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Miura, Takatomo; Kudo, Atsunari; Koyama, Daisuke; Obu, Tomoyuki; Samoto, Hirotaka
Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 10 Pages, 2023/10
Tokai Reprocessing Plant (TRP) had reprocessed 1,140 tons of spent fuel discharged from commercial reactors (BWR, PWR) and Advanced Thermal Reactor "Fugen" from 1977 to 2007. TRP had entered decommissioning stage in 2018. In order to reduce the risk of High Active Liquid Waste (HALW) held at the facility, the vitrification of HALW is given top priority. HALW generated from reprocessing of spent fuel contains not only fission products (FPs) but also trace amounts of uranium (U) and plutonium (Pu) within the liquid and insoluble residues (sludge). Under normal conditions, concentrations of U and Pu in HALW are very low so that it can not reach criticality. Since FPs with high neutron absorption effect coexists in HALW, even if the cooling function is lost due to serious accident and HALW evaporates to dryness, it is considered that criticality would not been reached. In order to confirm this estimation quantitatively, criticality safety evaluations were carried out for the increase of U and Pu concentrations by evaporation of HALW to the point of dryness. In this evaluation, infinite multiplication factors were calculated for each of solution system and sludge system of HALW with respect to the concentration change through evaporation to dryness. It is confirmed it could not reach criticality. The abundance ratios of U, Pu and FPs were set conservatively based on analytical data and ORIGEN calculation results. Multiplation factors for two-layer infinite slab model of solution and sludge systems of HALW were also calculated, and it was confirmed it could not reached criticality. In conclusion, the result was gaind that there could be no criticality even in the process through evaporation to dryness of HALW in TRP.
Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*
JAEA-Research 2023-001, 26 Pages, 2023/05
JAEA-Research-2023-001.pdf:1.61MB
An accident of evaporation to dryness by boiling of high-level radioactive liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into the atmosphere. Accurate quantitative estimation of released Ru is one of the important issues for risk assessment of those facilities. To resolve this issue, an analytical approach has been developed using computer simulation programs to assess the radioactive source term from those facilities. The proposed approach consists analyses with three computer programs. At first, the simulation of boiling behavior in the HLLW tank is conducted with SHAWED code. Next step, the thermal-hydraulic behavior in the facility building is simulated with MELCOR code based on the results at the first step simulation such as flowed out mixed steam flow rate, temperature and volatilized Ru from the tank. The final analysis step is carried out for estimating amount of released radioactive materials with SCHERN computer code which simulates chemical behaviors of nitric acid, nitrogen oxide and Ru based on the condition also simulated MELCOR. Series of sample simulations of the accident at a hypothetical typical facility are presented with the data transfer between those codes in this report.
Horita, Takuma; Yamagishi, Isao; Nagaishi, Ryuji; Kashiwaya, Ryunosuke*
JAEA-Technology 2021-012, 34 Pages, 2021/07
JAEA-Technology-2021-012.pdf:2.1MBJAEA-Technology-2021-012(errata).pdf:0.18MB
Waste mainly consisting of carbonate precipitates (carbonate slurry) from the Advanced Liquid Processing System (ALPS) and the improved ALPS at the Fukushima Daiichi Nuclear Power Station of Tokyo Electric Power Holdings, Inc. have been storing in the High Integrity Container (HIC). The supernatant solution of carbonate slurry contained in some of HICs were overflowed in April of 2015. The all of level of liquid in the HICs were investigated; however, almost of the HICs were under the level of overflow. The mechanism of overflow suggested to be depending on the difference of the properties of the carbonate slurry such as the retention/release characteristics of the bubbles. Therefore, in order to clarify the mechanism of leakage, the repeatability experiment was carried out by using simulated carbonate slurry. The simulated carbonate slurry was perpetrated by using the same cross-flow filter system of the actual ALPS. Moreover, the preparative conditions for the simulated carbonate slurry were the same as Mg/Ca concentration ratio in inlet water of the ALPS (raw water) and the ALPS operating conditions. The chemical characteristics of simulated carbonate slurries were revealed by ICP-AES, pH meter, etc. The density of the settled slurry layer tended to increase depending on the calcium concentration in the raw water. The bubble injection test was conducted in order to investigate the bubble retention/release behavior in the simulated carbonate slurry layer. The simulated carbonate slurry with high settling density, which was generated by high calcium concentration solution was revealed to retain the injected bubbles. Since the ratio of concentration calcium and magnesium during the carbonate slurry generation is assumed to affect the retention of bubbles in the slurry layer, the information on the composition of raw water is one of important factor for overflow of HICs.
Igarashi, Hiroshi
JAEA-Review 2020-006, 261 Pages, 2020/09
JAEA-Review-2020-006.pdf:4.42MB
A literature review was conducted on the increase in surface area of vitrified products of HLW due to the fracturing caused by cooling during glass pouring process and by mechanical impact, from the perspective of a parameter of the radionuclide release model in the performance assessment of geological disposal system studied overseas. The review was focused on the value of surface area increase factor set as a parameter in the model, the experimental work to evaluate an increase in surface area, and how the parameters on surface area were determined based on the experimental results. The surface area obtained from the experiments executed in Japan was also discussed in comparison with the overseas studies. On the basis of the investigation, the effects of various conditions on the surface area were studied, such as a diameter of vitrified product, cooling condition during and after the glass pouring, impact on vitrified products during their handling, environment after the closure of disposal facility, and others. The causes of fracturing are associated with the phenomena or events in the waste management process such as production, transport, storage, and disposal. The surface area increase factors set in the nuclide release model of the glass and their bases were reviewed. In addition, the measured values and the experimental methods for surface increase factors published so far were compared. Accordingly, the methods for measuring surface area as the bases were identified for these factors set in the models. The causes of fracturing and features of these factors were studied with respect to the relation with the waste management process. The results from the review and assessment can contribute to the expanding the knowledge for the conservative and realistic application of these factors to performance assessment, and to the developing and upgrading of safety case as a consequence.
Yamamoto, Masahiko; Do, V. K.; Taguchi, Shigeo; Kuno, Takehiko; Takamura, Yuzuru*
Spectrochimica Acta, Part B, 155, p.134 - 140, 2019/05
Times Cited Count：5 Percentile：41.46(Spectroscopy)The emission spectra of technetium (Tc) by liquid electrode plasma optical emission spectrometry have been investigated in this study. From the spectra, 52 emission peaks of Tc were observed in the 250-500 nm wavelength range. All peaks were assigned to the neutral state or singly ionized state. The relative intensities of these peaks were similar to those excited by an electric spark. The strongest intensity peaks were found at 254.3 nm, 261.0 nm, and 264.7 nm. Spectral interferences of coexisting elements in highly active liquid waste of reprocessing stream on those three strongest peaks were investigated using simulated sample. No spectral interferences were observed around the 264.7 nm Tc peak. Therefore, analytical performance using 264.7 nm peak was evaluated. The detection limit, estimated on standard and blank samples in 0.4 M nitric acid, was 1.9 mg/L. The relative standard deviation of Tc standard sample (12.0 mg/L) was 3.8% (N = 5, 1
).
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Takamura, Yuzuru*; Surugaya, Naoki; Kuno, Takehiko
Talanta, 183, p.283 - 289, 2018/06
Times Cited Count：10 Percentile：39.09(Chemistry, Analytical)We develop a novel analytical method employing liquid electrode plasma optical emission spectrometry for measurement of total cesium in highly active liquid wastes. Limit of detection and limit of quantification are 0.005 mg/L and 0.02 mg/L, respectively. The method is validated and applied to the real samples.
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：6 Percentile：43.12(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, 
Tc, Cs, Sr, Nd, Y, Mo, Rh and actinides such as 
Cm, 
Am. As a result, the release ratio was 0.20 for Ru and 1
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
C. Size distribution of the mist and other particle was measured.
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
. The release ratios of actinide nuclides such as Am were almost the same as those of non-volatile FPs.
Tashiro, Shinsuke; Uchiyama, Gunzo; Amano, Yuki; Abe, Hitoshi; Yamane, Yuichi; Yoshida, Kazuo
Nuclear Technology, 190(2), p.207 - 213, 2015/05
Times Cited Count：8 Percentile：51.03(Nuclear Science & Technology)The release behavior of radioactive materials from high active liquid waste (HALW) has been investigated under boiling accident conditions. Results of the experiment using a nonradioactive simulated HALW found Ru to be a volatile element under the accident conditions and to be released into the gas phase in the form of both mist and gas. The Ru release rate and the apparent Ru volatilization rate constant were obtained under the boiling conditions of simulated HALW. The other fission product elements such as Cs were found to be nonvolatile and to be released into the gasphase in the form of mist. The mist size distribution near the surface of the simulated HALW in the reactor vessel was found to range from 0.05 to 20 
m with a peak diameter of 
2 m.
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Kuno, Takehiko; Surugaya, Naoki; Takamura, Yuzuru*
no journal, ,
Commercial ICP AES is often applied for analysis of radioactive nuclides present in the waste stream. However, the instrument is bulky with auxiliary equipment. Consequently, it is difficult to maintain or replace those instruments in a shielded cell or a glove box. A novel liquid electrode plasma (LEP) would be a suitable option instead of ICP. LEP is compact to be easily installed, maintained and operated in a shielded cell or a glove box because the method does not require plasma gas, a nebulizer or large power supply. LEP allows only L-level waste emission due to the use of microchannel. In the study, we utilized LEP as an excitation source for analysis of radioactive nuclides. The newly installed instrument was characterized by determining cesium and strontium in a highly active waste simulated sample. The obtained result is promising for further application of LEP in the field of radiochemical analysis.
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Inada, Satoshi; Takamura, Yuzuru*; Kuno, Takehiko
no journal, ,
A simple and rapid method for determination of Cs and Tc in highly radioactive liquid waste (HALW) using liquid electrode plasma (LEP) has been developed. Effects of pulsed voltage sequence and nitric acid concentration on emissions of these elements are investigated. The method is applied to the quantitative analysis of Cs and Tc in HALW samples at Tokai reprocessing plant.
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Takamura, Yuzuru*; Kuno, Takehiko
no journal, ,
We report a new analytical method for determination of strontium in highly active liquid waste, which employs liquid electrode plasma optical emission spectrometry (LEP-OES) following online solid phase extraction (SPE). The homemade SPE column is constructed by packing Sr selective resin into a 30-cm long resin tube, which can be reused for tens of times. Preconcentration factor is estimated about 15. Total time for one measurement is 1.5 hours. The developed method is validated with the measurement of simulated HALW. We suppose that the method is able to measure 10000-fold diluted HALW with a volume of 5 mL.
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo; Inada, Satoshi; Takamura, Yuzuru*; Kuno, Takehiko
no journal, ,
An analytical technique for determination of elemental strontium in highly radioactive liquid waste (HALW) using liquid electrode plasma optical emission spectrometry (LEP-OES) has been developed. We use the LEP-OES instrument that is installed recently. Measurement condition including voltage and sample acidity is optimized. The method is validated using simulated HALW and comparing with inductively coupled plasma spectrometry (ICP-OES). The measurement of real HALW is being carried out.
Do, V. K.; Yamamoto, Masahiko; Taguchi, Shigeo*; Kuno, Takehiko; Sato, Soichi; Takamura, Yuzuru*
no journal, ,
Inductively coupled plasma optical emission spectrometry (ICP-OES) is widely considered as a routine elemental analytical method. However, the necessity of cooling system and plasma gas makes the method difficult in maintenance and repair once it is installed in a glove box for analysis of radioactive samples. Our study is applying liquid electrode plasma optical emission spectrometry (LEP-OES), which requires no plasma gas, nor cooling system, to highly active liquid wastes (HALW). The applications of the method for Cs, Sr, Na, K, Tc has been examined and reported in this presentation.
