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Journal Articles

Liquid decontamination using acidic electrolyzed water for various uranium-contaminated steel surfaces in dismantled centrifuge

Sakasegawa, Hideo; Nomura, Mitsuo; Sawayama, Kengo; Nakayama, Takuya; Yaita, Yumi*; Yonekawa, Hitoshi*; Kobayashi, Noboru*; Arima, Tatsumi*; Hiyama, Toshiaki*; Murata, Eiichi*

Progress in Nuclear Energy, 153, p.104396_1 - 104396_9, 2022/11

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

When dismantling centrifuges in uranium-enrichment facilities, decontamination techniques must be developed to remove uranium-contaminated surfaces of dismantled parts selectively. Dismantled uranium-contaminated parts can be disposed of as nonradioactive wastes or recycled after decontamination appropriate for clearance. previously, we developed a liquid decontamination technique using acidic electrolyzed water to remove uranium-contaminated surfaces. However, further developments are still needed for its actual application. Dismantled parts have various uranium-contaminated surface features due to varied operational conditions, inhomogeneous decontamination using iodine heptafluoride gas, and changes in long-term storage conditions after dismantling. Here, we performed liquid decontamination on specimens with varying uranium-contaminated surfaces cut from a centrifuge made of low-carbon steel. From the results, the liquid decontamination can effectively remove the uranium-contaminated surfaces, and radioactive concentrations fell below the target value within twenty minutes. Although the required time should also depend on dismantled parts' sizes and shapes in their actual application, we demonstrated that it could be an effective decontamination technique for uranium-contaminated steels of dismantled centrifuges.

JAEA Reports

Development of the desalting method for gross alpha activity determination (Contract research)

Koike, Yuko; Yamada, Ryohei; Nagaoka, Mika; Nakano, Masanao; Ono, Yosuke; Suitsu, Yuichi

JAEA-Technology 2021-011, 39 Pages, 2021/08

JAEA-Technology-2021-011.pdf:1.56MB

In the Analyzed Liquid Treatment Facility of Japan Nuclear Fuel Co., Ltd. (JNFL) MOX Fuel Fabrication Plant (J-MOX), the interfere by salts with the analysis of gross alpha activity concentration analysis will be caused during the treatment process. Therefore, JNFL devised the desalting method using a solid-phase extraction chromatography. Japan Atomic Energy Agency carried out the experimental study to confirm the validity of this desalting method for the treatment liquid based on the contract with JNFL. This study consists of three experiments as follows: Step 1 - Selection of an optical solid-phase extraction agent, Step 2 - Evaluation of variation optical solid-phase extraction agent, and Step 3 - Application of the imitation liquid waste. The result of Step 1 determined the solid-phase extraction agent (InertSep ME-2) and the optimum condition (aspiration method by manifold (about 5-10 mL/min), 3M nitric acid as eluent, pH: 5, and no adjustment of ionic valence). Then, the result of Step 2 and 3 made sure the validation of this method by obtaining over 70% recovery for the imitation liquid waste sample of the Analyzed Liquid Treatment Facility of J-MOX.

Journal Articles

Evaluation of change of LSD spikes by long-term storage

Shibano, Koya; Abe, Katsuo; Tsukasa, Kazuo*; Hosogane, Tatsuya; Kayano, Masashi; Sumi, Mika; Fujiwara, Hideki*; Yamaguchi, Kazuya*; Motoki, Chika*

Dai-41-Kai Nihon Kaku Busshitsu Kanri Gakkai Nenji Taikai Kaigi Rombunshu (Internet), 4 Pages, 2020/11

Large-sized dried spikes, called LSD spike, are used as reference material for accountancy analysis for Plutonium and Uranium by Isotope Dilution Mass Spectrometry. LSD spikes preparation is performed each steps as followed (1) Preparing Plutonium and Uranium mix solution, (2) Aliquoting mix solution to vials, and (3) Drying. J-MOX have planned prepared in-house LSD spike and utilized it for accountancy analysis. If LSD spikes are stored for long term, dried material peel off from bottom of vial and it may affect analytical results. In this study, LSD spikes, which have composition suitable for accountancy analysis in J-MOX, had been stored for about 2 years, then long-term stability of LSD spikes had been evaluated.

Journal Articles

Processes affecting land-surface dynamics of $$^{129}$$I impacted by atmospheric $$^{129}$$I releases from a spent nuclear fuel reprocessing plant

Ota, Masakazu; Terada, Hiroaki; Hasegawa, Hidenao*; Kakiuchi, Hideki*

Science of the Total Environment, 704, p.135319_1 - 135319_15, 2020/02

 Times Cited Count:6 Percentile:30.82(Environmental Sciences)

Land-surface transfers of $$^{129}$$I are modeled and incorporated into a land-surface model (SOLVEG-II), and the model was applied to the observed transfer of $$^{129}$$I at a vegetated field impacted by atmospheric releases of $$^{129}$$I from Rokkasho reprocessing plant during 2007 to investigate the importance of each $$^{129}$$I-transfer pathway. The model calculation revealed that contamination of leaves of wild bamboo grasses was mostly caused by foliar adsorption of $$^{129}$$I (81%) induced via wet deposition of $$^{129}$$I. Wet deposition of $$^{129}$$I was the main $$^{129}$$I-input to the soil, ten-fold the dry deposition of $$^{129}$$I$$_{2}$$; however, the deposition of $$^{129}$$I during 2007 was only 2% of the model-assumed $$^{129}$$I that pre-existed in the soil; indicating the importance of long-term accumulation of $$^{129}$$I in soils. The model calculation also revealed that root uptake of $$^{129}$$I, not methylation, control the long-term turnover of soil $$^{129}$$I.

Journal Articles

Study on decontamination of steel surface contaminated with uranium hexafluoride by acidic electrolytic water

Nakayama, Takuya; Nomura, Mitsuo; Mita, Yutaka; Yonekawa, Hitoshi*; Bunbai, Misako*; Yaita, Yumi*; Murata, Eiichi*; Hosaka, Katsumi*; Sugitsue, Noritake

Proceedings of 2019 International Congress on Advances in Nuclear Power Plants (ICAPP 2019) (Internet), 8 Pages, 2019/05

Clearance of contaminated metal is important for recycling and volume reduction of radioactive waste. Among applicable decontamination technologies, immersion method with ultrasonic cleaning is considered to be effective for metal materials having various shapes. in this study is to demonstrate decontamination of carbon steel contaminated by uranium hexafluoride to the target level for clearance (less than 0.04 Bq/cm$$^{2}$$), and minimize secondary waste. In this test, acidic electrolytic water, dilute hydrochloric acid, dilute sulfuric acid and ozone water with various pH and redox potential were used as decontamination solutions to be tested. We found that acidic electrolytic water is effective solution for decontamination of carbon steel contaminated by uranium hexafluoride. It could be decontaminate less than target level for clearance, and reduced secondary waste relatively.

JAEA Reports

Synchrotron radiation based XAFS analysis of the simulated nuclear waste glass samples prepared by bottom drain test in the full-scale mock-up melter (KMOC) (Contract research)

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Kano, Shigeru; Himeno, Haruyuki*; Kobayashi, Hiroshi*; Nakatani, Mikio*

JAEA-Research 2018-013, 18 Pages, 2019/03

JAEA-Research-2018-013.pdf:1.98MB

The chemical state and local structure of some elements in the simulated nuclear waste glass samples (20 batches) prepared by bottom drain test in the full scale mock-up tests using KMOC melter were investigated by synchrotron radiation based X-ray absorption fine structure (XAFS) analysis. As a result of the analysis of cerium element, it was confirmed that the oxidation proceeds gently as the batch advanced. For manganese, iron, and zinc, there was almost no difference between batches, which seemed to be stabilized by getting into the frame structure of the borosilicate glass. There were no elements that seemed to be clearly crystalline except for platinum group elements. Remarkable precipitation was hardly observed in zirconium and molybdenum with the imaging analysis.

Journal Articles

Release of radioactive materials from high active liquid waste in small-scale hot test for boiling accident in reprocessing plant

Yamane, Yuichi; Amano, Yuki; Tashiro, Shinsuke; Abe, Hitoshi; Uchiyama, Gunzo; Yoshida, Kazuo; Ishikawa, Jun

Journal of Nuclear Science and Technology, 53(6), p.783 - 789, 2016/06

 Times Cited Count:4 Percentile:43.6(Nuclear Science & Technology)

The release behavior of radioactive materials from high active liquid waste (HALW) has been experimentally investigated under boiling accident conditions. In the experiments using HALW obtained through laboratory scale reprocessing, release ratio was measured for the FP nuclides such as Ru, $$^{99}$$Tc, Cs, Sr, Nd, Y, Mo, Rh and actinides such as $$^{242}$$Cm, $$^{241}$$Am. As a result, the release ratio was 0.20 for Ru and 1$$times$$$$10^{-4}$$ for the FP and Ac nuclides. Ru was released into the gas phase in the form of both mist and gas. For its released amount, weak dependency was found to the initial concentration in the test solution. The release ratio decreased with the initial concentration. For other FP nuclides and actinides as non-volatile, released into the gas phase in the form of mist, the released amount increased with the initial concentration. The release ratio of Ru and NOx concentration increased with temperature of the test solutions. They were released almost at the same temperature between 200 and 300$$^{circ}$$C. Size distribution of the mist and other particle was measured.

Journal Articles

Study on the behavior of radiolytically produced hydrogen in a high-level liquid waste tank of a reprocessing plant; Comparison between actual and simulated solutions

Kinuhata, Hiroshi*; Yamamoto, Masahiko; Taguchi, Shigeo; Surugaya, Naoki; Sato, Soichi; Kodama, Takashi*; Tamauchi, Yoshikazu*; Shibata, Yuki*; Anzai, Kiyoshi*; Matsuoka, Shingo*

Nuclear Technology, 192(2), p.155 - 159, 2015/11

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

Experiments using a small-scale apparatus with 30 ml actual high-level liquid waste from the Tokai Reprocessing Plant were carried out to show that the hydrogen concentration in the gas phase reaches a steady-state value of much less than 4% (lower explosive limit) in the absence of sweeping-air. The H$$_{2}$$ concentration reached a steady-state value as was expected and it was compared with a value predicted from an equation with parameters which had been obtained using the simulated solution. Satisfactory agreement showed that the Pd-ion catalytic H$$_{2}$$ consumption reaction previously found in the simulated solution proceeded equally well in the actual solution.

JAEA Reports

Measurement of hydrogen generating from radiolysis of highly active liquid waste and its quantitative evaluation

Yamamoto, Masahiko; Surugaya, Naoki; Mori, Eito; Taguchi, Shigeo; Sato, Soichi

JAEA-Research 2015-013, 27 Pages, 2015/10

JAEA-Research-2015-013.pdf:2.84MB

The H$$_{2}$$ concentration generating from Highly Active Liquid Waste (HALW) of Tokai Reprocessing Plant is measured in a closed experimental system. The experimental results show that H$$_{2}$$ concentration gradually increases at first and then approaches a steady-state due to the H$$_{2}$$ consumption reaction by Pd ions. The highest H$$_{2}$$ concentration is 1200 ppm (0.1%) when the solution temperature is at 23$$^{circ}$$C. It is found that H$$_{2}$$ generating from HALW is equilibrated one order of magnitude lower than the H$$_{2}$$ combustion lower limit. Moreover, a model based on H$$_{2}$$ generation from HALW by the radiolysis and H$$_{2}$$ consumption reaction by Pd ions is proposed and applied to evaluate H$$_{2}$$ concentration behavior in the gas phase. The calculated H$$_{2}$$ concentrations from proposed model agreed well with the experimental values. It is demonstrated that the behavior of H$$_{2}$$ generating from HALW can be evaluated quantitatively by applying the proposed model in this study.

Journal Articles

Experimental study on boiling accident of high active liquid waste in reprocessing

Uchiyama, Gunzo; Tashiro, Shinsuke; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo; Ishikawa, Jun

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1056 - 1063, 2015/09

The experimental study for source term data of radioactive materials has been conducted at a boiling accident of high active liquid waste (HALW) in reprocessing plants. In the study, three kinds of tests have been conducted including a cold small scale test, a cold engineering scale test and a hot small scale test. The following results were obtained: Ruthenium and Technetium were released into the gas phase in the form of both mist and gas under the boiling accident conditions of a simulated HALW. Non-volatile fission products (FPs) such as Nd and Cs were released into the gas phase in the form of mist. The release ratios of non-volatile FPs from a vessel of the simulated HALW were about 10$$^{-4}$$. The release ratios of actinide nuclides such as Am were almost the same as those of non-volatile FPs.

Journal Articles

Chemical composition of insoluble residue generated at the Rokkasho Reprocessing Plant

Yamagishi, Isao; Odakura, Makoto; Ichige, Yoshiaki; Kuroha, Mitsuhiko; Takano, Masahide; Akabori, Mitsuo; Yoshioka, Masahiro*

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1113 - 1119, 2015/09

The characteristics of insoluble residues in fine suspension at the Rokkasho Reprocessing Plant were analyzed. The insoluble residues were washed with oxalic acid solution to dissolve zirconium molybdate residues. XRD profiles of unwashed residues showed the presence of a noble metal alloy, zirconium molybdate, and zirconia, but zirconium molybdate was not found after washing. More than 50% of the Sb-125 and Pu in thee residues was washed out as well. The noble metal alloy composed of Mo, Tc, Ru, Rh, and Pd occupied more than 90% of the total weight of 12 elements (Ca, Cr, Fe, Ni, Zr, Mo, Tc, Ru, Rh, Pd, Te, and U) found in the residues. In consideration of the chemical forms of 12 elements, the alloy-to-residue weight ratio was evaluated to be 64% and 78% with and without 18% of an unknown component, respectively.

Journal Articles

Investigation into cause of increasing count rate on PIMS at RRP, 1; Search of potential causes

Mukai, Yasunobu; Nakamura, Hironobu; Nakamichi, Hideo; Kurita, Tsutomu; Noguchi, Yoshihiko*; Tamura, Takayuki*; Ikegame, Ko*; Shimizu, Junji*

Proceedings of INMM 56th Annual Meeting (Internet), 9 Pages, 2015/07

The PIMS used at Rokkasho Reprocessing Plant can quantify plutonium amount in each process vessel located inside glovebox by means of neutron measurement. Since the PIMS is not used for the neutron coincidence counting, it is very important to maintain that those constants meet the actual process condition. PIMS was calibrated in 2006, and then JNFL has been started to measure the Pu amount directly in each glovebox for the purpose of facility NMA. However, it was found that PIMS counting was unexpectedly and continuously increased during long time of inter-campaign. In order to find out the main cause, JAEA and JNFL jointly conducted several investigations. In the investigations, correctness of system parameters and relevant constants, behavior of the neutron generation when MOX powder is stored in actual glovebox for a long time (to see O/M and moisture change) and the behavior focused on the relation between MOX powder and light element using inside glovebox (fluorine is included in the PTFE which is used in many gloveboxes as packing of instruments) were experimentally confirmed using MOX powder in PCDF. As a result, since the same behavior happened in the actual PIMS was confirmed in the testing environment in which MOX powder coexists with fluorine, it is concluded that the main potential cause of PIMS is the increasing of the probability of ($$alpha$$, $$n$$) reactions by a contact between PTFE and MOX powder.

Journal Articles

Trends of nitrogen oxide release during thermal decomposition of nitrates in highly active liquid waste

Amano, Yuki; Watanabe, Koji; Tashiro, Shinsuke; Yamane, Yuichi; Ishikawa, Jun; Yoshida, Kazuo; Uchiyama, Gunzo; Abe, Hitoshi

Nihon Genshiryoku Gakkai Wabun Rombunshi, 14(2), p.86 - 94, 2015/06

Radioactive materials could be released into air due to the accidental boiling of high active liquid waste (HALW) in reprocessing plants. Volatile radioactive nuclides, such as ruthenium, are released from the tanks into the atmosphere. Nitrogen oxides (NOx) are also released due to the thermal decomposition of metal nitrates in HALW. The released NOx transport volatile ruthenium and cause redox reactions associated with the composition or decomposition of volatile ruthenium. In this study, NOx release data were obtained by heating simulated HALW up to 600$$^{circ}$$C. As a result, the release of NOx from the simulated HALW was observed from 200$$^{circ}$$C to 600$$^{circ}$$C, and the main release of NOx was observed at about 340$$^{circ}$$C. All the lanthanide nitrates were found to decompose in the simulated HALW, and the thermal decomposition temperature of the lanthanide nitrates decreased after the addition of ruthenium dioxide to the mixed lanthanide nitrates solution.

Journal Articles

Release behavior of radioactive materials at a boiling accident of high active liquid waste in reprocessing plants

Uchiyama, Gunzo; Tashiro, Shinsuke; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo; Ishikawa, Jun

Proceedings of International Waste Management Symposia 2014 (WM2014) (Internet), 9 Pages, 2014/05

The experimental study for source term data of radioactive materials has been conducted at a boiling accident of high active liquid waste (HALW) in a reprocessing plant. In the small scale cold test using a non-radioactive simulated HALW, the release behavior of FP elements from the simulated HALW were investigated under various boiling accident conditions. In the engineering scale cold test, the release behavior of FP elements at boiling accident conditions was investigated mainly as a spatial function. In the small scale hot test using a radioactive simulated HALW, the release behavior of radioactive materials (FP, alpha nuclides) were obtained under typical boiling accident conditions. In the small scale hot test, the release fractions of Ru and non-volatile FPs obtained were almost the same as those of the small scale cold test.

Journal Articles

Study on release and transport of aerial radioactive materials in reprocessing plant

Amano, Yuki; Tashiro, Shinsuke; Uchiyama, Gunzo; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo

Proceedings of International Nuclear Fuel Cycle Conference; Nuclear Energy at a Crossroads (GLOBAL 2013) (CD-ROM), p.1411 - 1417, 2013/09

Journal Articles

High-temperature X-ray imaging study of simulated high-level waste glass melt

Okamoto, Yoshihiro; Nakada, Masami; Akabori, Mitsuo; Komamine, Satoshi*; Fukui, Toshiki*; Ochi, Eiji*; Nitani, Hiroaki*; Nomura, Masaharu*

Denki Kagaku Oyobi Kogyo Butsuri Kagaku, 81(7), p.543 - 546, 2013/07

 Times Cited Count:6 Percentile:18.03(Electrochemistry)

The molten state of simulated high-level waste glass and the behavior of ruthenium element in the melt were investigated by using synchrotron radiation based X-ray imaging technique. Melting, generating and moving of bubbles, condensation and sedimentation of ruthenium element were observed dynamically in continuous 12-bit gray-scale images from the CCD camera. X-ray intensity was obtained easily by digitizing gray-scale values in the image. The existence of ruthenium element is emphasized as a black color in the CCD image at X-ray energy higher than the Ru K-absorption edge. Position sensitive imaging X-ray absorption fine structure (XAFS) measurement was also performed to clarify the chemical state of ruthenium element in the melt.

Journal Articles

Stress corrosion cracking behavior of zirconium in boiling nitric acid solutions at oxide formation potentials

Ishijima, Yasuhiro; Kato, Chiaki; Motooka, Takafumi; Yamamoto, Masahiro; Kano, Yoichi*; Ebina, Tetsunari*

Materials Transactions, 54(6), p.1001 - 1005, 2013/06

 Times Cited Count:7 Percentile:39.58(Materials Science, Multidisciplinary)

Zirconium has been utilized in nuclear fuel reprocessing plants because of its superior corrosion resistance in nitric acid solutions. However, stress corrosion cracking (SCC) susceptibility of zirconium has been reported in boiling nitric acid solutions at the passivity breakdown potential. However, it has not been clear the SCC initiation and propagation behavior of zirconium. In this study, to clarify the SCC initiation and propagation behavior of zirconium, constant load tensile tests were carried out in boiling nitric acid solutions. From the results, many cracks were initiated under the oxide film and maximum crack led to rupture in the potentials that nobler than passivity breakdown potential. These results showed that the SCC of zirconium in boiling nitric acid solutions is due to the oxide formation. And this SCC behavior suggests that the SCC behavior of zirconium can be attributed to tarnish rupture model.

Journal Articles

High-temperature X-ray imaging study of simulated high-level waste glass melt

Okamoto, Yoshihiro; Nakada, Masami; Akabori, Mitsuo; Komamine, Satoshi*; Fukui, Toshiki*; Ochi, Eiji*; Nitani, Hiroaki*; Nomura, Masaharu*

Proceedings of 4th Asian Conference on Molten Salt Chemistry and Technology & 44th Symposium on Molten Salt Chemistry, Japan, p.47 - 52, 2012/09

The molten state of the simulated high-level waste glass and the behavior of ruthenium element in the melt were investigated by using synchrotron radiation based X-ray imaging technique. Melting, generating and moving of bubbles, condensation and sedimentation of ruthenium element were observed dynamically in continuous 12-bit gray-scale images from the CCD camera. The existence of ruthenium in the X-ray CCD image was emphasized over the energy of Ru K-absorption edge. X-ray intensity was obtained easily by digitalizing gray-scale values in the image. Position sensitive imaging X-ray absorption fine structure (XAFS) measurement was performed to clarify the chemical state of ruthenium element in the melt.

Journal Articles

Synchrotron radiation-based X-ray imaging study of ruthenium in simulated high-level waste glass

Okamoto, Yoshihiro; Nakada, Masami; Akabori, Mitsuo; Shiwaku, Hideaki; Komamine, Satoshi*; Fukui, Toshiki*; Ochi, Eiji*; Nitani, Hiroaki*; Nomura, Masaharu*

Nihon Genshiryoku Gakkai Wabun Rombunshi, 11(2), p.127 - 132, 2012/06

Distribution and the chemical state of Ru element in the simulated high-level waste glass were examined by using the synchrotron radiation based X-ray imaging technique. In this technique, a direct X-ray CCD camera is used in place of an ion chamber. Position sensitive X-ray absorption spectra were obtained by analyzing gray scale in images of the X-ray CCD camera. At first, we measured a test sample containing RuO$$_2$$ and Ru metal powder. We successfully obtained information on the Ru distribution in the sample. In addition, the chemical state (oxide or metal ?) of each small Ru-rich spot was evaluated by the corresponding position sensitive XAFS spectrum. The imaging XAFS technique was applied to some simulated high-level waste glass samples. The Ru distribution of the glass sample and their chemical state were confirmed by image analyses. It can be seen that Ru element scattered in the glass sample exists as oxide RuO$$_2$$.

Journal Articles

Development for advanced solution monitoring and measurement system (ASMS)

Mukai, Yasunobu; Nakamura, Hironobu; Yoshimoto, Katsunobu; Tamura, Takayuki*; Iwamoto, Tomonori*

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-32-Kai Nenji Taikai Rombunshu (Internet), 9 Pages, 2011/11

JNFL and JAEA are collaboratively developing an advanced solution monitoring and measurement system (ASMS) that is direct Pu measurement NDA system in the solution tank containing plutonium nitrate solution for the improvement of current safeguards subjects to be solved, and for next generation safeguards instrument. The target measurement uncertainty of ASMS is set less than 6% that is equivalent to detection level of partial defect at interim inventory verification by NDA. The ASMS detector was designed based on MCNPX calculation, and then manufactured. As an actual test, the detector was set in a process tank at Plutonium Conversion Development Facility, the calibration tests (known-alpha) for quantitative measurement was conducted. As a result, the total measurement uncertainty for Pu mass is about 3.4% except for the low liquid height region that is satisfied the target value. In addition, the monitoring capability of ASMS was confirmed.

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