Rizaal, M.; Miwa, Shuhei; Suzuki, Eriko; Imoto, Jumpei; Osaka, Masahiko; Goullo, M.*
ACS Omega (Internet), 6(48), p.32695 - 32708, 2021/12
JAEA-Data/Code 2021-003, 25 Pages, 2021/05
Development of technologies to investigate properties of deep geological environment and model development of geological environment have been pursued in "Geoscientific Research" in the Horonobe Underground Research Laboratory (HURL) project. In the fiscal year 2020, to proceed remaining important issues which were deduced from the conclusion of the investigations during the fiscal year 2015-2019, basic data such as groundwater chemistry need to be successively acquired. In the fiscal year 2020, groundwater was sampled from boreholes drilled in the 140 m, 250 m, 350 m gallery in the HURL, and water rings settled in three each vertical shaft, and groundwater chemistries of 41 samples were analyzed. Here, analytical results of groundwater chemistry such as physicochemical parameters, dissolved ions, oxygen and hydrogen isotope ratios, and tritium content, which were obtained in the fiscal year 2020, were reported along with a detailed description of analytical methods.
Toigawa, Tomohiro; Peterman, D. R.*; Meeker, D. S.*; Grimes, T. S.*; Zalupski, P. R.*; Mezyk, S. P.*; Cook, A. R.*; Yamashita, Shinichi*; Kumagai, Yuta; Matsumura, Tatsuro; et al.
Physical Chemistry Chemical Physics, 23(2), p.1343 - 1351, 2021/01
The candidate An(III)/Ln(III) separation ligand hexa--octylnitrilo-triacetamide (HONTA) was irradiated under envisioned SELECT (Solvent Extraction from Liquid waste using Extractants of CHON-type for Transmutation) process conditions using a solvent test loop in conjunction with cobalt-60 gamma irradiation. We demonstrate that HONTA undergoes exponential decay with increasing gamma dose to produce a range of degradation products which have been identified and quantified by HPLC-ESI-MS/MS techniques. The combination of HONTA destruction and degradation product ingrowth, particularly dioctylamine, negatively impacts the extraction and back-extraction of both americium and europium ions. The loss of HONTA was attributed to its reaction with the solvent (-dodecane) radical cation of (HONTA + R) = (7.61 0.82) 10 M s obtained by pulse radiolysis techniques. However, when this ligand is bound to either americium or europium ions, the observed -dodecane radical cation kinetics increase by over an order of magnitude. This large reactivity increase to additional reaction pathways occurring upon metal-ion binding. Lastly nanosecond time-resolved measurements showed that both direct and indirect HONTA radiolysis yielded the short-lived (100 ns) HONTA radical cation as well as a longer-lived (s) HONTA triplet excited state. These HONTA species are important precursors to the suite of HONTA degradation products observed.
Collaborative Laboratories for Advanced Decommissioning Science; Tokyo Institute of Technology*
JAEA-Review 2020-026, 41 Pages, 2020/12
The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2019. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2019, this report summarizes the research results of the "Development of Tailor-Made Adsorbents for Uranium Recovery from Seawater on the Basis of Uranyl Coordination Chemistry". On the basis of deep understanding on uranyl coordination chemistry, we design molecular structures of pentadentate ligands as functional moieties for uranium adsorption from seawater and study coordination chemistry of uranyl ion with those ligands in order to resolve current problems in uranium recovery technology from seawater and to develop novel selective and efficient adsorbents for this purpose.
Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Aosai, Daisuke*; Hara, Naohiro*
JAEA-Data/Code 2020-012, 80 Pages, 2020/10
Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2019. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.
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 vapor species and solids of CsSiO and CsFeSiO 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.
Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Aosai, Daisuke*; Kumamoto, Yoshiharu*; Iwatsuki, Teruki
JAEA-Data/Code 2019-019, 74 Pages, 2020/03
Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2018. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.
Development Group for LWR Advanced Technology
JAEA-Data/Code 2019-017, 59 Pages, 2020/03
ECUME (ffective hemistry database of fission products nder ultiphase raction) is the database for the analyses of FP chemistry which strongly affects all the FP behaviors in a severe accident (SA) of nuclear facility like LWR. ECUME consists of three kinds of datasets: CRK (dataset for hemical eaction inetics), EM (lemental odel set) and TD (hermoynamic dataset). The present version of ECUME is prepared especially for the more accurate evaluation of cesium and iodine distribution in a reactor and release amount into an environment which should be of crucial importance towards the decommissioning of Fukushima Daiichi Nuclear Power Station of Tokyo Electric Power Company Holdings (1F) and the enhancement of LWR safety after the 1F SA.
Miwa, Shuhei; Takase, Gaku; Imoto, Jumpei; Nishioka, Shunichiro; Miyahara, Naoya; Osaka, Masahiko
Journal of Nuclear Science and Technology, 57(3), p.291 - 300, 2020/03
For the evaluation of transport behavior of control material boron in a severe accident of BWR from the viewpoint of chemical effects on cesium and iodine behavior, boron chemistry during transportation in the high temperature region above 400 K was experimentally investigated. The heating tests of boron oxide specimen were conducted using the dedicated experimental apparatus reproducing fission product release and transport in steam atmosphere. Released boron oxide vapor was deposited above 1,000 K by the condensation onto stainless steel. The boron deposits and/or vapors significantly reacted with stainless steel above 1,000 K and formed the stable iron-boron mixed oxide (FeO)BO. These results indicate that released boron from degraded BWR control blade in a severe accident could remain in the high temperature region such as a Reactor Pressure Vessel. Based on these results, it can be said that the existence of boron deposits in the high temperature region would decrease the amount of transported cesium vapors from a Reactor Pressure Vessel due to possible formation of low volatile cesium borate compounds by the reaction of boron deposits with cesium vapors.
Kurata, Masaki; Osaka, Masahiko; Jacquemain, D.*; Barrachin, M.*; Haste, T.*
Advances in Nuclear Fuel Chemistry, p.555 - 625, 2020/00
The importance of fuel chemistry has been revivaled since Fukushima-Daiichi Nuclear Power Station (FDNPS) accident. The inspection and analysis of damaged three units, which had been operated in March 11, 2011, showed large differences in the accident progression sequence for these units, because operators attempted to prevent or mitigate the accident progression of each unit by all means possible. Characteristics of fuel debris are considered to be largely influenced by the difference in the sequence and, hence, deviated from those predicted from prototypic accident scenarios, which had been mainly identified from the analysis of Three Mile Island-2 (TMI-2) accident and the following sim-tests. For the proper improvement of our knowledge on severe accident (SA), including non-prototypic conditions, one has to start improving the phenomenology of fuel/core degradation and fission product (FP) behavior. Advances in the chemistry is the most essential approach. The present review attempts to focus on the recent updates and remaining concerns after the FDNPS accident.
Miwa, Shuhei; Miyahara, Naoya; Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Horiguchi, Naoki; Liu, J.; Miradji, F.; Imoto, Jumpei; Afiqa, B. M.; et al.
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05
We constructed the first version of fission product (FP) chemistry database named ECUME for LWR severe accident. The first 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, and thermodynamic data for CsBO vapor species and solids of CsSiO and CsFeSiO. The ECUME will provide more accurate 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.
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
The photooxidation of aqueous iodide ions (I) at sea surface results in the emission of gaseous iodine molecules (I) 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 (()) and the photooxidative quantum yields (()) of I, in the range of 290-500 nm. Through the investigation of the influence of pH and dissolved oxygen (DO) on (), the subsequent emission rates of I following the photooxidation of I in deionized water solution (pH 5.6, DO 7.8 mg L) and artificial seawater solution (pH 8.0, DO 7.0 mg L) were estimated. A global chemistry-climate model employed herein to assess the I ocean emission on a global scale indicated that the photooxidation of I by solar light can enhance the atmospheric iodine budget by up to 8% over some oceanic regions.
Fukuda, Kenji; Watanabe, Yusuke; Murakami, Hiroaki; Amano, Yuki; Hayashida, Kazuki*; Aosai, Daisuke*; Kumamoto, Yoshiharu*; Iwatsuki, Teruki
JAEA-Data/Code 2018-021, 76 Pages, 2019/03
Japan Atomic Energy Agency has been investigating groundwater chemistry to understand the influence of excavation and maintenance of underground facilities as part of the Mizunami Underground Research Laboratory (MIU) Project in Mizunami, Gifu, Japan. In this report, we compiled data of groundwater chemistry and microbiology obtained at the MIU in the fiscal year 2017. In terms of ensuring traceability of data, basic information (e.g. sampling location, sampling time, sampling method and analytical method) and methodology for quality control are described.
Ishikawa, Jun; Zheng, X.; Shiotsu, Hiroyuki; Sugiyama, Tomoyuki; Maruyama, Yu
Proceedings of Asian Symposium on Risk Assessment and Management 2018 (ASRAM 2018) (USB Flash Drive), 6 Pages, 2018/10
Uchida, Shunsuke*; Hanawa, Satoshi; Naito, Masanori*; Okada, Hidetoshi*; Lister, D. H.*
Corrosion Engineering, Science and Technology, 52(8), p.587 - 595, 2017/10
Based on the relationship among ECP, metal surface conditions, exposure time and other environmental conditions, a model to evaluate the ECP and corrosion rate of steel was developed by coupling a static electrochemical analysis and a dynamic oxide layer growth analysis. Major conclusion obtained on the model are as follows. The effect of HO and O concentrations on ECP were successfully explained as the effects of oxide layer growth. Hysteresis of ECP under changes in water chemistry conditions were successfully explained with the model. Decreases in ECP due to neutron exposure were explained well by radiation-induced diffusion in the oxide layers.
Osaka, Masahiko; Miwa, Shuhei; Nakajima, Kunihisa; Di Lemma, F. G.*; Suzuki, Chikashi; Miyahara, Naoya; Kobata, Masaaki; Okane, Tetsuo; Suzuki, Eriko
JAEA-Review 2016-026, 32 Pages, 2016/12
A fundamental research program on fission product (FP) chemistry has started since 2012 for the purpose of establishment of a FP chemistry database in each region of LWR under severe accident and improvement of FP chemical models based on the database. Research outputs are reflected as fundamental knowledge to both the research and development of decommissioning of Fukushima Daiichi Nuclear Power Station (1F) and enhancement of LWR safety. Four research items have thus been established considering the specific issues of 1F and the priority in the source term research area, as follows: effects of boron (B) release kinetics and thermal-hydraulic conditions on FP behavior, cesium (Cs) chemisorption and reactions with structural materials, enlargement of a thermodynamic and thermophysical properties database for FP compounds and development of experimental and analytical techniques for the reproduction of FP behavior and for direct measurement methods of chemical form of FP compounds. In this report, the research results and progress for the year 2015 are described. The main accomplishment was the installation of a reproductive test facility for FP release and transport behavior. Moreover, basic knowledge about the Cs chemisorption behavior was also obtained. In addition to the four research items, a further research item is being considered for deeper interpretation of FP behavior by the analysis of samples outside of the 1F units.
Kido, Kentaro; Hata, Kuniki; Maruyama, Yu; Nishiyama, Yutaka; Hoshi, Harutaka*
NEA/CSNI/R(2016)5 (Internet), p.204 - 212, 2016/05
Steinegger, P.*; Asai, Masato; Dressler, R.*; Eichler, R.*; Kaneya, Yusuke*; Mitsukai, Akina*; Nagame, Yuichiro; Piguet, D.*; Sato, Tetsuya; Schdel, M.; et al.
Journal of Physical Chemistry C, 120(13), p.7122 - 7132, 2016/04
A new experimental method "vacuum chromatography" has been developed to measure adsorption enthalpy of superheavy elements, and its feasibility has been examined using short-lived thallium isotopes. The short-lived thallium isotopes were produced at the JAEA tandem accelerator. The thallium ion beam prepared with an on-line isotope separator which ionized and mass-separated the thallium isotopes was injected into an isothermal vacuum chromatography apparatus. A temperature-dependent adsorption property of thallium atom on SiO surface were measured. The adsorption enthalpy of thallium was determined to be 158 kJ/mol. The thallium is a homolog of element 113. Thus, the vacuum chromatography developed in this study enables us to perform chemical experiments for short-lived superheavy elements with half-lives of a order of one second.
Secretariat of Symposium on Advanced Photon Research
JAEA-Conf 2016-001, 53 Pages, 2016/03
The 16th Symposium on Advanced Photon Research was held at Kansai Photon Science Institute, Japan Atomic Energy Agency (JAEA-KPSI) in Kizugawa city, Kyoto on October 15 - 16, 2015. This report consists of invited and contributed papers presented at the oral and poster sessions in the Symposium.
Uchida, Shunsuke; Hanawa, Satoshi; Kysela, J.*; Lister, D. H.*
Power Plant Chemistry, 18(1), p.6 - 17, 2016/01
In order to establish reliable NPP operation, each plant requires its own unique optimal water chemistry control based on careful consideration of its system, materials and operational history. Electrochemistry is one of key issues that determine corrosion related problems, e.g., FAC. Based on the relationships among ECP, metal surface conditions and exposure time, a model to evaluate ECP and corrosion rate of steel was developed by coupling an electrochemical model and an oxide layer growth model. Major conclusions are as follows. (1) The effects of water chemistry improvement and mass transfer coefficients due to local flow velocity on FAC wall thinning rate and ECP could be evaluated with the proposed model. (2) The effects of HO and O concentrations on ECP were evaluated with the model. Exposure time dependent ECPs were also explained as the effects of oxide film growth on the specimens. (3) Decreases in ECP due to neutron exposure were explained by radiation-induced diffusion in the oxide layers.