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Journal Articles

Separation of Am and Cm from HLLW by extraction chromatography using novel R-BTP extraction resins

Wei, Y.*; Hoshi, Harutaka; Morita, Yasuji; Bruggeman, A.*; Goethals, P.*

Proceedings of International Conference on Advanced Nuclear Fuel Cycle; Sustainable Options & Industrial Perspectives (Global 2009) (CD-ROM), p.1086 - 1093, 2009/09

To separate the long-lived minor actinides (MA = Am, Cm) from high level liquid waste (HLLW), we have been studying an advanced process by extraction chromatography which uses minimal organic solvent and compact equipment. Generally, the process consists of two separation columns packed with CMPO extraction resin for elemental group separation and R-BTP extraction resin for the isolation of MA from lanthanides (Ln), respectively. R-BTP is a family of nitrogen-donor ligand which has been verified to have stronger adsorption affinity for trivalent MA over Ln(III). As an extractant or adsorbent, it is generally considered that R-BTP compounds shall be used in a weakly acid medium, since the compounds show less stability in acidic medium due to the protonation of nitrogen atoms. However, we have found that the adsorption selectivity for Am(III) and Cm(III) and chemical stability of R-BTP adsorbents strongly depend on the length and structure of the alkyl group.

JAEA Reports

Study on investigation of microbial effects for geological disposal, 2 (Joint research)

Tochigi, Yoshikatsu; Yoshikawa, Hideki; Aoki, Kazuhiro; Yui, Mikazu; Asano, Takahiro*; Honjo, Hideko*; Haginuma, Masashi*; Kawakami, Yasushi*; Suzuki, Kazunori*

JAEA-Research 2008-025, 55 Pages, 2008/03

JAEA-Research-2008-025.pdf:8.55MB

Results of joint research on fiscal year 2006 between Japan Atomic Energy Agency (JAEA) and Institute of Research and Innovative (IRI) titled as "Study on investigation of microbial effects for geological disposal" are described in this report. The objective of this study is to develop a method for estimating microbial effects for barrier performance of geological disposal site. The modeling was performed to examine the effect on the change in groundwater chemistry (mainly by electron acceptors) by microbial metabolism as well as microbial activities. In order to use the data (chemical composition, biomass, etc.) in the MINT code, groundwater was collected from the drilled well prepared for chemical and microbial analyses of groundwater. The well was prepared in observation field near Horonobe Underground Research Center of JAEA in fiscal year 2006. Then, numerical modeling using collected data of groundwater with numerical modeling program code "MINT" considering microbial effects was carried out. The modeling was carried out to evaluate the microbial effect for stability of chemical and microbial composition of groundwater. As the result of the modeling, relatively low microbial effect for groundwater composition was observed in particular for the concentration of dissolved methane, methanogen, sulfur reducing bacteria (SRB) and sulfur ion. The result shows that low redox potential is stable in the well in spite of shallow depth.

Journal Articles

Study on valence of Pu, Np and Tc in nitric acid after electrolytic reduction

Hoshi, Harutaka*; Wei, Y.-Z.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Journal of Alloys and Compounds, 444-445, p.663 - 667, 2007/10

 Times Cited Count:4 Percentile:33.26(Chemistry, Physical)

no abstracts in English

JAEA Reports

Study on simulation of salt accumulation (Joint research)

Fujita, Tomoo; Yui, Mikazu; Suzuki, Hideaki*; Fujisaki, Kiyoshi; Sazarashi, Masami*

JAEA-Research 2007-017, 47 Pages, 2007/03

JAEA-Research-2007-017.pdf:9.27MB

This report describes the results of a joint research entitled "Study on Simulation of Salt Accumulation" which was conducted under the collaboration between the Institute of Research and Innovation and the Japan Atomic Energy Agency. In the experiments for salt accumulation, accumulation of ${it Na$_{2}$SO$_{4}$}$ and ${it CaSO$_{4}$}$ was observed near the heater surface. Based on the facts from experiments, we have made hypothesis for mechanism of salt accumulation, and developed the model for it. Then, we conducted numerical simulations for salt accumulation phenomena under the saturated condition using the geochemical code "PHREEQC". It became clear that salt accumulation behavior can be evaluated qualitatively from these simulations, but quantitative evaluation requires more realistic modeling. Moreover we evaluated salt accumulation phenomena by simulations using coupled thermo - hydro - mechanical and chemical model / code assuming the unsaturated and / or saturated condition. A series of simulations were conducted focusing on accumulation of gypsum, and the result showed that tendency of salt accumulation phenomena was in agreement with that of experiments, but the profile of distribution of accumulated gypsum was not in agreement. In conclusion, it became clear that more realistic boundary condition should be considered and problems on coupled model / code were identified for further study.

JAEA Reports

Study on investigation of microbial effects for geological disposal, 1 (Joint research)

Tochigi, Yoshikatsu; Yoshikawa, Hideki; Aoki, Kazuhiro; Yui, Mikazu; Honjo, Hideko*; Haginuma, Masashi*; Kawakami, Yasushi*; Suzuki, Kazunori*

JAEA-Research 2007-010, 51 Pages, 2007/03

JAEA-Research-2007-010.pdf:4.82MB

Results of joint research on Fiscal 2005 between Japan Atomic Energy Agency (JAEA) and Institute of Research and Innovative (IRI) titled as "Study for investigation of microbial effects on geological disposal" are described in this report. The objective of this study is constructing advanced method for examining microbial effect for barrier performance of geological disposal site. In fiscal 2005, groundwater and rock core sample have been collected from drilled well on observation field near Horonobe Underground Research Center of JAEA and chemical analysis for collected ground water have been carried out and sensitivity analysis for existing observed data of groundwater with numerical analysis program code "MINT" considering microbial effect have been carried out.

JAEA Reports

Reliability improvement of hydro-geochemical and hydrogeological model on geological environment in Horonobe Underground Research Laboratory project; Report on the 2005 FY research (Joint research)

Hama, Katsuhiro; Kunimaru, Takanori; Kurikami, Hiroshi; Sasamoto, Hiroshi; Takahashi, Yasuhiro*; Haginuma, Masashi*; Ishii, Tomoko*; Matsuo, Yuji*

JAEA-Research 2006-070, 93 Pages, 2006/09

JAEA-Research-2006-070.pdf:23.48MB
JAEA-Research-2006-070(errata).pdf:0.08MB

Japan Atomic Energy Agency and Institute of Research and Innovation have started collaborative study in order to enhance the reliability of technology for the geological disposal of High-level Radioactive Waste (HLW) since 2005 fiscal year. In this collaborative study, the analysis has carried out to estimate long-term evolution of groundwater chemistry and groundwater flow. The study items and results are summarized in this report. (1) Groundwater Chemistry. The following items have been carried out: 1. Multivariate analysis. 2. Estimation of distribution of groundwater chemistry. 3. Construction of geochemical model. (2) Groundwater Flow: 1. Construction of geological model. 2. Construction of hydrogeological model. 3. Groundwater flow analysis. The modeling work will be continued in 2006 fiscal year. The applicability of the modeling methodology will also be evaluated.

Journal Articles

Separation of minor actinides and lanthanides from nitric acid solution by R-BTP extraction resin

Hoshi, Harutaka*; Wei, Y.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Recent Advances in Actinide Science, p.596 - 598, 2006/06

Recently, extraction selectivity for trivalent minor actinides (MA = Am and Cm) over lanthanides (Ln) has been found in some extractants containing soft donor, such as S or N, ligands. Kolarik et al. reported that a new N-donor ligand 2,6-bis(5,6-dialkyl-1,2,4-triazine-3-yl)-pyridine (R-BTP) shows high selectivity for MA (III) over Ln(III) [1]. However, protonation of R-BTP results in its acidic hydrolysis in acidic medium. Stability in acidic solution was improved by substitution of long normal chain or branched chain [2]. In this work, separation of MA(III) and Ln(III) from nitric acid solution was studied by using novel R-BTP impregnated resin. Branched R-BTP resin had high affinity for Am from up to 4 M HNO$$_{3}$$ solution and its distribution coefficient was over 10$$^{4}$$.

Journal Articles

Separation of trivalent actinides from lanthanides by using R-BTP resins and stability of R-BTP resin

Hoshi, Harutaka*; Wei, Y.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Journal of Alloys and Compounds, 408-412, p.1274 - 1277, 2006/02

 Times Cited Count:39 Percentile:84.47(Chemistry, Physical)

For the development of advanced aqueous reprocessing system, it is one of the most important subjects to separate minor trivalent actinides (MA = Am and Cm). Recently, extraction selectivity for MA(III) over Ln(III) has been found in some extractants containing soft donor, such as S or N, ligands. Kolarik et al. reported that a new N-donor ligand 2,6-bis(5,6-dialkyl-1,2,4-triazine-3-yl)-pyridine (R-BTP) shows high selectivity for MA (III) over Ln(III). The novel silica-based extraction resins were prepared by impregnating some R-BTP molecules into a macroreticular styrene-divinylbenzene copolymer which is immobilized in porous silica particles with a mean diameter of 50 $$mu$$m. Separation of simulated high level liquid waste solution containing Ln(III) and trace amount of Am(III) was studied. Am(III) was mutually separated from Ln(III) through a packed column with R-BTP impregnating resin, very high decontamination factor ($$>$$ 10$$^{7}$$) for Am, and all the elements were recovered quantitatively.

Journal Articles

Development of the ERIX process for reprocessing spent FBR-MOX fuel; A Study on minor actinides separation process

Hoshi, Harutaka*; Wei, Y.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Proceedings of International Conference on Nuclear Energy System for Future Generation and Global Sustainability (GLOBAL 2005) (CD-ROM), 6 Pages, 2005/10

For the development of nuclear fuel cycle, it is one of the most important tasks to improve reprocessing more economically and efficiently. Especially, to establish the Fast Breeder Reactor (FBR) cycle system for the future, it is strongly desirable to develop a new reprocessing which uses more compact equipments and produces less radioactive wastes compared to the present PUREX process. For this purpose, we have proposed a novel aqueous reprocessing system named ERIX Process to treat spent FBR-MOX fuels. This process consists of (1) Pd removal by selective adsorption using a specific anion exchanger; (2) electrolytic reduction for the valence adjustment of the major actinides including U, Pu, Np and some fission products (FP) such as Tc and Ru; (3) anion exchange separation for the recovery of U, Pu and Np using a new type of anion exchanger, AR-01; and (4) selective separation of long-lived minor actinides (MA = Am and Cm) by extraction chromatography. In this work, MA separation process was studied.

JAEA Reports

Study of Cs Recovery by Extraction Chromatography (2)

Hoshi, Harutaka*; Zhang, A.*; Uchida, Hiromi*; Kuraoka, Etsushu*

JNC TJ8400 2005-011, 20 Pages, 2005/02

JNC-TJ8400-2005-011.pdf:0.86MB

In order to apply CalixR14 extractant to extraction chromatography for Cs separation, basic characteristics of CalixR14 adsorbent were studied. CalixR14 impregnated resin and CalixR14 + TBP impregnated resin were prepared. CalixR14 extractant showed no adsorption for Cs by liquid-liquid extraction and CalixR14 impregnated resin also showed no adsorption for Cs. Therefore, it is concluded that CalixR14 itself has no affinity for Cs. On the other hand, Cs was adsorbed onto CalixR14-TBP impregnated resin from a concentrated nitric acid solution. The distribution coefficients of Cs were more than 10 cm$$^{3}$$/g from 2 to 6 M nitric acid. While Rb showed week adsorption, Na, K, Sr and La showed no adsorption and separation factor was over 199. A slight amount of CalixR14 and TBP was leaked from impregnated resin into the aqueous phase. Separation from simulated liquid waste was carried out by using a column packed with CalixR14-TBP adsorbent. Na, K, Sr and La were not adsorbed onto the column, however, Cs and Rb were adsorbed onto the column. Cs and Rb were eluted from the column by water. Cs and Rb were quantitatively recovered.

Journal Articles

Electrolytic reduction of Tc(VII) in nitric acid solution using glassy carbon electrode

Hoshi, Harutaka*; Wei, Y.*; Kumagai, Mikio*; Asakura, Toshihide; Morita, Yasuji

Journal of Radioanalytical and Nuclear Chemistry, 262(3), p.601 - 605, 2005/01

Electroreduction of Tc(VII) in nitric acid solution using grassy carbon electrode was studied. The electroreduction was conducted at a constant potential -300 mV (vs. Ag/AgCl) with a potentiostat. It was found that difference of the Tc concentration in the solutions before and after the electrolysis was negligibly small. This means that there were almost no TcO$$_{2}$$ or Tc deposited on the carbon fiber electrode during the electroreduction. Absorption spectra and distribution coefficients obtained by ion-exchange analysis indicated that Tc(VII) was reduced to Tc(IV).

JAEA Reports

Experimental Study on a Novel Cation Exchanger (3)

Hoshi, Harutaka*; Zhang, A.*; Kuraoka, Etsushu*; Yamaguchi, Hiromi*

JNC TJ8420 2004-001, 23 Pages, 2004/02

JNC-TJ8420-2004-001.pdf:1.01MB

The separation behavior of rare earth in simulated high-level liquid waste was examined by using a cation exchanger, which is synthesized by embedding a macroreticular resin containing sulfonic acid group as exchanger site in porous silica particles.

JAEA Reports

Experimental Study on the Basic Characteristics of TODGA Adsorbent

Hoshi, Harutaka*; Zhang, A.*; Kuraoka, Etsushu*; Yamaguchi, Hiromi*

JNC TJ8410 2004-001, 26 Pages, 2004/02

JNC-TJ8410-2004-001.pdf:1.16MB

In order to apply the extraction chromatography for trivalent actinides (Am and Cm) recovery process from high level liquid waste, the basic characteristics of TODGA adsorbent were experimentally studied.

JAEA Reports

Experimental Study on Extraction Chromatography Using CMPO Adsorbent (3)

Hoshi, Harutaka*; Zhang, A.*; Kuraoka, Etsushu*

JNC TJ8410 2004-008, 27 Pages, 2003/12

JNC-TJ8410-2004-008.pdf:0.68MB

In order to investigate the possibility to realize an engineering system of extraction chromatographyusing CMPO adsorbent, experiments on CMPO leak and process flowsheet were carried out.

JAEA Reports

Experimental Study on Sr Separation by Extraction Chromatography

Kuraoka, Etsushu*; Zhang, A.*

JNC TJ8400 2003-073, 26 Pages, 2003/03

JNC-TJ8400-2003-073.pdf:0.95MB

In order to study the applicability of extraction chromatographic technology to the separation of Sr from high level liquid waste, a novel silica-supported Sr-adsorbent was prepared. Adsorption and separation experiments for Sr and other FP elements in nitric acid solution were carried out.

JAEA Reports

Experimental Study on a Novel Cation Exchanger (2)

Kuraoka, Etsushu*; Arai, Tsuyoshi*; Zhang, A.*

JNC TJ8420 2003-003, 25 Pages, 2003/02

JNC-TJ8420-2003-003.pdf:1.19MB

In order to study the applicability of the separation of Am, Cm and rare earths from each other by cation exchange technology, a novel silica-based cation exchanger (SiSCR) with sulfonic acid group as exchange site has been synthesized. Its thermo-decomposition property and the performance of adsorption, elution and separation for some rare earths were investigated.

JAEA Reports

Experimental Study on Extraction Chromatography Using CMPO Adsorbent (2)

Kuraoka, Etsushu*; Zhang, A.*; Arai, Tsuyoshi*

JNC TJ8400 2003-078, 43 Pages, 2002/12

JNC-TJ8400-2003-078.pdf:1.86MB

In order to study the applicability of extraction chromatography for minor actinides separation in the program of the Feasibility Study on Commercialized Fast Reactor Fuel Cycle Systems, basic characteristics of a novel silica-supported CMPO adsorbent was investigated.

Journal Articles

Preparation of novel silica-based R-BTP extraction-resins and their application to trivalent actinides and lanthanides separation

Wei, Y.*; Hoshi, Harutaka*; Kumagai, Mikio*; Asakura, Toshihide; Uchiyama, Gunzo*

Journal of Nuclear Science and Technology, 39(Suppl.3), p.761 - 764, 2002/11

To separate long-lived minor actinides and specific fission products such as Zr and Mo from nitrate acidic high-level liquid waste, we studied an advanced partitioning process by extraction chromatography using minimal organic solvent and compact equipment. In this work, we synthesized several new type of nitrogen donor ligands, 2,6-bi-(5,6-dialkyl-1,2,4-triazine-3-yl)-pyridine (R-BTP) with different alkyl groups and prepared novel silica-based extraction-resins by impregnating these ligands into the SiO$$_{2}$$-P support with a diameter of 50 $$mu$$m. The adsorption performance of $$^{243}$$Am and Ln (III) from nitrate solution was investigated. It was found that the adsorption behavior depends strongly on the alkyl group in R-BTP. ${it n}$Bu-BTP/SiO$$_{2}$$-P and ${it n}$Hex-BTP/SiO$$_{2}$$-P showed high absorbability and selectivity for Am (III) over Ln (III). The separation factor is about 10$$^{4}$$ for Am/Ce and near 10$$^{2}$$ for Am/Eu-Gd, respectively. Effective Am (III) separation form Ln (III) by extraction chromatography using R-BTP/SiO$$_{2}$$-P extraction-resins is expected.

JAEA Reports

Conceptual study of the equipment for MA recovery by extraction chromatography

Kuraoka, Etsushu*; *; Kumagai, Mikio*; *

JNC TJ8400 2002-005, 58 Pages, 2002/07

JNC-TJ8400-2002-005.pdf:2.94MB

In order to study the possibility of a pilot-plant-scale test for MA recovery process by extraction chromatography which has been evaluated to have the potentials of small construction area and low cost, this work investigated the process flow sheet, the configuration and installation layout of equipment. Furthermore, the treatment methods for the organic wastes such as CMPO adsorbent were examined. The proposed process consists of two separation columns packed with CMPO adsorbent, where the 1st one is for the recovery of MA, heavy RE, Zr and Mo from the HLLW and the 2nd one for the removal of the Zr and Mo from the effluent of the 1st column, recovering the MA and the heavy RE as a nitrate acidic solution. The results of the separation experiments using simulated HLLW solutions indicate that the expected separation performance for the main elements was achieved and the proposed process is principally applicable. In addition, the process has the advantages such as "salt-free", the possible recovery of Zr-Mo and Pd from HLLW. The process flow diagram for the proposed separation process was drawn and the mass balance for one test of pilot-plant-scale was evaluated. The structure and size of the main equipment including the separation columns were conceptually designed and the installation layout of the equipment was drawn. The cost of the equipment was preliminary estimated based the specification of the equipment. In addition, the effective treatment methods for the organic wastes including depleted CMPO adsorbent, DTPA or oxalic acid containing waste solution were examined based on article survey. Moreover, some exploratory experiments for the decomposition treatment of these wastes were conducted by using the Fenton reagents. Finally, the subjects remained in this process were extracted.

JAEA Reports

None

Kuraoka, Etsushu*; Arai, Tsuyoshi*

JNC TJ8420 2002-003, 35 Pages, 2002/03

JNC-TJ8420-2002-003.pdf:0.59MB

no abstracts in English

38 (Records 1-20 displayed on this page)