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Horita, Takuma; Yamagishi, Isao; Nagaishi, Ryuji; Kashiwaya, Ryunosuke*
JAEA-Technology 2021-012, 34 Pages, 2021/07
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.
Horita, Takuma; Asai, Shiho*; Konda, Miki; Matsueda, Makoto; Hanzawa, Yukiko; Kitatsuji, Yoshihiro
Bunseki Kagaku, 69(10/11), p.619 - 626, 2020/10
Times Cited Count:0 Percentile:0(Chemistry, Analytical)We have developed a Sr adsorption fiber for rapid analysis of Sr. The prepared Sr adsorption fiber has a Sr-extraction layer that densely retains a Sr-selective extractant, an 18-crown-6 ether derivative, on the fiber surface. Hydrophobic group-containing polymer chains embedded onto the surface of the fiber allow to form a hydrophobic phase, incorporating Sr-selective extractants. This unique surface structure provides high adsorption capacity, leading to rapid and highly efficient adsorption of Sr
. The adsorption capacity of the Sr adsorption fiber was 3 times higher than commercially available 18-crown-6 ether derivative-impregnated resin (Sr Resin). The equilibrium adsorption capacity of the Sr adsorption fiber was comparable to the Sr Resin. The retained
Sr was finally determined by a GM counter. The total analysis time including the Sr adsorption and measurement was about 1 hour.
Asai, Shiho*; Ohata, Masaki*; Hanzawa, Yukiko; Horita, Takuma; Yomogida, Takumi; Kitatsuji, Yoshihiro
Analytical Chemistry, 92(4), p.3276 - 3284, 2020/02
Times Cited Count:4 Percentile:32.41(Chemistry, Analytical)The long-term safety assessment of spent Cs adsorbents produced during the decontamination of radiocesium-containing water at the Fukushima Daiichi Nuclear Power Plant requires one to estimate their Cs content prior to final disposal.
Cs is usually quantified by inductively coupled plasma mass spectrometry (ICP-MS), which necessitates the elution of Cs from Cs adsorbents. However, this approach suffers from the high radiation dose from
Cs. To address this challenge, we herein employed laser ablation ICP-MS for direct quantitation of
Cs in Cs adsorbents and used a model Cs adsorbent prepared by immersion of a commercially available Cs adsorbent into radiocesium-containing liquid waste to verify the developed technique. The use of the
Cs/
Cs ratio and
Cs radioactivity obtained by gamma spectrometry achieved simple and precise quantitation of
Cs and the resulting
Cs activity of 0.36 Bq agreed well with that in the original radiocesium-containing liquid waste.
Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
Analytical and Bioanalytical Chemistry, 411(5), p.973 - 983, 2019/02
Times Cited Count:9 Percentile:61.32(Biochemical Research Methods)Determination of radiopalladium Pd is required for ensuring the radiation safety of Pd extracted from spent nuclear fuel for recycling or disposal. We employed laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to simplify an analytical procedure of
Pd. Pd was separated through selective Pd precipitation reaction from spent nuclear fuel. Laser ablation allows direct measurement of the Pd precipitates, skipping the dissolution and dilution procedure. In this study,
Pd in natural Pd standard solution was used as an internal standard, taking advantage of its absence in spent nuclear fuel. The Pd precipitate was uniformly embedded on the surface of the centrifugal filter, forming a microscopically thin flat surface of Pd. The resulting homogeneous Pd layer is suitable for obtaining a stable signal ratio of
Pd/
Pd. The amount of
Pd obtained by LA-ICP-MS corresponds to the values obtained by conventional solution nebulization measurement.
Yomogida, Takumi; Asai, Shiho; Saeki, Morihisa*; Hanzawa, Yukiko; Horita, Takuma; Esaka, Fumitaka; Oba, Hironori*; Kitatsuji, Yoshihiro
Bunseki Kagaku, 66(9), p.647 - 652, 2017/09
Times Cited Count:2 Percentile:7.92(Chemistry, Analytical)Palladium-107 is a long-lived fission product, which can be found in high-level radioactive liquid wastes (HLLW). Determination of the Pd contents in HLLW is essential to evaluate the long-term safety of HLLW repositories. However, the
Pd content in HLLW has not been reported because of difficulties in pretreatment for the measurement. In this study, we investigated applicability of laser-induced photoreduction to HLLW solution: it enables a simple and non-contact separation of Pd. The results showed the recovery of 60% was achieved at the conditions: 40% ethanol, 20 min irradiation, 100 mJ of pulse energy. Additionally, major radionuclides and potentially interfering components in ICP-MS were removed from the simulated HLLW over a wide concentration range of Pd from 0.24 to 24 mg L
, showing the applicability of the proposed separation technique to HLLW samples.
Segawa, Yukari; Horita, Takuma; Kitatsuji, Yoshihiro; Kumagai, Yuta; Aoyagi, Noboru; Nakada, Masami; Otobe, Haruyoshi; Tamura, Yukito*; Okamoto, Hisato; Otomo, Takashi; et al.
JAEA-Technology 2016-039, 64 Pages, 2017/03
The laboratory building No.1 for the plutonium research program (Bldg. Pu1) was chosen as one of the facilities to decommission by Japan Atomic Energy Agency Reform in September, 2013. The research groups, users of Bldg. Pu1, were driven by necessity to remove used equipment and transport nuclear fuel to other facilities from Bldg. Pu1. Research Group for Radiochemistry proactively established the Used Equipment Removal Team for the smooth operation of the removal in April, 2015. The team classified six types of work into the nature of the operation, removal of used equipment, disposal of chemicals, stabilization of mercury, stabilization of nuclear fuel, transportation of nuclear fuel and radioisotope, and survey of contamination status inside the glove boxes. These works were completed in December, 2015. This report circumstantially shows six works process, with the exception of the approval of the changes on the usage of nuclear fuel in Bldg. Pu1 to help prospective decommission.
Horita, Takuma; Asai, Shiho; Konda, Miki; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Sugo, Takanobu*; Kitatsuji, Yoshihiro
Bunseki Kagaku, 66(3), p.189 - 193, 2017/03
Times Cited Count:1 Percentile:3.87(Chemistry, Analytical)A Sr-selective adsorption fiber was prepared for rapid analysis of Sr content by using radiation-induced emulsion graft polymerization and subsequent chemical modification. A polyethylene fiber with a diameter of 13
m was first immersed in a methanol solution of an epoxy-group-containing vinyl monomer, glycidyl methacrylate (GMA), and polyoxyethylene sorbitol ester (Tween20) as a surfactant for graft-polymerization of GMA. Octadecylamine was then bound to a polymer chain extending from the fiber surface providing hydrophobicity to the polymer chain. Dicyclohexano-18-crown-6 (DCH18C6) was finally impregnated onto the polymer chain via a hydrophobic interaction between the octadecyl moiety of the polymer chain and the cyclohexyl moiety of DCH18C6. The fiber surface structure, characterized by DCH18C6 molecules loosely entangled with polymer chains, afforded realizes the rapid and selective adsorption of Sr ions with an adsorption rate approximately 100 times higher than that of a commercially available Sr-selective resin (Sr Resin).
Asai, Shiho; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
Analytical Chemistry, 88(24), p.12227 - 12233, 2016/12
Times Cited Count:15 Percentile:55.16(Chemistry, Analytical)Safety evaluation of a radioactive waste repository requires credible activity estimates confirmed by actual measurements. A long-lived radionuclide, Pd, which can be found in radioactive wastes, is one of the difficult-to-measure nuclides and results in a deficit in experimentally determined contents. In this study, a precipitation-based separation method has been developed for the determination of
Pd with ICP-MS. The photoreduction induced by laser irradiation at 355 nm provides short-time and one-step recovery of Pd. The proposed method was verified by applying it to a spent nuclear fuel sample. In order to efficiently recover Pd, a natural Pd standard was employed as the Pd carrier. The chemical yield of Pd was about 90% with virtually no impurities, allowing accurate quantification of
Pd.
Horita, Takuma; Asai, Shiho; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Sugo, Takanobu*; Kitatsuji, Yoshihiro
no journal, ,
There has been an increasing demand for rapid analysis of Sr to ensure a prompt action against the contaminated water in the Fukushima Daiichi NPP. Precedent works demonstrated that Cs adsorption fibers prepared by utilizing graft polymerization technology achieved high-speed removal of
Cs in the contaminated water. In this study, we have investigated the applicability of such proven technology to the preparation of a Sr adsorption fiber specialized for the selective extraction of Sr. In the prepared fiber, an extractant for Sr
,dicyclohexano-18-crown-6-ether (DCH18C6) was impregnated via hydrophobic interaction between DCH18C6 and the hydrophobic polymer chains attached onto the surface of the fiber. To increase the adsorption capacity, emulsion graft polymerization which promotes the polymer chains to grow longer was applied. The densely-packed DCH18C6 inside the interfacial phase formed by the polymer chains facilitates the efficient adsorption. The amounts of Sr adsorbed is comparable to those of conventional adsorbents, indicating that the prepared fiber has a feasible performance for Sr adsorption.
Horita, Takuma; Asai, Shiho; Konda, Miki; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Sugo, Takanobu*; Kitatsuji, Yoshihiro
no journal, ,
High activity concentrations of Sr, which greatly exceed the regulatory limit (30 Bq/L), are detected in contaminated waters sampled in Fukushima Daiichi NPP. However, analytical method for
Sr associated with time-consuming procedure causes delay in understanding the current status of
Sr contamination. In this study, we have prepared a Sr adsorption fiber (Sr Fiber) based on radiation-induced graft polymerization technique to achieve a rapid adsorption of Sr ions. Dicyclohexano-18-crown-6 ether that has high affinity for Sr was impregnated in the hydrophobic interfacial phase provided by hydrophobic polymer chains attached on the fiber surface through graft polymerization. The time required to reach the Sr adsorption equilibrium for the Sr Fiber is approximately 180 times shorter than that for a commercially available Sr adsorbent (Sr Resin), showing that the Sr Fiber has a potential to efficiently reduce the analytical time of
Sr.
Asai, Shiho; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
no journal, ,
Pd is a long-lived radionuclide that can be found in HLW. The estimation of the amount of
Pd in HLW is considered crucial for long-term safety evaluation of HLW. However, experimentally determined concentrations of
Pd in HLW has not been reported due to the difficulty in recovering significant amount of Pd from HLW which has high radioactivity. In this study, we have focused on remotely operated separation technique based on laser-induced photoreduction, which allows to keep the distance from samples. To validate the applicability of the proposed method, spent nuclear fuel with a traceable irradiation history was employed instead of HLW. The resulting Pd precipitate contained almost no impurities, such as actinides (U, Np, Pu, Am, Cm), major fission products (Zr, Mo, Tc, Ru, Rh, Ba, Cs, Ce), resulting in the interference-free measurement of
Pd with ICP-MS. The amount of
Pd per 1 mg of
U in the sample was 239
9 ng/mg-
U.
Horita, Takuma; Asai, Shiho; Konda, Miki; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Kitatsuji, Yoshihiro
no journal, ,
There has been an increasing importance of the development of rapid separation techniques for Sr analysis, responding to needs in Fukushima Daiichi NPP. However, conventional
Sr analytical methods require two different separation steps for Sr and Y, respectively, resulting in a long processing time of about one month. In this study, we prepared a Sr adsorptive fiber (Sr fiber) that has a high density Sr adsorption phase on its surface, allowing to highly efficient
-ray counting by minimizing the self-attenuation effects. The adsorption capacity of the prepared Sr fiber was about 14 g/mol, which is equivalent to that of a commercially available Sr adsorptive resin (Sr Resin). The selectivity of the Sr fiber was nearly the same as that of the Sr resin. Considering that the Sr fiber has a specific surface area 1000 times smaller than that of the Sr Resin, the Sr ions can be concentrated to 1000 times on its surface, capable of achieving highly-efficient
-ray counting. From these result, we confirmed that Sr fiber has adsorption capacity and selectivity necessary for highly efficient
-ray counting of
Sr.
Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
no journal, ,
Yomogida, Takumi; Asai, Shiho; Saeki, Morihisa*; Hanzawa, Yukiko; Horita, Takuma; Esaka, Fumitaka; Oba, Hironori*; Kitatsuji, Yoshihiro
no journal, ,
Recently, we developed a precipitation-based separation method for the determination of Pd with ICP-MS. However, a pulsed-laser light source is indispensable to form Pd precipitation in the separation method. There were difficulties in handling of a pulsed-laser light source. Simplified irradiation procedure is desirable to facilitate a Pd separation procedure. In this study, we developed a simple Pd separation technique based on photoreduction with Xe lamp irradiation and applied the technique to a simulated HLW solution. The Pd recovery from a simulated HLW solution reached 50%, while 99% of the other 13 elements were removed. These results indicate that selective separation of Pd is achieved with the simplified irradiation procedure.
Horita, Takuma; Asai, Shiho; Hanzawa, Yukiko; Saito, Kyoichi*; Sugo, Takanobu*; Fujiwara, Kunio*; Kitatsuji, Yoshihiro
no journal, ,
There has been an increasing importance of the development of rapid Sr analysis technique, responding to needs in Fukushima Daiichi NPP. We have been trying to achieve a rapid analysis using a fibrous Sr adsorbent which has high selectivity for Sr
. The fiber we prepared that has a high-density Sr adsorption phase on its surface, and so it can adsorb Sr
on the fiber surface. On the other hand, base material of a conventional Sr adsorptive resin for
Sr analysis (Sr Resin) is bead-shaped resin, and
Sr is adsorbed inside pores. The fiber allows highly efficient
counting by minimizing the self-attenuation effects. The adsorption capacity and selectivity of the fiber was nearly the same as those of the Sr Resin. From these results, we confirmed that the fiber has performance for efficient
counting of
Sr.
Konda, Miki; Horita, Takuma; Asai, Shiho; Matsueda, Makoto; Hanzawa, Yukiko; Saito, Kyoichi*; Fujiwara, Kunio*; Sugo, Takanobu*; Kameo, Yutaka
no journal, ,
no abstracts in English
Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
no journal, ,
Safe and cost-effective disposal of radioactive wastes requires reliable evaluation of the amount of the radionuclides found in such wastes. Measurement of Pd, one of the radionuclides that are necessary to be evaluated, is associated with highly radioactive sample (e.g., spent nuclear fuel sample), resulting in only a few data in published forms. We separated Pd as a precipitate from a spent nuclear fuel sample and then determined the precise amount of
Pd. However, the method needed dissolution of the Pd precipitate to carry it to the sample introduction system of ICP-MS. In this study, we tried direct measurement of the Pd precipitate with laser-ablation (LA)-ICP-MS that enables solid sample measurement. The diameters of the recovered Pd precipitates were less than 500 nm, which is much smaller than the ablation spot. This allowed Pd to be uniformly vaporized, leading to sufficiently stable signals with high precisions equivalent to those of conventional ICP-MS.
Do, V. K.; Horita, Takuma; Miura, Katsue; Iwasaki, Maho
no journal, ,
Radioactive Material Analysis and Research Facility has been recently established to support the analysis of samples including fuel debris and radioactive wastes from the decommissioning of Fukushima Daiichi Nuclear Power Station (1F). ICP-MS is considered as a potential analytical tool for long-lived nuclides in fuel debris because of its superior sensitivity. Moreover, the use of ICP-MS is aimed to increase the analysis capacity, which make possible to repeat measurements in order to obtain precise results and to reduce exposed dose of analysts because ICP-MS is much more rapid than radiometric methods. Employing latest advanced technologies, a triple quadrupole ICP-MS, Agilent 8900 (ICP-QQQ-MS), enables to suppress the isobaric interference. In this presentation, we report some demonstrative separations of difficult-to-measure nuclides using the ICP-QQQ-MS system. The obtained results indicate that the separations are possible with suitable reaction gases.
Saeki, Morihisa*; Asai, Shiho; Yomogida, Takumi; Hanzawa, Yukiko; Taguchi, Tomitsugu*; Horita, Takuma; Kitatsuji, Yoshihiro; Oba, Hironori*
no journal, ,
Platinum-group metals (PGMs), such as Pd, Ru, and Rh are generated by nuclear fission of U and can be found in spent nuclear fuel (SNF) and high-level radioactive waste (HLW). Separation techniques for PGMs from HLW have been investigated for the safety assessment of HLW and the reuse of PGMs as resources. Among such PGMs, only Pd has a long-lived radionuclide Pd. Accordingly, the precise measurement of the amount of
Pd in HLW is essential for the long-term safety management of HLW. The determination of
Pd requires a reliable separation technique that allows selective Pd recovery with high purity. We developed a new separation technique specialized for PGMs. The technique involves UV-laser irradiation that induces selective reduction of ions of PGMs. The reduced PGMs can be readily recovered as precipitates. At the conference, the separation performances of PGMs and some applications of our technique will be discussed.
Horita, Takuma; Iwasaki, Maho
no journal, ,
no abstracts in English