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Journal Articles

Direct quantitation of $$^{135}$$Cs in spent Cs adsorbent used for the decontamination of radiocesium-containing water by laser ablation inductively coupled plasma mass spectrometry

Asai, Shiho*; Ohata, Masaki*; Hanzawa, Yukiko; Horita, Takuma; Yomogida, Takumi; Kitatsuji, Yoshihiro

Analytical Chemistry, 92(4), p.3276 - 3284, 2020/02

 Times Cited Count:1 Percentile:27.48(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 $$^{135}$$Cs content prior to final disposal. $$^{135}$$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 $$^{137}$$Cs. To address this challenge, we herein employed laser ablation ICP-MS for direct quantitation of $$^{135}$$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 $$^{135}$$Cs/$$^{137}$$Cs ratio and $$^{137}$$Cs radioactivity obtained by gamma spectrometry achieved simple and precise quantitation of $$^{135}$$Cs and the resulting $$^{135}$$Cs activity of 0.36 Bq agreed well with that in the original radiocesium-containing liquid waste.

Journal Articles

Determination of $$^{107}$$Pd in Pd purified by selective precipitation from spent nuclear fuel by laser ablation ICP-MS

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:2 Percentile:45.8(Biochemical Research Methods)

Determination of radiopalladium $$^{107}$$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 $$^{107}$$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, $$^{102}$$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 $$^{107}$$Pd/$$^{102}$$Pd. The amount of $$^{107}$$Pd obtained by LA-ICP-MS corresponds to the values obtained by conventional solution nebulization measurement.

Journal Articles

Rapid separation of zirconium using microvolume anion-exchange cartridge for $$^{93}$$Zr determination with isotope dilution ICP-MS

Asai, Shiho; Hanzawa, Yukiko; Konda, Miki; Suzuki, Daisuke; Magara, Masaaki; Kimura, Takaumi; Ishihara, Ryo*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

Talanta, 185, p.98 - 105, 2018/08

 Times Cited Count:3 Percentile:67.24(Chemistry, Analytical)

Estimating the risks associated with radiation from long-lived fission products (LLFP) in radioactive waste is essential to ensure the long-term safety of potential disposal sites. In this study, the amount of $$^{93}$$Zr, a LLFP, was determined by ICP-MS after separating Zr from a spent nuclear fuel solution using a microvolume anion-exchange cartridge (TEDA cartridge). The TEDA cartridge achieved highly selective separation of Zr regardless of its small bed volume of 0.08 cm$$^{3}$$. The time taken to complete the Zr separation was 1.2 min with a flow rate of 1.5 mL/min, which was 10 times faster than that for a conventional anion-exchange resin column. Almost all the other elements were removed, leading to accurate measurement of $$^{93}$$Zr. The result connects experimental value to theoretical prediction provided by ORIGEN2, which requires verification. With the measured value, we demonstrated that the theoretical value is reliable enough to estimate radiation risks.

Journal Articles

Non-contact and selective Pd separation based on laser-induced photoreduction for determination of $$^{107}$$Pd by ICP-MS; The Relation between separation conditions and Pd recovery

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:1 Percentile:92.51(Chemistry, Analytical)

Palladium-107 is a long-lived fission product, which can be found in high-level radioactive liquid wastes (HLLW). Determination of the $$^{107}$$Pd contents in HLLW is essential to evaluate the long-term safety of HLLW repositories. However, the $$^{107}$$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$$^{-1}$$, showing the applicability of the proposed separation technique to HLLW samples.

Journal Articles

Preparation of Sr adsorptive fiber by impregnating with crown ether derivative for $$^{90}$$Sr measurement

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:0 Percentile:100(Chemistry, Analytical)

A Sr-selective adsorption fiber was prepared for rapid analysis of $$^{90}$$Sr content by using radiation-induced emulsion graft polymerization and subsequent chemical modification. A polyethylene fiber with a diameter of 13 $$mu$$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).

Journal Articles

Determination of $$^{107}$$Pd in Pd recovered by laser-induced photoreduction with inductively coupled plasma mass spectrometry

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:7 Percentile:57.18(Chemistry, Analytical)

Safety evaluation of a radioactive waste repository requires credible activity estimates confirmed by actual measurements. A long-lived radionuclide, $$^{107}$$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 $$^{107}$$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 $$^{107}$$Pd.

JAEA Reports

Preparation of Zr-91 stable isotope standard solution for determination of Zr-93 by mass spectrometry

Konda, Miki; Asai, Shiho; Hanzawa, Yukiko; Magara, Masaaki

JAEA-Technology 2015-054, 22 Pages, 2016/03


Isotope dilution mass spectrometry (IDMS) with ICP-MS is reliable method for determination of Zr-93, which is one of the long-lived fission products found in spent nuclear fuel and high-level radioactive wastes. In order to use an isotope standard solution of zirconium as the spike for IDMS, dissolving a commercially available solid isotope standard is indispensable. Prior to the dissolution of the Zr-91 isotope standard, solubility of metal zirconium in a mixture of HNO$$_3$$ and HF was evaluated using zirconium metal chips. Then, 2 mg of the Zr-91 isotope standard was dissolved with 0.2 mL of 1 M HNO$$_3$$-3 v/v% HF mixed solution, followed by adjusting the concentration of Zr-91 to approximately 1,000 $$mu$$g/g. IDMS, in which a natural isotopic abundance standard solution of zirconium was used as the spike, was employed for the determination of the concentration of Zr-91 in the prepared Zr-91 isotope standard solution. The concentration of Zr-91 in the prepared Zr-91 isotope standard solution was (9.6$$pm$$1.0) $$times$$ 10$$^2$$ $$mu$$g/g, which is in good agreement with the predicted concentration. This indicates that the Zr-91 metal isotope standard was completely dissolved with sufficient chemical stability. Additionally, no impurities were detected in the prepared Zr-91 isotope standard solution. These positive results denote that the Zr-91 isotope standard solution with the preferable quality for IDMS of Zr-93 can be obtained by the proposed dissolution procedures.

Journal Articles

Preparation of microvolume anion-exchange cartridge for inductively coupled plasma mass spectrometry-based determination of $$^{237}$$Np content in spent nuclear fuel

Asai, Shiho; Hanzawa, Yukiko; Konda, Miki; Suzuki, Daisuke; Magara, Masaaki; Kimura, Takaumi; Ishihara, Ryo*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

Analytical Chemistry, 88(6), p.3149 - 3155, 2016/03

 Times Cited Count:7 Percentile:57.18(Chemistry, Analytical)

Neptunium-237 ($$^{237}$$Np) is one of the major long-lived radionuclides found in spent nuclear fuel. To evaluate the long-term safety of a HLW repository, the $$^{237}$$Np content in spent nuclear fuel must be determined. In this study, micro-volume anion-exchange porous polymer disk-packed cartridges were prepared for Am-Np separation, which is required prior to the measurement of $$^{237}$$ Np with ICP-MS. Disks with a volume of 0.08 cm$$^{3}$$ were cut out from porous sheets having triethylenediamine (TEDA)-containing polymer chains densely attached on the pore surface. The resulting TEDA-introduced disk cartridge was applied to a spent nuclear fuel sample. The chemical yield of Np was 90.4%, which is sufficiently high for ICP-MS measurement of $$^{237}$$Np. Compared with the conventional separation technique using commercially available anion-exchange resin columns, the time required to adsorb, wash and elute Np using the TEDA-introduced disk cartridge was reduced by 75%.

Journal Articles

Increase in rare earth element concentrations controlled by dissolved organic matter in river water during rainfall events in a temperate, small forested catchment

Matsunaga, Takeshi; Tsuzuki, Katsunori; Yanase, Nobuyuki; Kritsananuwat, R.*; Hanzawa, Yukiko; Naganawa, Hirochika

Journal of Nuclear Science and Technology, 52(4), p.514 - 529, 2015/04

 Times Cited Count:3 Percentile:62.51(Nuclear Science & Technology)

In a temperate, forested river catchment, distribution of dissolved rare earth elements (REE) during rainfall events was studied as analogues elements for transuranic nuclides. Concentrations of dissolved REE showed almost concurrent increases and decreases with the river water discharge during rainfall events. The concentration variations were tightly coupled with those of optical properties related to humic substances of dissolved organic matter (DOM). An ultrafiltration analysis revealed that colloidal REE present in 10 k - 30 kDa size fraction was the chief component for dissolved REE increase in high water flow condition. Shale-normalized concentration patterns of REE suggest an involvement of humic substances of DOM. A high correlation between size fractioned REE concentrations and specific ultraviolet absorbance suggests that aromaticity would be an essential property of DOM in regard to its complexation with dissolved REE in the studied river water.

Journal Articles

Application of capillary electrophoresis with laser-induced fluorescence detection for the determination of trace neodymium in spent nuclear fuel using complexation with an emissive macrocyclic polyaminocarboxylate probe

Haraga, Tomoko; Saito, Shingo*; Sato, Yoshiyuki; Asai, Shiho; Hanzawa, Yukiko; Hoshino, Hitoshi*; Shibukawa, Masami*; Ishimori, Kenichiro; Takahashi, Kuniaki

Analytical Sciences, 30(7), p.773 - 776, 2014/07

 Times Cited Count:5 Percentile:75.13(Chemistry, Analytical)

A simple and rapid method with low radiation exposure risk was developed for the determination of neodymium in spent nuclear fuel by CE with LIF detection using a fluorescent ligand having a macrocyclic hexadentate polyaminocarboxylate structure. The concentration of Nd(III) in a spent nuclear fuel sample was determined with no interference from various matrix elements, including lanthanides and uranium (at a 200-fold excess), with 92 $$pm$$ 3% recovery. This is due to method's high resolution based on establishing a ternary complex equilibrium during migration in which the hydroxyl ion plays an auxiliary role.

Journal Articles

Temporal variations in metal enrichment in suspended particulate matter during rainfall events in a rural stream

Matsunaga, Takeshi; Tsuzuki, Katsunori; Yanase, Nobuyuki; Kritsananuwat, R.*; Ueno, Takashi; Hanzawa, Yukiko; Naganawa, Hirochika

Limnology, 15(1), p.13 - 25, 2014/01

 Times Cited Count:5 Percentile:72.04(Limnology)

We studied a discharge of heavy metals/metalloids in rainfall events to a rural stream in Kuji River basin of central Japan. In terms of elemental enrichment with respect to the crustal composition, we found similarity between atmospheric deposits and suspended particulate matter (SPM) at a rural stream. Both exhibited distinctive enrichment in several metals (Ni, Cu, Pb, Sb, and Cd). Elemental analysis of SPM in the stream in rainfall events at short intervals revealed that the metal enrichment factors in SPM were progressively decreased with an increase of flow rate. Judging from features of SPM, this phenomenon was probably caused by alternative change of SPM matrices from upper soil constituents to more lithologic material with increasing stream flow rate. In quantification of respective contributions of metals of different origins to fluvial discharge, change of SPM matrices during a rainfall event and involvement of dissolved fraction need to be taken into consideration.

Journal Articles

Continuous extraction of uranium from actual uranium-containing liquid wastes using an "emulsion flow" extractor

Nagano, Tetsushi; Yanase, Nobuyuki; Naganawa, Hirochika; Mitamura, Hisayoshi; Hanzawa, Yukiko; Mita, Yutaka; Kanda, Nobuhiro; Ohashi, Yusuke; Endo, Yuji; Matsubara, Tatsuo

Nippon Genshiryoku Gakkai Wabun Rombunshi, 12(4), p.277 - 285, 2013/12

no abstracts in English

Journal Articles

Isotope dilution inductively coupled plasma mass spectrometry for determination of $$^{126}$$Sn content in spent nuclear fuel sample

Asai, Shiho; Toshimitsu, Masaaki; Hanzawa, Yukiko; Suzuki, Hideya; Shinohara, Nobuo; Inagawa, Jun; Okumura, Keisuke; Hotoku, Shinobu; Kimura, Takaumi; Suzuki, Kensuke*; et al.

Journal of Nuclear Science and Technology, 50(6), p.556 - 562, 2013/06

 Times Cited Count:7 Percentile:41.02(Nuclear Science & Technology)

The $$^{126}$$Sn content in a spent nuclear fuel solution was determined by ICP-MS for its inventory estimation in high-level radioactive waste. An irradiated UO$$_{2}$$ fuel was used as a sample to evaluate the reliability of the methodology. Prior to the measurement, Sn was separated from $$^{126}$$Te, which causes major isobaric interference in the determination of $$^{126}$$Sn content, along with highly radioactive coexisting elements using an anion-exchange column. The absence of counts attributed to Te in the Sn-containing effluent indicates that Te was completely removed. After washing, Sn retained on the column was readily eluted with 1 M HNO$$_{3}$$. The isotope ratios of Sn were successfully determined and showed good agreement with those obtained through ORIGEN2 calculations. The results reported in this paper are the first experimental values of $$^{126}$$Sn content in the spent nuclear fuel solution originating in spent nuclear fuel irradiated at a nuclear power plant in Japan.

Journal Articles

Simple cation-exchange separation for ICP-MS measurement of $$^{79}$$Se in spent nuclear fuel sample

Asai, Shiho; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Okumura, Keisuke; Shinohara, Nobuo; Kimura, Takaumi; Inagawa, Jun; Suzuki, Kensuke*; Kaneko, Satoru*

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 5 Pages, 2011/12

Journal Articles

New ORIGEN2 libraries based on JENDL-4.0 and their validation for long-lived fission products by post irradiation examination analyses of LWR spent fuels

Kojima, Kensuke; Okumura, Keisuke; Asai, Shiho; Hanzawa, Yukiko; Okamoto, Tsutomu; Toshimitsu, Masaaki; Inagawa, Jun; Kimura, Takaumi; Kaneko, Satoru*; Suzuki, Kensuke*

Proceedings of International Conference on Toward and Over the Fukushima Daiichi Accident (GLOBAL 2011) (CD-ROM), 5 Pages, 2011/12

Accurate inventory estimation of long-lived fission products (LLFPs) in LWR spent fuels is important for the quality management and for long-term safety assessment of high-level radioactive vitrified wastes. In Japan, ORIGEN2 has been widely used to estimate the fuel compositions. However, equipped library data in the original ORIGEN2 are old and are not validated enough for LLFPs, such as $$^{79}$$Se, $$^{99}$$Tc, $$^{126}$$Sn and $$^{135}$$Cs, because available post irradiation examination (PIE) data are limited for these nuclides, which have difficulties in radiochemical analyses. For more accurate the estimation, new ORIGEN2 libraries are developed from the latest nuclear data library JENDL-4.0 for cross sections and fission yields, and from other libraries for half-lives, and so on. The new libraries are validated by PIE analyses of the sample fuels irradiated in Cooper, Calvert-Cliffs-1, H. B. Robinson-2, and Ohi-1. As a result, it was found that the new library gives good results for the estimation.

Journal Articles

Analyses of assay data of LWR spent nuclear fuels with a continuous-energy Monte Carlo code MVP and JENDL-4.0 for inventory estimation of $$^{79}$$Se, $$^{99}$$Tc, $$^{126}$$Sn and $$^{135}$$Cs

Okumura, Keisuke; Asai, Shiho; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Inagawa, Jun; Okamoto, Tsutomu; Shinohara, Nobuo; Kaneko, Satoru*; Suzuki, Kensuke*

Progress in Nuclear Science and Technology (Internet), 2, p.369 - 374, 2011/10

For accurate inventory estimation of long-lived fission products in LWR spent fuels, a new burn-up chain model and decay data based on the latest nuclear data such as JENDL-4.0 was developed. MVP-BURN with the latest nuclear data was applied to several post irradiation examinations including inventory measurements of $$^{79}$$Se, $$^{99}$$Tc, $$^{126}$$Sn and $$^{135}$$Cs. One of them is a new measurement by JAEA. From the PIE analyses, it is found that the new PIE data obtained by JAEA is consistent with the other PIE data by different laboratory with different techniques. It is also confirmed that the present calculation results show good agreements with experimental ones within about 10% for productions of $$^{79}$$Se and $$^{135}$$Cs. In contrast, amounts of $$^{99}$$Tc and $$^{126}$$Sn are overestimated by about 50%. These discrepancies are likely due to the effect of insoluble residue produced during sample dissolution and/or errors of fission yields in the analyses.

Journal Articles

Validation of correlations between Nd isotopes and difficult-to-measure nuclides predicted with burn-up calculation code by post irradiation examination

Asai, Shiho; Okumura, Keisuke; Hanzawa, Yukiko; Suzuki, Hideya; Toshimitsu, Masaaki; Inagawa, Jun; Kimura, Takaumi; Kaneko, Satoru*; Suzuki, Kensuke*

Proceedings of 14th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2011) (CD-ROM), p.1437 - 1442, 2011/09

Journal Articles

Computational study for inventory estimation of Se-79, Tc-99, Sn-126, and Cs-135 in high-level radioactive wastes from spent nuclear fuels of light water reactors

Okumura, Keisuke; Asai, Shiho; Hanzawa, Yukiko; Okamoto, Tsutomu; Suzuki, Hideya; Toshimitsu, Masaaki; Inagawa, Jun; Kimura, Takaumi; Suzuki, Kensuke*; Kaneko, Satoru*

Proceedings of 14th International Conference on Environmental Remediation and Radioactive Waste Management (ICEM 2011) (CD-ROM), p.1443 - 1450, 2011/09

Inventory estimation of long-lived fission products (LLFPs) in high-level radioactive wastes (HLW) from spent nuclear fuels of light water reactors is important for a safety assessment of their disposal. In order to develop an inventory estimation method of difficult-to-measure LLFPs (Se-79, Tc-99, Sn-126, and Cs-135), a parametric study was carried out by using a sophisticated burnup calculation code and data. In the parametric study, fuel specifications and irradiation conditions are changed in the conceivable range. The considered parameters are fuel assembly types (PWR / BWR), U-235 enrichment, moderator temperature, void fraction, power density, and so on. From the calculated results, we clarify the burnup characteristics of the target LLFPs and their possible ranges of generations. Finally, candidates of the key nuclide are proposed for the scaling factor method of HLW.

Journal Articles

Determination of $$^{79}$$Se and $$^{135}$$Cs in spent nuclear fuel for inventory estimation of high-level radioactive wastes

Asai, Shiho; Hanzawa, Yukiko; Okumura, Keisuke; Shinohara, Nobuo; Inagawa, Jun; Hotoku, Shinobu; Suzuki, Kensuke*; Kaneko, Satoru*

Journal of Nuclear Science and Technology, 48(5), p.851 - 854, 2011/05

 Times Cited Count:21 Percentile:11.84(Nuclear Science & Technology)

Journal Articles

Evaluation of the affinity of some toxic elements to schwertmannite in natural streams contaminated with acid mine drainage

Nagano, Tetsushi; Yanase, Nobuyuki; Hanzawa, Yukiko; Takada, Morio*; Mitamura, Hisayoshi; Sato, Tsutomu*; Naganawa, Hirochika

Water Air and Soil Pollution, 216(1-4), p.153 - 166, 2011/03

 Times Cited Count:6 Percentile:72.82(Environmental Sciences)

Schwertmannite is a poorly-crystalline ferric sulphate mineral that secondarily forms in acid mine drainages (AMD) as a result of the oxidative weathering of pyrite (FeS2), and is known to work as a naturally-occurring scavenger of some toxic elements in AMD-contaminated streams due to its high fixation potentials. In this study, to examine the feasibility of using schwertmannite in water purification technique, we evaluate the affinity of some selected elements to schwertmannite using two parameters: (1) conventional apparent solid-liquid partition coefficients between schwertmannite and stream waters, and (2) newly introduced parameters that correspond to ratios of ions fixed by schwertmannite to those existing as dissolved phases. As a result, both of the two parameters revealed that schwertmannite has high fixation potential for fluvial transport of various toxic anions such as V, Cr, As, Mo and Sb in AMD-contaminated streams, and that it could be used for purification of waters contaminated with these toxic anions.

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