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Journal Articles

Flow-electrode CDI removes the uncharged Ca-UO$$_{2}$$-CO$$_{3}$$ ternary complex from brackish potable groundwater; Complex dissociation, transport, and sorption

Ma, J.*; Zhang, Y.*; Collins, R. N.*; Tsarev, S.*; Aoyagi, Noboru; Kinsela, A. S.*; Jones, A. M.*; Waite, T. D.*

Environmental Science & Technology, 53(5), p.2739 - 2747, 2019/03

 Percentile:100(Engineering, Environmental)

Journal Articles

Optical properties of trinuclear citrate complexes containing 4f and 5f block metals

Aoyagi, Noboru; Palladino, G.*; Nagasaki, Shinya*; Kimura, Takaumi

Bulletin of the Chemical Society of Japan, 91(6), p.882 - 890, 2018/06

 Percentile:100(Chemistry, Multidisciplinary)

The speciation and coordination geometries of M(III)-citrate complexes in aqueous solutions, where M denotes Eu, Tb, Lu, or Cm, are studied using potentiometric titration, nuclear magnetic resonance spectroscopies. Their photophysical properties are also characterized by time-resolved fluorescence spectra. The formation constants of mononuclear, dinuclear, and trinuclear Lu-citrate species were determined by potentiometric titration in 3.00 M NaClO$$_{4}$$ aqueous media. Terminal carboxylic conformation in trinuclear complexes comprised both the five- and six-membered rings at different exchanging rates. Hydration states evaluated for Eu$$^{3+}$$ ions are the chemical formula of [Eu(Cit)$$_{2}$$ (H$$_{2}$$ O)$$_{2.5}$$ ]$$^{3-}$$ and [Eu$$_{3}$$(OH)$$_{4}$$(Cit)$$_{4}$$(H$$_{2}$$O)$$_{3.4}$$]$$^{7-}$$. These complexes in aqueous solution have geometrical similarity to the crystal structures in the literature. Furthermore, the entity of the hetero-trinuclear complex induces the intramolecular energy transfer from Tb$$^{3+}$$ to Eu$$^{3+}$$. The incorporation of Cm$$^{3+}$$ into these homo/hetero-trinuclear citrate complexes proved to be a successful trial to probe the formation of actinide polymer at a trace level.

Journal Articles

Europium binding to humic substances extracted from deep underground sedimentary groundwater studied by time-resolved laser fluorescence spectroscopy

Saito, Takumi*; Aoyagi, Noboru; Terashima, Motoki

Journal of Nuclear Science and Technology, 54(4), p.444 - 451, 2017/04

 Times Cited Count:2 Percentile:42.02(Nuclear Science & Technology)

Humic substances (HSs) are ubiquitous in various environments including deep underground and play an important role in the speciation and mobility of radionuclides. The binding of Eu$$^{3+}$$, a chemical homologue of trivalent actinide ions, to HSs isolated from sedimentary groundwater at -250 m below the surface was studied by time-resolved laser fluorescence spectroscopy combined with parallel factor analysis (PARAFAC) as a function of pH and salt concentration. PARAFAC modeling reveals the presence of multiple factors that corresponds to different Eu$$^{3+}$$ species. These factors resemble those observed for Eu$$^{3+}$$ binding to HSs from surface environments; however, detailed comparison shows that there are some particularities in Eu$$^{3+}$$ binding to the deep groundwater HSs. The distribution coefficients ($$K_{rm d}$$) of Eu$$^{3+}$$ binding to the HSs calculated from the PARAFAC modeling exhibits a rather strong salt effect. At 0.01 M NaClO$$_{4}$$ the $$K_{rm d}$$ values are relatively large and comparable to those to the surface HSs; they are decreaed at 0.1 M NaClO$$_{4}$$ by more than an order of the magnitude. The $$K_{rm d}$$ values are larger for humic acid fraction of the deep underground HSs than fulvic acid over the entire range of pH and salt concentration investigated in this study.

JAEA Reports

Preliminary missions for the decommissioning of the laboratory building No.1 for the plutonium research program

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

JAEA-Technology-2016-039.pdf:5.24MB

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.

Journal Articles

Role of Tf$$_{2}$$N$$^{-}$$ anions in the ionic liquid-water distribution of europium(III) chelates

Okamura, Hiroyuki; Aoyagi, Noboru; Shimojo, Kojiro; Naganawa, Hirochika; Imura, Hisanori*

RSC Advances (Internet), 7(13), p.7610 - 7618, 2017/01

 Times Cited Count:8 Percentile:33.34(Chemistry, Multidisciplinary)

The role of bis(trifluoromethanesulfonyl)imide (Tf$$_{2}$$N$$^{-}$$) anions in the ionic liquid-water distribution systems of the Eu(III) chelates with 2-thenoyltrifluoroacetone (Htta) was investigated by the liquid-liquid distribution and time-resolved laser-induced fluorescence spectroscopy (TRLFS). The effect of the ionic liquids on the distribution constant of Eu(tta)$$_{3}$$ was evaluated by the regular solution theory. The distribution constant of Eu(tta)$$_{3}$$ in 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([C$$_{n}$$mim][Tf$$_{2}$$N]) was increased dramatically by the solvation effects of Eu(tta)$$_{3}$$ in [C$$_{n}$$mim][Tf$$_{2}$$N]. TRLFS for [Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$] synthesized revealed that the Eu(tta)$$_{3}$$ chelate was almost completely dehydrated in a series of [C$$_{n}$$mim][Tf$$_{2}$$N]. The Eu(tta)$$_{3}$$ chelate exists as di- or tri-hydrates in 1-ethyl-3-methylimidazolium perchlorate ([C$$_{2}$$mim][ClO$$_{4}$$]) containing 20 M water, whereas mono-hydrated chelate was formed in [C$$_{2}$$mim][Tf$$_{2}$$N, ClO$$_{4}$$] in the presence of 0.50 M Tf$$_{2}$$N$$^{-}$$ and 20 M water. These results show that the coordinated water molecules of [Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$] were replaced by the Tf$$_{2}$$N$$^{-}$$ anions. In fact, an anionic adduct, [Eu(tta)$$_{3}$$(Tf$$_{2}$$N)]$$^{-}$$, was observed by electrospray ionization mass spectrometry in the presence of [C$$_{4}$$mim][Tf$$_{2}$$N].

Journal Articles

Sorption of Eu$$^{3+}$$ on Na-montmorillonite studied by time-resolved laser fluorescence spectroscopy and surface complexation modeling

Sasaki, Takayuki*; Ueda, Kenyo*; Saito, Takumi; Aoyagi, Noboru; Kobayashi, Taishi*; Takagi, Ikuji*; Kimura, Takaumi; Tachi, Yukio

Journal of Nuclear Science and Technology, 53(4), p.592 - 601, 2016/04

 Times Cited Count:3 Percentile:57.25(Nuclear Science & Technology)

The influences of pH and the concentrations of Eu$$^{3+}$$ and NaNO$$_{3}$$ on the sorption of Eu$$^{3+}$$ to Na-montmorillonite were investigated through batch sorption measurements and time-resolved laser fluorescence spectroscopy (TRLFS). The pH had a little effect on the distribution coefficients (Kd) in 0.01 M NaNO$$_{3}$$, whereas the Kd strongly depended on pH at 1 M NaNO$$_{3}$$. A cation exchange model combined with a one-site non-electrostatic surface complexation model was successfully applied to the measured Kd. The TRLFS spectra of Eu$$^{3+}$$ sorbed were processed by parallel factor analysis (PARAFAC), which corresponded to one outer-sphere (factor A) and two inner-sphere (factor B and C) complexes. It turned out that factors A and B correspond to Eu$$^{3+}$$ sorbed by ion exchange sites and inner-sphere complexation with hydroxyl groups of the edge faces, respectively. Factor C became dominant at relatively high pH and ionic strength and likely correspond to the precipitation of Eu(OH)$$_{3}$$ on the surface.

Journal Articles

Physicochemical and ion-binding properties of highly aliphatic humic substances extracted from deep sedimentary groundwater

Saito, Takumi; Terashima, Motoki; Aoyagi, Noboru; Nagao, Seiya*; Fujitake, Nobuhide*; Onuki, Toshihiko

Environmental Science; Processes & Impacts, 17(8), p.1386 - 1395, 2015/08

 Times Cited Count:3 Percentile:78.45(Chemistry, Analytical)

The deep groundwater HSs were different from surface HSs, having high aliphaticities, sulfur contents, and small molecular sizes. The amounts of their acidic functional groups were comparable to or slightly larger than those of surface HSs; however, the magnitude of Cu$$^{2+}$$ binding to the deep groundwater HSs was smaller. The NICA-Donnan model attributed this to the binding of Cu$$^{2+}$$ to chemically homogeneous carboxylic-type sites via mono-dentate coordination at relatively low pH. The binding mode tended to shift to multi-dentate coordination with carboxylic-type and probably more heterogeneous alcoholic hydroxide-type groups at higher pH. This study shows the particularity of the deep groundwater HSs in terms of their physicochemical and ion-binding properties, compared with surface HSs.

Journal Articles

Uranium binding mechanisms of the acid-tolerant fungus ${{it Coniochaeta fodinicola}}$

V$'a$zquez-Campos, X.*; Kinsela, A. S.*; Collins, R. N.*; Neilan, B. A.*; Aoyagi, Noboru; Waite, T. D.*

Environmental Science & Technology, 49(14), p.8487 - 8496, 2015/07

 Times Cited Count:10 Percentile:40.86(Engineering, Environmental)

The uptake and binding of uranium by a moderately acidophilic fungus, ${{it Coniochaeta fodinicola}}$, recently isolated from a uranium mine site, is examined in this work in order to better understand the potential impact of organisms such as this on uranium sequestration in hydrometallurgical systems. Our results show that the viability of the fungal biomass is critical to their capacity to remove uranium from solution. Indeed, live biomass were capable of removing 16 mg U/g dry weight in contrast with dead biomass which removed 45 mg U/g dry weight after 2 h. Furthermore, the uranium binds with different strength, with a fraction ranging from 20-50 % being easily leachable from the exposed biomass by a 10 min acid washing. Results from X-ray absorption spectroscopy measurements show that the strength of uranium binding is strongly influenced by cell viability, with live cells showing a more well-ordered uranium bonding environment, while the distance to carbon or phosphorus second neighbours is similar in all samples. When coupled with laser spectroscopy, the importance of organic acids and phosphates, and polysaccharides, likely released with fungal cell death, appear to be the primary determinants of uranium binding in this system. These results provide an important progression to our understanding with regard to uranium sequestration in hydrometallurgical applications.

Journal Articles

Photophysical property of $$catena$$-bis(thiocyanato)aurate(I) complexes in ionic liquids

Aoyagi, Noboru; Shinha, Yusuke*; Ikeda, Atsushi*; Haga, Yoshinori; Shimojo, Kojiro; Brooks, N. R.*; Izuoka, Akira*; Naganawa, Hirochika; Kimura, Takaumi; Binnemans, K.*

Crystal Growth & Design, 15(3), p.1422 - 1429, 2015/03

 Times Cited Count:7 Percentile:31.11(Chemistry, Multidisciplinary)JP, 2009-116985   Licensable Patent Information Database   Patent publication (In Japanese)

The photochemistry of a gold(I) thiocyanate complex has been investigated to determine the coordination structure in both the solid and liquid states. The coordination geometries of the supramolecular complex and the concomitant exciplex have mainly been analyzed by crystallographic analysis and X-ray absorption spectroscopy. The Au-S bond distance and Au-Au separation of the compound in the ground state and in the phosphorescent excited state were compared. Upon irradiation with UV light, the excimeric interactions were enhanced, resulting in a contraction of the Au-Au aurophilic distance. A broad luminescence spectrum was observed for the one-dimensional chain suprastructure. The time-resolved luminescence spectra indicated the entity of several oligomeric species in the crude liquid without neutral solvent molecules. In addition, EXAFS spectroscopy exhibited a slight change in the nearest Au-S distance due to the photo-switched transformation. The deformation of the (Au-Au)* exciplexes was not apparently promoted in the liquid state with the asymmetrical imidazoium cations having a non-local charge distribution in the present observation. This is plausibly due to a flexible molecular structure and a property in the liquid state. In conclusion, the photo-excited nature of the pseudo-one dimensional complexes is emerged in controlling bond distances among the supramolecular networks.

Journal Articles

Optical properties of tetravalent uranium complexes in non-aqueous media

Aoyagi, Noboru; Watanabe, Masayuki; Kirishima, Akira*; Sato, Nobuaki*; Kimura, Takaumi

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1095 - 1098, 2015/02

 Times Cited Count:2 Percentile:66.76(Chemistry, Analytical)

Journal Articles

Time-resolved laser-induced fluorescence spectroscopy combined with parallel factor analysis; A Robust speciation technique for UO$$_{2}$$$$^{2+}$$

Saito, Takumi; Aoyagi, Noboru; Kimura, Takaumi

Journal of Radioanalytical and Nuclear Chemistry, 303(2), p.1129 - 1132, 2015/02

 Times Cited Count:7 Percentile:22.72(Chemistry, Analytical)

Time-resolved laser-induced fluorescence spectroscopy (TRLFS) is a powerful speciation technique for fluorescent metal ions and can be further improved by combining with multi-mode factor analysis such as parallel factor analysis (PARAFAC). This study demonstrates the applicability of TRLFS combined with PARAFAC for the speciation of uranyl (UO$$_{2}$$$$^{2+}$$) in the presence of silicic acid (Si(OH)$$_{4}$$). A series of TRLFS data with varied Si(OH)$$_{4}$$ concentration was processed by PARAFAC, resulting in three factors corresponding to free UO$$_{2}$$$$^{2+}$$, UO$$_{2}$$SiO(OH)$$_{3}$$$$^{+}$$, and UO$$_{2}$$OH$$^{+}$$. The stability constant of UO$$_{2}$$SiO(OH)$$_{3}$$$$^{+}$$ was further optimized, based on the intensity profiles of the factors.

Journal Articles

Radioactive fallout cesium in sewage sludge ash produced after the Fukushima Daiichi nuclear accident

Kozai, Naofumi; Suzuki, Shinichi; Aoyagi, Noboru; Sakamoto, Fuminori; Onuki, Toshihiko

Water Research, 68, p.616 - 626, 2015/01

 Times Cited Count:13 Percentile:21.5(Engineering, Environmental)

The radioactive fallout cesium ($$^{137}$$Cs) in the sewage sludge ashes (SSAs) produced after the Fukushima Daiichi Nuclear Accident was tested. Two of tested five SSAs contained $$^{137}$$Cs above the radioactivity criterion for controlled landfill disposal in Japan. The minerals of SSAs are divided into two groups: an HCl-soluble phase mainly composed of phosphates and metal oxides; and silicates. The majority of $$^{137}$$Cs was contained in the HCl-soluble phase. Among the HCl-soluble subphases, Fe-bearing phases, probably iron oxides, were mainly responsible for $$^{137}$$Cs retention. Pre-pulverizing SSAs and heating them in an aqueous HCl was the most effective method of dissolving the HCl-soluble phase. The radioactivity concentrations of $$^{137}$$Cs in all the HCl-treatment residues were below the criterion. This residue was mostly composed of silicates. Static leaching tests of the residue revealed that $$^{137}$$Cs is very stably immobilized in the silicates.

JAEA Reports

Stabilization of uranium hexafluoride by hydrolysis method for decommissioning of safeguard laboratory facility

Inagawa, Jun; Hotoku, Shinobu; Oda, Tetsuzo; Aoyagi, Noboru; Magara, Masaaki

JAEA-Technology 2014-007, 48 Pages, 2014/03

JAEA-Technology-2014-007.pdf:5.76MB

In safeguard laboratory (SGL) facility of Nuclear Science Research Institute of JAEA, uranium hexafluoride (UF$$_{6}$$) of enriched uranium of various enrichment was used for research and development of a spectrometric method for the determination of the enrichment of uranium in April 1983 through March 1993. After completion of this R&D, the UF$$_{6}$$ has been stored in SGL facility. It was decided that the UF$$_{6}$$ is carried to out of the facility, because the SGL facility will be decommissioning until March 2015. To transport and store in safety after transportation, it is necessary that the UF$$_{6}$$ should be converted to stable chemical form. Hydrolysis of UF$$_{6}$$ to uranyl fluoride (UO$$_{2}$$F$$_{2}$$) and evaporation to solid state were selected for the stabilization method. The equipment for hydrolysis and evaporation was installed in the SGL facility. Stabilization was operated in this equipment, and all of the UF$$_{6}$$ in the SGL facility was converted to UO$$_{2}$$F$$_{2}$$ solid state in October 2012 through August 2013. In this report, results of examination and operation for stabilization of UF$$_{6}$$ were reported.

Journal Articles

Highly efficient extraction separation of lanthanides using a diglycolamic acid extractant

Shimojo, Kojiro; Aoyagi, Noboru; Saito, Takumi*; Okamura, Hiroyuki; Kubota, Fukiko*; Goto, Masahiro*; Naganawa, Hirochika

Analytical Sciences, 30(2), p.263 - 269, 2014/02

 Times Cited Count:23 Percentile:17.78(Chemistry, Analytical)

Journal Articles

Speciation of actinides by laser spectroscopy

Aoyagi, Noboru; Saito, Takumi*; Kimura, Takaumi

Bunseki, 2013(9), p.536 - 542, 2013/09

no abstracts in English

Journal Articles

Luminescence and potentiometric studies on the complexation of europium(III) by picolinate in an aqueous solution

Aoyagi, Noboru; Toraishi, Takashi*; Nagasaki, Shinya*; Tanaka, Satoru*

Journal of Applied Solution Chemistry and Modeling, 1(2), p.148 - 155, 2012/12

Journal Articles

Specific cooperative effect of a macrocyclic receptor for metal ion transfer into an ionic liquid

Okamura, Hiroyuki; Ikeda, Atsushi*; Saito, Takumi*; Aoyagi, Noboru; Naganawa, Hirochika; Hirayama, Naoki*; Umetani, Shigeo*; Imura, Hisanori*; Shimojo, Kojiro

Analytical Chemistry, 84(21), p.9332 - 9339, 2012/11

 Times Cited Count:18 Percentile:34.34(Chemistry, Analytical)

Journal Articles

Speciation of Eu$$^{3+}$$ bound to humic substances by time-resolved laser fluorescence spectroscopy (TRLFS) and parallel factor analysis (PARAFAC)

Lukman, S.*; Saito, Takumi*; Aoyagi, Noboru; Kimura, Takaumi; Nagasaki, Shinya*

Geochimica et Cosmochimica Acta, 88, p.199 - 215, 2012/07

 Times Cited Count:15 Percentile:40.89(Geochemistry & Geophysics)

Journal Articles

Surface speciation of Eu$$^{3+}$$ adsorbed on kaolinite by time-resolved laser fluorescence spectroscopy (TRLFS) and parallel factor analysis (PARAFAC)

Ishida, Keisuke*; Saito, Takumi*; Aoyagi, Noboru; Kimura, Takaumi; Nagaishi, Ryuji; Nagasaki, Shinya*; Tanaka, Satoru*

Journal of Colloid and Interface Science, 374(1), p.258 - 266, 2012/05

 Times Cited Count:16 Percentile:49.77(Chemistry, Physical)

Journal Articles

Laser-induced fluorescence and infrared spectroscopic studies on the specific solvation of tris(1-(2-thienyl)-4,4,4-trifluoro-1,3-butanedionato)europium(III) in an ionic liquid

Okamura, Hiroyuki; Sakae, Hiroki*; Kidani, Keiji*; Hirayama, Naoki*; Aoyagi, Noboru; Saito, Takumi*; Shimojo, Kojiro; Naganawa, Hirochika; Imura, Hisanori*

Polyhedron, 31(1), p.748 - 753, 2012/01

 Times Cited Count:18 Percentile:14.9(Chemistry, Inorganic & Nuclear)

99 (Records 1-20 displayed on this page)