for in-situ measurements. In mine tailings the activity concentrations for 238U, 232Th and 40K were found to range from 209.95 to 2578.68 Bq/kg, 19.49 to 108.00 Bq/kg and 31.30 to 626.00 Bq/kg, respectively. In surface soil, the activity concentration of 238U for all measurements ranged between 12.35 and 941.07 Bq/kg, with an average value of 59.15 Bq/kg. 232Th levels ranged between 12.59 and 78.36 Bq/kg, with an average of 34.91 Bq/kg. For 40K the average activity concentration was found to be 245.64 Bq/kg, in a range of 31.30 - 1345.90 Bq/kg. For the rock samples analyzed, average activity concentrations were 32.97 Bq/kg, 32.26 Bq/kg and 351.52 Bg/kg for 238U, 232Th and 40K, respectively. The results indicate that higher radioactivity levels are found in mine tailings than in rocks and soils. 238U was found to contribute significantly to the overall activity concentration in tailings dams as compared to 232Th and 40K. It has been observed that the mine tailings have a potential to impact on the activity concentration of 238U in soil in the immediate vicinity. However, on a regional scale it was found that the radioactivity levels in surface soil mainly depend on the radioelement concentration of the underlying rocks. The contamination is only confined to areas where mine tailings materials are washed off and deposited on surface soils in close proximity to tailings sources. This serves as an indication that the migration of uranium from tailings dams is localized and occurs within short distances. It is recommended that further radiological monitoring be conducted in areas found to have elevated concentration of uranium-238.

Keywords-In-situ gamma-ray spectrometry, Mine tailings, Radioactivity, Soil.

How to cite: Moshupya, P., Abiye, T., and Korir, I.: In-situ measurements of natural radioactivity levels in the gold mine tailings dams of the West Rand District, South Africa., EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-11669, https://doi.org/10.5194/egusphere-egu22-11669, 2022.

Virtual presentation
Michio Aoyama et al.

Radiocaesium derived from the Fukushima Dai-ichi Nuclear Power Plant (FNPP1) accident was observed across a wide area of the North Pacific, not only in surface seawater, but also in the ocean interior. In this presentation, we summarized the time scale of Lagrangian transport of the FNPP1 derived radiocaesium in surface water during the period from the time of the accident to March 2021 in the North Pacific and the Arctic Oceans and its marginal seas as shown below.

Initial observation results until December 2012 in the surface layer in the North Pacific Ocean by the global observations revealed that a typical feature within one year after the accident was a westward movement across the North Pacific Ocean, speed of which was reported at 7 km day-1 until August 2011. After that, the main body of FNPP1-derived radiocaesium moved east as 3 km day-1 and is separated from Japan in 2013. The arrival of the FNPP1 signal at the west coast of the American continent was reported in 2014. The elevation in the FNPP1 derived radiocaesium concentration in the Bering Sea in 2017 and in the Arctic Ocean in 2019 was reported. The northward bifurcation of the Kuroshio Extension made these obvious transport of the FNPP1 derived radiocaesium to the subarctic and arctic region while the transport by southward bifurcation was not observed. At Hawaii Islands in the subtropical gyre, there was no signal of the FNPP1 derived radiocaesium during the period from March 2011 and February 2017. At Yonaguni Island where the Kuroshio enters the East China Sea, the FNPP1 signal arrived at Yonaguni Islands eight years after the time of the accident, and these might be transported mainly from the subtropical gyre.

At the marginal seas of the North Pacific Ocean, the elevation in the FNPP1 derived radiocaesium concentration in the northern East China Sea in 2014, in the Sea of Japan in 2014/2015 were observed.

We also briefly summarize study results on nuclides other than radiocaesium (e.g., 90Sr, 239240Pu, and 129I).

How to cite: Aoyama, M., Kumamoto, Y., and Inomata, Y.: Ten-year long-range transport of radiocaesium in the surface layer in the Pacific Ocean and its marginal seas, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-9022, https://doi.org/10.5194/egusphere-egu22-9022, 2022.

Virtual presentation
Hyoe Takata

European seas such as, Baltic, North, and Norwegian Seas are mostly affected areas by the accident at the Chernobyl nuclear power plant (CNPP) in 1986. Since Fukushima Daiichi nuclear power plant (FDNPP) is located on the coast of the North Pacific Ocean in east Japan, its accident resulted in the release of large amounts of radiocesium to the surrounding coastal marine environment (i.e. the waters off Fukushima and neighboring prefectures). The temporal change of radiocaesium concentration in seawater after both accidents was largely dependent on their submarine topography: The Baltic Sea is a semi-closed basin, while Norwegian and North Seas, and the waters off Fukushima and neighboring prefectures is directly connected to open-water. Although concentration of radioacesium (137Cs) in the surface water of the Baltic Sea (central part) continuously decreased, the values in 1996, ten years after the accident, were even higher than pre-accident level in 1985. On the other hand, in the waters off Fukushima and neighboring prefectures 137Cs concentrations in 2020, nine years after the accident, are approaching the pre-accident levels of 2010. The quick decrease is attributable to the intrusion or mixing of water masses with low 137Cs.

How to cite: Takata, H.: Temporal trends of radio-cesium concentration in the marine environment after the Chernobyl and Fukushima Dai-ichi Nuclear Power Plant accidents, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-10644, https://doi.org/10.5194/egusphere-egu22-10644, 2022.

Virtual presentation
Daisuke Tsumune et al.

Radioactive cesium (137Cs) is distributed in the global ocean due to global fallout by atmospheric nuclear weapons tests, releases from reprocessing plants in Europe, and supplied to the ocean by the Fukushima Daiichi Nuclear Power Plant (1F NPP) accident. In order to detect future contamination by radionuclides, it is necessary to understand the global distribution of radionuclides such as 137Cs. For this purpose, observed data have been summarized in a historical database (MARIS) by IAEA. The spatio-temporal density of the observations varies widely, therefore simulation by an ocean general circulation model (OGCM) can be helpful in the interpretation of these observations.

In order to clarify the behavior of 137Cs in the global ocean, OGSM simulations were conducted. Parallel Ocean Program version 2 (POP2) of the Community Earth System Model version 2 (CESM2) is employed. The horizontal resolution is 1.125 degree of longitude, and from 0.28 degree to 0.54 degree of latitude. There are 60 vertical levels with a minimum spacing of 10 m near the ocean surface, and increased spacing with depth to a maximum of 250 m. The simulated period was from 1945 to 2030 with the circulation forced by repeating (“Normal Year”) atmospheric conditions. As input sources of 137Cs to the model, global fallout from atmospheric nuclear tests, releases from reprocessing plants in Europe, and input from the 1F NPP accident were considered. It was assumed that the input conditions in 2020 would continue after 2020.

The simulated 137Cs activity agrees well with the observed data in the database, especially in the Atlantic and Pacific Oceans where the observation density is large. Since 137Cs undergoes radioactive decay with a half-life of 30 years, the inventory for each basin is the difference between the decay corrected cumulative input and flux. In the North Pacific, the inventory reached its maximum in 1966 due to the global fallout by atmospheric nuclear weapons tests. Fluxes from the North Pacific to the Indian Ocean, Arctic Ocean, and Central Pacific were positive, and the North Pacific was a source of supply for other ocean basins. The 1F NPP accident caused a 20% increase in the inventory in 2011. In the North Atlantic, the inventory reaches its maximum in the late 1970s, due to the releases from the reprocessing plant. The outflow flux from the North Atlantic to the Greenland Sea is larger than the other fluxes and is a source of supply to other ocean basins. After 2000, the inflow flux to the North Pacific from the Labrador Sea and the South Atlantic is larger than the outflow flux.

The time series of 137Cs inventory in each ocean basin and the fluxes among ocean basins were quantitatively analyzed by OGCM simulations, and the predictions for the next 10 years were made.  The 137Cs activity concentrations by global fallout can be detected in the global ocean after 2030. The OGCM simulations will be useful in planning future observations to fill the gaps in the database.

How to cite: Tsumune, D., Bryan, F., Lindsay, K., Misumi, K., Tsubono, T., and Aoyama, M.: Estimation of 137Cs inventories in each ocean basin by a global ocean general circulation model for the global database interpolation, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-11022, https://doi.org/10.5194/egusphere-egu22-11022, 2022.

Discussion (1) How to proceed Chernobyl study

Thu, 26 May, 10:20–11:50

Chairperson: Yuichi Onda

On-site presentation
Sourabie Deo et al.

Chlorine 36 (36Cl, T1/2 = 301,000 years) is a radionuclide with natural and anthropogenic origin that can be rejected accidentally during decommissioning of nuclear power plants or chronically during recycling of nuclear waste. Once emitted into the atmosphere, 36Cl (gas and particles) can be transferred to the soil and vegetal cover by dry and wet deposition. However, knowledge of these deposits is very scarce. Because of its relatively high mobility in the geosphere and its high bioavailability, 36Cl fate in the environment should be studied for environmental and human impact assessments. So, the objective of this work is to determine the dry deposition rates of chlorine 36 on grassland. Grass is studied, as it is a link in the human food chain via cow's milk.

In order to achieve this objective, a method for extracting the chlorine contained in plant leaves has been developed. This method consists in heating the dried and grounded plant sample in presence of sodium hydroxide. A temperature gradient up to 450°C allows the extraction to be carried out in two stages: (i) The chlorides with a strong affinity for alkaline environments are first extracted from the plant and preserved in sodium hydroxide; (ii) The organic matter is then destroyed by combustion and the sodium hydroxide crystallised. Brought out from the oven, the dry residue is dissolved in ultrapure water and chemically prepared for the measurement of chlorine 36. This extraction method was validated by its application to NIST standards of peach and apple leaves. The average extraction efficiency of chlorides was 83 ± 3%.

For the determination of dry deposition rates, 1m2 of grass was exposed every 2 weeks at the IRSN La Hague technical platform (PTILH) located 2 km downwind from Orano la Hague, a chronic source of low-level chlorine 36 emissions. A mobile shelter with automatic humidity detection covered the grass during rainy episodes. In proximity to the grass, atmospheric chlorine was also sampled at the same frequency as the grass. Gaseous chlorine was sampled by bubbling in sodium hydroxide and by an AS3000 sampler containing activated carbon cartridge. Particulate chlorine was collected on a composite (teflon and glass fibre) filter. Chlorine 36 was measured by accelerated mass spectrometry ASTER (Accelerator for Earth Sciences, Environment and Risks) at CEREGE, Aix-en-Provence, France. All samples were subjected to a succession of chemical preparations in order to remove the sulphur 36 (an isobaric interferent) and to collect the chlorides in the form of AgCl pastilles. The results show a chlorine 36 deposition flux on the grass of 2.94.102 at/m2.s with a deposition velocity in dry weather vd(gas+particles) = 8.10-4 m/s for a contribution of 65.5% of particulate chlorine 36 and 34.5% of gaseous chlorine 36. Based on these experimental results, a modelling of the dry and wet deposits will be carried out considering the parameters related to the canopy and the atmospheric turbulence.

How to cite: Deo, S., Hebert, D., Benedetti, L., Vitorge, E., Lourino Cabana, B., Guillou, V., and Maro, D.: Dry deposition velocity of chlorine 36 on grassland, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-666, https://doi.org/10.5194/egusphere-egu22-666, 2022.

Virtual presentation
Shuhan Zhuang et al.

Wet deposition has been identified as a critical impactor for the modelling of 137Cs in the Fukushima Daiichi Nuclear power plant (FDNPP) accident. However, it is difficult to simulate due to the involvement of close interaction between various complicated meteorological and physical processes during the wet deposition process. The limitation of measurement of the in-cloud and below-cloud scavenging also contribute to the uncertainty in wet deposition modeling, leading to the great variation of 137Cs wet deposition parameterization. These variations can be amplified further by inaccurate meteorological input, making simulation of radionuclide transport sensitive to the choice of wet scavenging parameterization. Moreover, simulations can also be influenced by differences between radionuclide transport models, even if they adopt similar parameterization for wet scavenging. Although intensively investigated, wet deposition simulation is still subject to uncertainties of meteorological inputs and wet scavenging modeling, leading to biased 137Cs transport prediction.

To improve modeling of 137Cs transport, both in- and below-cloud wet scavenging schemes were integrated into the Weather Research and Forecasting-Chemistry (WRF-Chem) model, yielding online coupled modeling of meteorology and the two wet scavenging processes. Overall, 25 combinations of different in- and below-cloud scavenging schemes of 137Cs, covering most wet scavenging schemes reported in the literature, were integrated into WRF-Chem. Additionally, two microphysics schemes were compared to improve the simulation of precipitation. These 25 models and the ensemble mean of 9 representative models were systematically compared with a previous below-cloud-only WRF-Chem model, using the cumulative deposition and atmospheric concentrations of 137Cs measurements. The findings could elucidate the range of variation among these schemes both within and across the five in-cloud groups, reveal the behaviors and sensitivities of different schemes in different scenarios.

The results revealed that the Morrison's double moment cloud microphysics scheme improves the simulation of rainfall and deposition pattern. Furthermore, the integration of the in-cloud schemes in WRF-Chem substantially reduces the bias in the cumulative deposition simulation, especially in the Nakadori and Tochigi regions where light rain dominated. For atmospheric concentration of 137Cs, those models with in-cloud schemes that consider cloud parameters showed better and more stable performance, among which Hertel-Bakla performed best for atmospheric concentration and Roselle-Apsimon performed best for both deposition and atmospheric concentration. In contrast, the in-cloud schemes that rely solely on rain intensity were found sensitive to the meteorological conditions and showed varied performance in relation to the plume events examined. The analysis based on the spatial pattern shows that the Roselle scheme, which considers cloud liquid water content and depth, can achieve a more balanced allocation of 137Cs between the air and the ground in these two cases than that achieved by the empirical power function scheme Environ. The ensemble mean achieves satisfactory performance except for one plume event, but still outperforms most models. The range of variation of the 25 models covered most of the measurements, reflecting the reasonable capability of WRF-Chem for modeling 137Cs transport.

How to cite: Zhuang, S., Dong, X., and Fang, S.: Sensitivity analysis on the wet deposition parameterization for 137Cs transport modeling following the Fukushima Daiichi Nuclear Power Plant accident, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-177, https://doi.org/10.5194/egusphere-egu22-177, 2022.

Virtual presentation
Joffrey Dumont Le Brazidec et al.

    The Fukushima-Daiichi accident involved massive and complex releases of radionuclides in the atmosphere. The releases assessment is a key issue and can be achieved by advanced inverse modelling techniques combined with a relevant dataset of measurements. A Bayesian inversion is particularly suitable to deal with this case. Indeed, it allows for rigorous statistical modelling and enables easy incorporation of informations of different natures into the reconstruction of the source and the associated uncertainties.
    We propose several methods to better quantify the Fukushima-Daiichi 137Cs source and the associated uncertainties. Firstly, we implement the Reversible-Jump MCMC algorithm, a sampling technique able to reconstruct the distributions of the 137Cs source magnitude together with its temporal discretisation. Secondly, we develop methods to (i) mix both air concentration and deposition measurements, and to (ii) take into account the spatial and temporal information from the air concentration measurements in the error covariance matrix determination.
    Using these methods, we obtain distributions of hourly 137Cs release rates from 11 to 24 March and assess the performance of our techniques by carrying out a model-to-data comparison. Furthermore, we demonstrate that this comparison is very sensitive to the statistical modelling of the inverse problem.

How to cite: Dumont Le Brazidec, J., Bocquet, M., Saunier, O., and Roustan, Y.: Integrating measurement representativeness and release temporal variability to improve the Fukushima-Daiichi 137Cs source reconstruction, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-5397, https://doi.org/10.5194/egusphere-egu22-5397, 2022.

Virtual presentation
Xinwen Dong et al.

The nuclear emergency response for accidental release around the nuclear power plant site (NPPs) requires a fast and accurate estimate of the influence caused by gaseous hazardous pollutants spreading, which is critical for and preventing protecting lives, creatures, and the environment. However, as usual, the NPPs is consist of dense buildings and multi-type terrain, e.g. river and mountain, which poses challenges to atmospheric dispersion calculation for response tasks. Micro-SWIFT SPRAY (MSS) comprises both the diagnostic wind model and the dispersion model, which enables the airflows and atmospheric dispersion simulation with the meteorological and other inputs. For a small-scale scenario, especially, the separate module for obstacles influence modeling provides the potential capability of precise atmospheric dispersion. But the error behavior of such a scenario around a nuclear power plant site with complex topography remains to be further demonstrated. In this study, MSS is comprehensively evaluated against a wind tunnel experiment with a 1:600 scale for the small-scale (3 km × 3km) atmospheric dispersion modeling. Tens of buildings located in this scenario of a NPPs surrounded by a mountain and river. The evaluations for diagnostic wind modeling include the speed, direction, and distribution of horizontal airflows and vertical profile of speed at a representative site. And for the concentration calculation, horizontal distribution, axis profile, and vertical profile at a representative site. The results demonstrate the MSS can reproduce fine airflows near the buildings but overestimate the wind speed. The maximum deviation of vertical speed is around 2.09 m/s at the representative site. The simulated plume of concentration reproduces the highest concentration place and matches the observations well. The axis profile of concentration is underestimated and the vertical profile displays an increasing deviation with the height increase. Compared with the observations, the FAC5 and FAC2 of concentration simulation reach 0.945 and 0.891 in the entire calculation domain, which convinces the performance of MSS in small-scale modeling.

How to cite: Dong, X., Zhuang, S., and Fang, S.: Micro-SWIFT SPRAY modeling of atmospheric dispersion around a nuclear power plant site with complex topography, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-190, https://doi.org/10.5194/egusphere-egu22-190, 2022.

Dean Connor et al.

All radiological measurements acquired from airborne detectors suffer from the issues of geometrical signal dilution, signal attenuation and a complex interaction of the effective sampling area of the detector system with the 3D structure of the surrounding environment. Understanding and accounting for these variables is essential in recovering accurate dose rate maps that can help protect responding workforces in radiologically contaminated environments.

Two types of terrain-cognisant methods of improving source localisation and the contrast of airborne radiation maps are presented in this work, comprising of ‘Point Cloud Constrained 3D Backprojection’ and ‘Point Cloud Constrained Randomised Kaczmarz Inversion’. Each algorithm uses a combination of airborne gamma-spectrometry and 3D scene information collected by UAS platforms and have been applied to data collected with lightweight, simple (non-imaging) detector payloads at numerous locations across the Chornobyl Exclusion Zone (CEZ).

Common to both the algorithms is the projection of the photopeak intensity onto a point cloud representation of the environment, taking into account the position and orientation of the UAS in addition to the 3D response of the spectrometer. The 3D Backprojection method can be considered a relatively fast method of mapping of through proximity, in which the measured photopeak intensity is split over the point cloud according to the above factors. It is an additive technique, with each measurement increasing the overall magnitude of the radiation field assigned to the survey area, meaning that more measurements continues to increase the total radiation of the site. The total measured intensity of the solution is then normalised according to the time spent in proximity to each point in the scene, determined by splitting and projecting the nominal measurement time at each survey point over the point cloud according to the distance from the survey position. Thus accounting for sampling biases during the survey.

The inversion approach adapts algorithms routinely used in medical imaging for the unconstrained world in which the detector is no longer completely surrounding the subject/target. A forward projection model, based on the contribution of distant point sources to the detector intensity, is used to determine the relationship between the full set of measurements and the 3D scene. This results in a hypercube of linear equations where it is assumed every point in the scene contributes to the measured intensity. The algorithm randomly adds measurements from within the aerial set and back-projects this onto the point cloud, with the initial state of the solution set to emit no radiation. After a given number of iterations, the fit of the current solution to the original measurements is assessed though a least squares method and updated when this produces a fit better than the current best estimate. This continues to happen until a minimum value is reached before the divergence of the system, representing the most confident solution. Based on examples from both simulations and real world data, the improvement in contrast of airborne maps using this inversion method can make them equivalent to ground-based surveys, even when operating at 20 m AGL and above.

How to cite: Connor, D., Megson-Smith, D., Wood, K., Mackenzie, R., Connolly, E., White, S., Russell-Pavier, F., Ryan-Tucker, M., Martin, P., Verbelen, Y., Richardson, T., Smith, N., and Scott, T.: Mapping of Post-Disaster Environments using 3D Backprojection and Iterative Inversion Methods Optimised for Limited-Pixel Gamma Spectrometers on Unoccupied Aerial Systems (UAS). , EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-11571, https://doi.org/10.5194/egusphere-egu22-11571, 2022.

Virtual presentation
Evaldas Maceika et al.

Considerable amounts of 14C in the nuclear reactor are generated by neutrons. It accumulates in reactor components, coolant, and cleaning systems, and partly is released into the environment as gaseous releases and as liquid effluents. Two RBMK-1500 type reactors were exploited at Ignalina NPP (Lithuania) 1983-2009. Releases from NPP radiocarbon accumulated in local biosphere by photosynthesis, including terrestrial and aquatic media, as INPP used Lake Drūkšiai as a cooling pond

Temporal variation of 14C in lake ecosystem was examined by analyzing measured radiocarbon concentration of the organic compounds (Alkali soluble-AS) and alkali insoluble-AIS) derived from the layers of the Drūkšiai lake bottom sediments. The lake sediment cores were sampled in 2013 and 2019, sliced to 1 cm layers and 14C concentration was measured of every layer. AS and AIS organic fractions of sediment samples were extracted by using the acid-base-acid method.

Tree ring cores were collected from Pinus Sylvestris pines around the Ignalina NPP site at different directions and distances. Cellulose extraction was performed with BABAB (base-acid-base-acid-bleach) procedure, and all samples were graphitized and measured by a single state accelerator mass spectrometry at Vilnius Radiocarbon facility. Tree rings 14C concentration analysis provides atmospheric radiocarbon concentration in locations around the nuclear object. This analysis provides an opportunity to evaluate the impact of a nuclear object on water and terrestrial ecosystems.

The results showed a pronounced increase of 14C above background up to 17.8 pMC in the tree rings during INPP exploitation as well during decommission (since 2010) periods. According to the recorded data in 2004-2017 of the local Ignalina NPP meteorological station, the prevailing wind direction was towards the North and East during warm and light time periods. The radiocarbon released from the INPP stack dilutes when it travels in a downwind direction from the INPP. However, even 6.6 km away from the INPP, the impact of the power plant is still clearly visible. By using our created Gaussian dispersion model, the estimated annual emissions of 14C activity from the Ignalina NPP to the air vary from year to year. When only the 1st INPP reactor Unit was operating in 1985-1987, average emissions were 1.2 TBq/year. Emissions almost doubled to 2.1 TBq/year in 1988, when the 2nd Unit became operational. Later, emission levels increased. It could be explained by the large amount of 14C accumulating in the graphite of the RBMK reactor and its gradual release.

14C concentration profile analysis of the lake bottom sediments core revealed a significant impact of the Ignalina NPP on the Drūkšiai lake ecosystem. An increase of 14C concentration in the layers of bottom sediments by 80 pMC in the AS fraction and only by 9 pMC in the AIS fraction was observed, corresponding to the period about years of 1998-2003. The maximum peak in AS of 189 pMC was reached approximately in 2001, followed by gradual lake recovery. This radiocarbon peak in the lake represents a large single one-time pollution release. The critical period was in 2000s when maintenance works of the reactors were performed.

How to cite: Maceika, E., Barisevičiūtė, R., Juodis, L., Pabedinskas, A., Ežerinskis, Ž., Šapolaitė, J., Butkus, L., and Remeikis, V.: Retrospective assessment of 14C aquatic and atmospheric releases from Ignalina Nuclear Power Plant due to exploitation of two RBMK-1500 type reactors, EGU General Assembly 2022, Vienna, Austria, 23–27 May 2022, EGU22-11502, https://doi.org/10.5194/egusphere-egu22-11502, 2022.

Discussion(2) Counter measure possible new accident.