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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:8 Percentile:31.98(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

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:8 Percentile:29.82(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

Simple method for high-density impregnation of Aliquat 336 onto porous sheet and binding performance of resulting sheet for palladium ions

Tanaka, Ryota*; Ishihara, Ryo*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*; Asai, Shiho; Yamada, Shinsuke*; Hirota, Hideyuki*

Separation Science and Technology, 49(1), p.154 - 159, 2014/01

 Times Cited Count:4 Percentile:16.82(Chemistry, Multidisciplinary)

Journal Articles

Determination of mole percentages of brush and root of polymer chain grafted onto porous sheet

Uchiyama, Shoichiro*; Ishihara, Ryo*; Umeno, Daisuke*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*; Asai, Shiho

Journal of Chemical Engineering of Japan, 46(6), p.414 - 419, 2013/06

 Times Cited Count:7 Percentile:26.06(Engineering, Chemical)

Journal Articles

Crosslinked-chelating porous sheet with high dynamic binding capacity of metal ions

Wada, Go*; Ishihara, Ryo*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*; Asai, Shiho; Yamada, Shinsuke*; Hirota, Hideyuki*

Solvent Extraction and Ion Exchange, 31(2), p.210 - 220, 2013/02

 Times Cited Count:2 Percentile:12.24(Chemistry, Multidisciplinary)

A crosslinked chelating porous sheet was prepared by cografting ethylene glycol dimethacrylate (EGDMA) with glycidyl methacrylate onto an electron-beam-irradiated porous polyethylene sheet, followed by the introduction of an iminodiacetate group. At a molar percentage of EGDMA of 1.0 mol%, the sheet exhibited a maximum dynamic binding capacity for copper ions of 0.93 mmol/g, while the equilibrium binding capacity remained the same (1.2 mmol/g) as that of a non-crosslinked chelating porous sheet. The crosslinking of the grafted chain causes copper ions to lower their diffusion rate along the sheet thickness driven by the gradient of the amount of copper ions adsorbed.

Journal Articles

Dependence of lanthanide-ion binding performance on HDEHP concentration in HDEHP impregnation to porous sheet

Ishihara, Ryo*; Asai, Shiho; Otosaka, Shigeyoshi; Yamada, Shinsuke*; Hirota, Hideyuki*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*

Solvent Extraction and Ion Exchange, 30(2), p.171 - 180, 2012/02

 Times Cited Count:8 Percentile:31.67(Chemistry, Multidisciplinary)

Journal Articles

Effect of chelating group density of crosslinked graft chain on dynamic binding capacity for metal ions

Wada, Go*; Ishihara, Ryo*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*; Asai, Shiho; Yamada, Shinsuke*; Hirota, Hideyuki*

Nihon Ion Kokan Gakkai-Shi, 22(2), p.47 - 52, 2011/01

no abstracts in English

Journal Articles

Modification of a hydrophobic-ligand-containing porous sheet using tri-$$n$$-octylphosphine oxide, and its adsorption/elution of bismuth ions

Tanaka, Ryota*; Ishihara, Ryo*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*; Asai, Shiho; Yamada, Shinsuke*; Hirota, Hideyuki*

Reactive and Functional Polymers, 70(12), p.986 - 990, 2010/12

 Times Cited Count:7 Percentile:29.11(Chemistry, Applied)

Journal Articles

Application of diethylamino-group-containing porous-polymeric-disk-packed cartridge to separation of U in urine sample

Asai, Shiho; Kimura, Takaumi; Miyoshi, Kazuyoshi*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

Nihon Ion Kokan Gakkai-Shi, 21(3), p.334 - 339, 2010/07

JAEA Reports

Wall current monitor for SPring-8 linac

; *; *; ; *; Yoshikawa, Hiroshi; ; Sakaki, Hironao; *; Yokomizo, Hideaki

JAERI-M 94-078, 29 Pages, 1994/06

JAERI-M-94-078.pdf:1.05MB

no abstracts in English

Oral presentation

Highly efficient separation of actinides using porous polymer sheet with anion-exchange group

Asai, Shiho; Magara, Masaaki; Shinohara, Nobuo; Yamada, Shinsuke*; Nagai, Masanori*; Miyoshi, Kazuyoshi*; Saito, Kyoichi*

no journal, , 

A porous sheet with a diethylamino (DEA) group as anion-exchange group was prepared for achieving rapid separation of U and Pu. The epoxy group containing monomer, glycidyl methacrylate was grafted onto the surface of the porous sheet. The epoxy group of the poly-GMA graft polymer chain was converted into a DEA group. The amount of the DEA group was increased with increasing reaction time and leveled off at 3.4 mol/kg of the sheet. An iron solution as a model metal ion solution was forced to permeate through the pores of the DEA-introduced sheet (DEA sheet) at a permeation rate of 20 mL/min. The equilibrium adsorption capacity of the DEA sheet for Fe ions (FeCl$$_{4}$$$$^{-}$$) was calculated as 1.1 mol-Fe/kg-DEA sheet. This value is comparable to or higher than those of conventional anion-exchange resins. U and Pu in the sample solution were separated using the DEA sheet. Trace amounts of U (38.16 pg) and Pu (0.34 pg) were found to be successfully separated with the DEA sheet.

Oral presentation

Highly efficient solid-phase extraction of inorganic ions using ion-exchange porous polymer disk cartridge

Asai, Shiho; Magara, Masaaki; Shinohara, Nobuo; Yamada, Shinsuke*; Nagai, Masanori*; Miyoshi, Kazuyoshi*; Saito, Kyoichi*

no journal, , 

The use of a column charged with an ion-exchange resin has been widely employed to separation of actinides. However, the use of the resin-packed column has a drawback in that a higher flow rate of the sample solution through the column results in a lower recovery. In order to overcome this drawback in the use of the conventional column, we prepared an anion-exchange cartridge charged with a diethylamino-group-containing porous disk. To evaluate the applicability, the binding efficiencies of U and Pu were determined at various flow rates. 5 mL of standard solution containing U and Pu was permeated through the anion-exchange cartridge at the flow rate raging from 0.3 to 80 mL/min. Adsorption efficiencies of U and Pu were 1.0 irrespective of the flow rate. This adsorption characteristic is advantageous over the conventional anion-exchange resin-packed column in that a higher flow rate of the sample solution, i. e., a shorter processing time of analysis, is achievable.

Oral presentation

Preparation of cation-exchange porous sheet for determination of selenium in high-level radioactive liquid waste

Asai, Shiho; Esaka, Fumitaka; Shinohara, Nobuo; Yamada, Shinsuke*; Nagai, Masanori*; Miyoshi, Kazuyoshi*; Saito, Kyoichi*

no journal, , 

no abstracts in English

Oral presentation

Separation of fission products using cation-exchange porous disk for determination of Selenium-79

Asai, Shiho; Esaka, Fumitaka; Shinohara, Nobuo; Hirota, Hideyuki*; Yamada, Shinsuke*; Miyoshi, Kazuyoshi*; Saito, Kyoichi*

no journal, , 

no abstracts in English

Oral presentation

Development of functionalized porous polymeric sheet for inorganic analysis

Asai, Shiho; Otosaka, Shigeyoshi; Tanaka, Ryota*; Miyoshi, Kazuyoshi*; Ishihara, Ryo*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

no journal, , 

no abstracts in English

Oral presentation

Preparation of functionalized porous polymeric sheet prepared with radiation-induced graft polymerization

Asai, Shiho; Kimura, Takaumi; Miyoshi, Kazuyoshi*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*

no journal, , 

no abstracts in English

Oral presentation

Impregnation of Aliquat 336 to carboxydecanyl-thiol-group-containing polymer chain grafted onto a porous sheet

Tanaka, Ryota*; Ishihara, Ryo*; Miyoshi, Kazuyoshi*; Umeno, Daisuke*; Saito, Kyoichi*; Asai, Shiho; Yamada, Shinsuke*; Hirota, Hideyuki*

no journal, , 

A basic extractant Aliquat 336 dissolved in a mixture of ethanol and NaOH aqueous solution was impregnated to carboxydecanyl-thiol (CDT) group containing polymer chains grafted onto a porous sheet. The CDT group was introduced into the graft chain by a reaction of the epoxy group of poly-glycidyl methacrylate (GMA) chain grafted onto the porous sheet with 11-mercaptoundecanoic acid. The electrostatic interaction between the carboxyl moiety of the CDT group and the quaternary ammonium group of Aliquat 336 gave rise to a high-density impregnation of Aliquat 336. Palladium chloride (50 mg-Pd/L) in 1 M HCl was forced to permeate through the pores of the Aliquat 336-impregnated porous sheet. The binding efficiency, defined as the ratio of number of moles of palladium adsorbed to half the number of moles of impregnated Aliquat 336, was found to be 64%.

Oral presentation

Anion-exchange porous polymer sheet for rapid analysis of $$^{237}$$Np in spent nuclear fuel

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

no journal, , 

no abstracts in English

Oral presentation

Determination of $$^{237}$$Np in spent nuclear fuel using anion-exchange porous polymeric filter

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

no journal, , 

no abstracts in English

Oral presentation

Performance evaluation of micro-volume anion-exchange filter prepared by graft polymerization on Zr separation and its application to determination of Zr-93 in spent fuel

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

no journal, , 

$$^{93}$$Zr is a long-lived fission product which can be found in spent nuclear fuel and HLW. The estimation of the$$^{93}$$Zr content is indispensable to achieve a safety disposal of HLW because $$^{93}$$Zr is predicted to be one of the major contributors to radiation dose. However, only a few measured $$^{93}$$Zr values have been reported, leading to a high demand for development of an efficient analytical method. Our group has been prepared a new porous filter cartridge which has densely bound ion-exchanger onto the pore surface of the filter, enabling a high-capacity and rapid adsorption. In order to apply this filter cartridge to a pretreatment for the $$^{93}$$Zr measurement with ICP-MS, an elution profiles of Zr and the other coexisting elements were examined. According to the resultant separation conditions, Zr in a spent nuclear fuel sample was successfully separated. The measured $$^{93}$$Zr content is 98.2 $$pm$$ 5.1 ng, which agrees with the theoretical value.

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