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Journal Articles

Sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions onto sedimentary rock in the presence of gamma-irradiated humic acid

Zhao, Q.*; Saito, Takeshi*; Miyakawa, Kazuya; Sasamoto, Hiroshi; Kobayashi, Taishi*; Sasaki, Takayuki*

Journal of Hazardous Materials, 428, p.128211_1 - 128211_10, 2022/04

The influence of humic acid and its radiological degradation on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ by sedimentary rock was investigated to understand the sorption process of metal ions and humic substances. Aldrich humic acid (HA) solution was irradiated with different doses of gamma irradiation using a Co-60 gamma-ray source prior to the contact between the metal ions and the solid sorbent. The HA molecule decomposed to smaller molecules with a lower complexation affinity. Batch sorption experiments were performed to evaluate the effect of gamma-irradiated HA on the sorption of Cs$$^{+}$$ and Eu$$^{3+}$$ ions. The addition of non-irradiated HA weakened the sorption of Eu because of the lower sorption of the neutral or negatively charged Eu-HA complexes compared with free Eu ions. The sorption of monovalent Cs ions was barely affected by the presence of HA and its gamma irradiation. The concentration ratio of HA complexed species and non-complexed species in the solid and liquid phases was evaluated by sequential filtration and chemical equilibrium calculations. The ratios supported the minimal contribution of HA to Cs sorption. However, the concentration ratio for Eu$$^{3+}$$ in the liquid phase was high, indicating that the complexing ability of HA to Eu$$^{3+}$$ was higher than that of HA to Cs$$^{+}$$ ions. Therefore, the sorption of free Eu$$^{3+}$$ would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.

Journal Articles

Decrease of radionuclide sorption in hydrated cement systems by organic ligands; Comparative evaluation using experimental data and thermodynamic calculations for ISA/EDTA-actinide-cement systems

Ochs, M.*; Dolder, F.*; Tachi, Yukio

Applied Geochemistry, 136, p.105161_1 - 105161_11, 2022/01

Various types of radioactive wastes and environments contain organic substances that can stabilize the aqueous complexes with radionuclides and therefore lead to a decrease of sorption. The present study focuses on testing a methodology to quantify sorption reduction factors (SRFs) in the presence of organic ligands for cement systems. Three approaches for the estimation of SRFs; (1) analogy with solubility enhancement factors, (2) radionuclide speciation based on the thermodynamic calculations, and (3) experimental sorption data in ternary systems, were coupled and tested for the representative organic ligands (ISA and EDTA) and selected key radionuclides (actinides). Our approach allows to critically evaluate the dependence of SRFs for various systems on the chosen method of quantification, in accordance with the data availability for a given systems. The reliable SRFs can only be derived from the sorption measurements in ternary systems. SRF often need to be derived in the absence of such direct evidence, and estimations need to be made based on analogies and speciation information. However, such estimates may be subject to substantial uncertainties.

Journal Articles

A Scaling approach for retention properties of crystalline rock; Case study of the in-situ long-term sorption and diffusion experiment (LTDE-SD) at the $"A$sp$"o$ Hard Rock Laboratory in Sweden

Tachi, Yukio; Ito, Tsuyoshi*; Gylling, B.*

Water Resources Research, 57(11), 20 Pages, 2021/11

This paper focuses on the scaling approach for sorption and diffusion parameters from laboratory to in-situ conditions using the dataset of LTDE-SD experiment performed at the $"A$sp$"o$ HRL. The near-surface heterogeneities at both fracture surface and rock matrix could be evaluated by conceptual model with high porosity and diffusivity, and sorption capacity, and their gradual change at the near-surface zones. The modelling results for non-sorbing Cl-36 and weak-sorbing Na-22 could validate the model concept and the parameter estimation of porosity and diffusivity, by considering the disturbed zone of 5 mm thickness with gradual parameter changes. The De values of these cationic and anionic tracers showed typical cation excess and anion exclusion effects. The modelling results for high sorbing tracers (Cs-137, Ra-226, Ni-63 and Np-237) with different sorption mechanism could confirm the validity of the scaling approaches of Kd values as a function of particle size and their relation to the near-surface disturbances.

Journal Articles

Experimental study on modeling of Pu sorption onto quartz

Hemmi, Ko; Walker, A.*; Yamaguchi, Tetsuji

Radiochimica Acta, 109(7), p.539 - 546, 2021/07

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Plutonium(IV) sorption onto quartz in carbonate solutions was systematically investigated under anaerobic conditions to analyze the sorption behaviors of Pu(IV) with a non-electrostatic model (NEM). Pu(IV) sorption data was obtained from batch sorption experiments as a function of pH and carbonate concentration. The Pu(IV) sorption onto quartz showed similar tendencies to Th(IV), which is considered to be chemically analogous as a tetravalent actinoid. The distribution coefficient, ${it K}$d, of Pu(IV) onto quartz showed inverse proportionality to the square of the total carbonate concentration under the investigated pH conditions of 8 to 11. The modeling study, however, revealed a Th(IV) sorption model, which is $$equiv$$SOTh(OH)$$_{4}$$$$^{-}$$ and $$equiv$$SOThOH(CO$$_{3}$$)$$_{2}$$$$^{2-}$$, could not be applied to simulate the Pu(IV) sorption onto quartz. It was inferred that the electrostatic repulsion between negatively charged ligands limited the formation of $$equiv$$SOM(OH)$$_{4}$$$$^{-}$$ and $$equiv$$SOMOH(CO$$_{3}$$)$$_{2}$$$$^{2-}$$ for Pu(IV) with smaller ionic radii than Th(IV). The Pu(IV) sorption model was developed as $$equiv$$SOPu(OH)$$_{3}$$ and $$equiv$$SOPu(OH)$$_{4}$$$$^{-}$$. In addition, data of Pu(IV) sorption onto muscovite was obtained in order to be compared with data for quartz.

Journal Articles

Evaluation report of Task 9B based on comparisons and analyses of modelling results for the $"A$sp$"o$ HRL LTDE-SD experiments

Soler, J. M.*; Meng, S.*; Moreno, L.*; Neretnieks, I.*; Liu, L.*; Kek$"a$l$"a$inen, P.*; Hokr, M.*; $v{R}$$'i$ha, J.*; Vete$v{s}$n$'i$k, A.*; Reimitz, D.*; et al.

SKB TR-20-17, 71 Pages, 2021/07

Task 9B of the SKB Task Force on Modelling of Groundwater Flow and Transport of Solutes in fractured rock focused on the modelling of experimental results from the LTDE-SD in situ tracer test performed at the $"A$sp$"o$ Hard Rock Laboratory in Sweden. Ten different modelling teams provided results for this exercise, using different concepts and codes. Three main types of modelling approaches were used: (1) analytical solutions to the transport-retention equations, (2) continuum-porous-medium numerical models, and (3) microstructure-based models accounting for small-scale heterogeneity (i.e. mineral grains and microfracture distributions). The modelling by the different teams allowed the comparison of many different model concepts, especially in terms of potential zonations of rock properties (porosity, diffusion, sorption), such as the presence of a disturbed zone at the rock and fracture surface, the potential effects of micro- and cm-scale fractures.

Journal Articles

Consideration on modeling of Nb sorption onto clay minerals

Yamaguchi, Tetsuji; Ohira, Saki; Hemmi, Ko; Barr, L.; Shimada, Asako; Maeda, Toshikatsu; Iida, Yoshihisa

Radiochimica Acta, 108(11), p.873 - 877, 2020/11

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Journal Articles

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant, 2; Sorption and fixation behaviors and their relationship to sediment properties

Tachi, Yukio; Sato, Tomofumi*; Takeda, Chizuko*; Ishidera, Takamitsu; Fujiwara, Kenso; Iijima, Kazuki

Science of the Total Environment, 724, p.138097_1 - 138097_10, 2020/07

 Times Cited Count:2 Percentile:39.03(Environmental Sciences)

To understand and predict radiocesium transport behaviors in the environment, sorption and fixation behaviors of radiocesium on river sediments from Ukedo and Odaka rivers around the Fukushima Daiichi Nuclear Power Plant were investigated systematically focusing on Cs sorption and fixation mechanisms and their relationship with Cs concentrations and sediment properties including clay mineralogy and organic matter.

Journal Articles

Development of fission product chemistry database ECUME for the LWR severe accident

Miwa, Shuhei; Nakajima, Kunihisa; Miyahara, Naoya; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Imoto, Jumpei; Afiqa, B. M.; et al.

Mechanical Engineering Journal (Internet), 7(3), p.19-00537_1 - 19-00537_11, 2020/06

We constructed the fission product (FP) chemistry database named ECUME for LWR severe accident. This version of ECUME is equipped with dataset of the chemical reactions and their kinetics constants for the reactions of cesium(Cs)-iodine(I)-boron(B)-molybdenum(Mo)-oxygen(O)-hydrogen(H) system in gas phase, the elemental model for the high temperature chemical reaction of Cs with stainless steel applied as the structural material in a reactor, and thermodynamic data for CsBO$$_{2}$$ vapor species and solids of Cs$$_{2}$$Si$$_{4}$$O$$_{9}$$ and CsFeSiO$$_{4}$$ for these chemical reactions. The ECUME will provide estimation of Cs distribution due to the evaluation of effects of interaction with BWR control material B and stainless steel on Cs behavior in the Fukushima Daiichi Nuclear Power Station.

Journal Articles

Study on chemisorption model of cesium hydroxide onto stainless steel type 304

Nakajima, Kunihisa; Nishioka, Shunichiro*; Suzuki, Eriko; Osaka, Masahiko

Mechanical Engineering Journal (Internet), 7(3), p.19-00564_1 - 19-00564_14, 2020/06

A large amount of cesium (Cs) chemisorbed onto stainless steel is predicted to be present especially in the upper region of reactor pressure vessel (RPV) during light water reactor severe accident (LWR SA) and a chemisorption model was developed for estimation of such amounts of Cs for stainless steel type 304 (SS304). However, this existing chemisorption model cannot accurately reproduce experimental results. Therefore, in this study, a modified Cs chemisorption model which accounts for silicon content in SS304 and concentration of cesium hydroxide (CsOH) in gaseous phases was constructed by combining penetration theory for gas-liquid mass transfer with chemical reaction and mass action law for CsOH decomposition at interface between gaseous and solid phases. As a result, it was found that the modified model was able to reproduce the experimental data more accurately than the existing model.

Journal Articles

Sorption behavior of selenide on montmorillonite

Sugiura, Yuki; Tomura, Tsutomu*; Ishidera, Takamitsu; Doi, Reisuke; Francisco, P. C. M.; Shiwaku, Hideaki; Kobayashi, Toru; Matsumura, Daiju; Takahashi, Yoshio*; Tachi, Yukio

Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05

 Times Cited Count:1 Percentile:0.01(Chemistry, Analytical)

JAEA Reports

Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2019

Sugiura, Yuki; Suyama, Tadahiro*; Tachi, Yukio

JAEA-Data/Code 2019-022, 40 Pages, 2020/03


Sorption behavior of radionuclides (RNs) in buffer materials, rocks and cementitious materials is one of the key processes in a safe geological disposal. This report focuses on updating of JAEA sorption database (JAEA-SDB) as a basis of integrated approach for the performance assessment (PA)-related distribution coefficient (K$$_{rm d}$$) setting and development of mechanistic sorption models. K$$_{rm d}$$ data and their quality assurance (QA) results were updated by focusing on the following systems as potential needs extracted from our recent activities on the K$$_{rm d}$$ setting and development of mechanistic models, i.e., clay minerals, sedimentary rocks and cementitious materials. As a result, 6,702 K$$_{rm d}$$ data from 60 references were added and the total number of K$$_{rm d}$$ values in JAEA-SDB reached 69,679. The QA/classified K$$_{rm d}$$ data reached about 72% for all K$$_{rm d}$$ data in JAEA-SDB.

JAEA Reports

Data acquisition for radionuclide sorption on barrier materials for performance assessment of geological disposal of TRU wastes

Tachi, Yukio; Suyama, Tadahiro*; Mihara, Morihiro

JAEA-Data/Code 2019-021, 101 Pages, 2020/03


Sorption of radionuclides in cement and bentonite as engineered barrier materials, and rocks as natural barrier is the one of key processes in the performance assessment of geological disposal of TRU and high-level waste. The magnitude of sorption, expressed normally by a distribution coefficient (K$$_{rm d}$$), needs to be measured and determined taking into account the properties of barrier materials and geochemical conditions and associated uncertainty in the performance assessment. The basic concept for TRU waste disposal contains cementitious materials as an engineered barrier materials, in addition to bentonite and rock. It is therefore needed to consider the effects of the cement degradation and co-existing substances such as nitrates on radionuclide sorption. This report focused on data acquisition of distribution coefficient (K$$_{rm d}$$) by batch sorption experiments for the systems coupling barrier material-chemical condition-radionuclides that are needed to consider for the performance assessment of geological disposal of TRU waste. The barrier materials considered are ordinary Portland cement (OPC), degraded OPC and tuff rock. The chemical conditions are distilled water and synthetic seawater equilibrated with OPC and those containing nitrates and ammonium salts, etc. The radionuclides considered are organic carbon, inorganic carbon, Cl, I, Cs, Ni, Se, Sr, Sn, Nb, Am and Th. Although K$$_{rm d}$$ values have been partly reported previously as RAMDA (Radionuclide Migration Datasets) for the performance assessment in the TRU-2 report, these results and addition K$$_{rm d}$$ data are reported with the details of experimental methods and conditions.

Journal Articles

Cesium chemisorbed species onto stainless steel surfaces; An Atomistic scale study

Miradji, F.; Suzuki, Chikashi; Nakajima, Kunihisa; Osaka, Masahiko

Journal of Physics and Chemistry of Solids, 136, p.109168_1 - 109168_9, 2020/01

 Times Cited Count:1 Percentile:23.44(Chemistry, Multidisciplinary)

Journal Articles

An Experimental investigation of influencing chemical factors on Cs-chemisorption behavior onto stainless steel

Nishioka, Shunichiro; Nakajima, Kunihisa; Suzuki, Eriko; Osaka, Masahiko

Journal of Nuclear Science and Technology, 56(11), p.988 - 995, 2019/11

 Times Cited Count:6 Percentile:75.46(Nuclear Science & Technology)

In order to contribute to improvement of Cs chemisorption model used in severe accident analysis codes, the influence of chemical factors (temperature, atmosphere, concentration of affecting chemical elements etc.) on the Cs chemisorption behaviour onto stainless steel was investigated experimentally. It was found that the surface reaction rate constant used in the current Cs-chemisorption model was influenced by not only temperature, as already known, but also atmosphere, cesium hydroxide (CsOH) concentration in the gas phase and silicon content in SS304. Such chemical factors should be considered for the construction of the improved Cs-chemisorption model. Another important finding is that the chemisorption behavior at lower temperatures, around 873 K, could differ from those above 1073 K. Namely, Cs-Fe-O compounds would form as the main Cs-chemisorbed compounds at 873 K while Cs-Si-Fe-O compounds at more than 1073 K.

Journal Articles

Experimental determination of the photooxidation of aqueous I$$^{-}$$ as a source of atmospheric I$$_{2}$$

Watanabe, Kosuke*; Matsuda, Shohei; Cuevas, C. A.*; Saiz-Lopez, A.*; Yabushita, Akihiro*; Nakano, Yukio*

ACS Earth and Space Chemistry (Internet), 3(4), p.669 - 679, 2019/04

 Times Cited Count:2 Percentile:26.9(Chemistry, Multidisciplinary)

The photooxidation of aqueous iodide ions (I$$^{-}$$$$_{(aq)}$$) at sea surface results in the emission of gaseous iodine molecules (I$$_{2}$$$$_{(g)}$$) into the atmosphere. It plays a certain role in the transport of iodine from ocean to the atmosphere in the natural cycle of iodine. In this study, we determined the photooxidation parameters, the molar absorption coefficient ($$varepsilon$$$$_{iodide}$$($$lambda$$)) and the photooxidative quantum yields ($$Phi$$$$_{iodide}$$($$lambda$$)) of I$$^{-}$$$$_{(aq)}$$, in the range of 290-500 nm. Through the investigation of the influence of pH and dissolved oxygen (DO) on $$Phi$$$$_{iodide}$$($$lambda$$), the subsequent emission rates of I$$_{2}$$$$_{(g)}$$ following the photooxidation of I$$^{-}$$$$_{(aq)}$$ in deionized water solution (pH 5.6, DO 7.8 mg L$$^{-1}$$) and artificial seawater solution (pH 8.0, DO 7.0 mg L$$^{-1}$$) were estimated. A global chemistry-climate model employed herein to assess the I$$_{2}$$$$_{(g)}$$ ocean emission on a global scale indicated that the photooxidation of I$$^{-}$$$$_{(aq)}$$ by solar light can enhance the atmospheric iodine budget by up to $$sim$$8% over some oceanic regions.

Journal Articles

A Systematic radionuclide migration parameter setting approach for potential siting environments in Japan

Hamamoto, Takafumi*; Ishida, Keisuke*; Shibutani, Sanae*; Fujisaki, Kiyoshi*; Tachi, Yukio; Ishiguro, Katsuhiko*; McKinley, I. G.*

Proceedings of 2019 International High-Level Radioactive Waste Management Conference (IHLRWM 2019) (USB Flash Drive), p.77 - 82, 2019/04

Journal Articles

Modelling of cesium chemisorption under nuclear power plant severe accident conditions

Miradji, F.; Suzuki, Chikashi; Nishioka, Shunichiro; Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko; Barrachin, M.*; Do, T. M. D.*; Murakami, Kenta*; Suzuki, Masahide*

Proceedings of 9th Conference on Severe Accident Research (ERMSAR 2019) (Internet), 21 Pages, 2019/03

Journal Articles

Laser-induced breakdown spectroscopy and related resonance spectroscopy for nuclear fuel cycle management and for decommissioning of "Fukushima Daiichi Nuclear Power Station"

Wakaida, Ikuo; Oba, Hironori; Miyabe, Masabumi; Akaoka, Katsuaki; Oba, Masaki; Tamura, Koji; Saeki, Morihisa

Kogaku, 48(1), p.13 - 20, 2019/01

By Laser Induced Breakdown Spectroscopy and by related resonance spectroscopy, elemental and isotope analysis of Uranium and Plutonium for nuclear fuel materials and in-situ remote analysis under strong radiation condition for melt downed nuclear fuel debris at damaged core in "Fukushima Daiichi Nuclear Power Station", are introduced and performed as one of the application in atomic energy research field.

Journal Articles

Evaluation and modelling report of Task 9A based on comparisons and analyses of predictive modelling results for the REPRO WPDE experiments; Task 9 of SKB Task Force GWFTS - Increasing the realism in solute transport modelling based on the field experiments REPRO and LTDE-SD

Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Trinchero, P.*; Iraola, A.*; Ebrahimi, H.*; Molinero, J.*; et al.

SKB R-17-10, 153 Pages, 2019/01

The SKB Task Force is an international forum on modeling of groundwater flow and solute transport in fractured rock. The WPDE experiments are matrix diffusion experiments in gneiss performed at the ONKALO underground facility in Finland. Synthetic groundwater containing several conservative and sorbing tracers was injected along a borehole interval. The objective of Task 9A was the predictive modeling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches, participated in this exercise. An important conclusion from this exercise is that the modeling results were very sensitive to the magnitude of dispersion in the borehole opening, which is related to the flow of water. Focusing on the tails of the breakthrough curves, which are more directly related to matrix diffusion and sorption, the results from the different teams were more comparable. The modeling results have also been finally compared to the measured breakthroughs.

Journal Articles

Online chemical adsorption studies of Hg, Tl, and Pb on SiO$$_{2}$$ and Au surfaces in preparation for chemical investigations on Cn, Nh, and Fl at TASCA

Lens, L.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Asai, Masato; Ballof, J.*; Block, M.*; David, H. M.*; Despotopulos, J.*; Di Nitto, A.*; Eberhardt, K.*; et al.

Radiochimica Acta, 106(12), p.949 - 962, 2018/12

 Times Cited Count:2 Percentile:33.17(Chemistry, Inorganic & Nuclear)

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$$_{2}$$ and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO$$_{2}$$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$$_{2}$$ surface at room temperature. On the other hand, the Hg did not adsorb on the SiO$$_{2}$$ surface, but adsorbed on the Au surface. The results demonstrated that the adsorption properties of short-lived Hg, Tl, and Pb could be studied with this setup, and that this method is applicable to the experiment for Cn, Nh, and Fl.

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