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Journal Articles

Extraction properties of trivalent rare earth ions from nitric acid using a triamide-amine extractant

Uchino, Seiko*; Narita, Hirokazu*; Kita, Keisuke*; Suzuki, Hideya*; Matsumura, Tatsuro; Naganawa, Hirochika*; Sakaguchi, Koichi*; Oto, Keisuke*

Solvent Extraction Research and Development, Japan, 30(1), p.39 - 46, 2023/00

The extraction of trivalent rare earth ions (RE$$^{3+}$$) from HNO$$_{3}$$ solution using a triamide amine, tris(N,N-di-2-ethylhexyl-ethylamide)amine (DEHTAA), was conducted, and the extraction mechanism was estimated from extraction behavior of HNO$$_{3}$$ and RE$$^{3+}$$ and the relationship between atomic number and extraction percentages (E%) for RE$$^{3+}$$. A DEHTAA molecule dominantly formed a DEHTAA HNO$$_{3}$$ at 1.0 M HNO$$_{3}$$ and a DEHTAA(HNO$$_{3}$$)$$_{2}$$ at 6.0 M HNO$$_{3}$$ in the acid-equilibrated organic phase. This would provide the unique dependence of E% for the light RE$$^{3+}$$ on the HNO$$_{3}$$ concentration, in which the E% value had a minimum and maximum at $$sim$$0.5 M and $$sim$$2 M HNO$$_{3}$$, respectively. The results of the slope analyses for the distribution ratios for RE$$^{3+}$$ suggested that the dominant RE$$^{3+}$$ complex was RE(NO$$_{3}$$)$$_{3}$$DEHTAA(DEHTAA HNO$$_{3}$$) at 1.0 M HNO$$_{3}$$. The E% for RE$$^{3+}$$ decreased from La$$^{3+}$$ to Lu$$^{3+}$$ at 1.0 M HNO$$_{3}$$; on the other hand, those increased from La$$^{3+}$$ to Nd$$^{3+}$$ at 0.25 M and from La$$^{3+}$$ to Sm$$^{3+}$$ and 6.0 M HNO$$_{3}$$.

Journal Articles

Urea-introduced ionic liquid for the effective extraction of Pt(IV) and Pd(II) ions

Ueda, Yuki; Eguchi, Ayano; Tokunaga, Kohei; Kikuchi, Kei*; Sugita, Tsuyoshi; Okamura, Hiroyuki; Naganawa, Hirochika

Industrial & Engineering Chemistry Research, 61(19), p.6640 - 6649, 2022/05

 Times Cited Count:0 Percentile:13.93(Engineering, Chemical)

no abstracts in English

Journal Articles

Synergistic enhancement of the extraction and separation efficiencies of lanthanoid(III) ions by the formation of charged adducts in an ionic liquid

Okamura, Hiroyuki; Mizuno, Masayoshi*; Hirayama, Naoki*; Shimojo, Kojiro; Naganawa, Hirochika; Imura, Hisanori*

Industrial & Engineering Chemistry Research, 59(1), p.329 - 340, 2020/01

 Times Cited Count:14 Percentile:58.64(Engineering, Chemical)

The synergistic ionic-liquid extraction and extraction equilibrium of lanthanoid(III) (Ln(III)) ions have been investigated using 2-thenoyltrifluoroacetone (Htta) and trioctylphosphine oxide (TOPO) in the ionic liquid 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([C$$_{4}$$mim][Tf$$_{2}$$N]). The selective synergistic effect for heavier Ln(III) ions was found using a combination of Htta and TOPO in [C$$_{4}$$mim][Tf$$_{2}$$N], leading to enhanced separability among Ln(III) ions. The extracted Ln(III) species and the extraction constants in the Htta-TOPO system were determined by three-dimensional extraction equilibrium analysis. The selective synergism for heavier Ln(III) ions in the Htta-TOPO system was ascribed to the formation of hydrophobic, charged adducts, such as Ln(tta)$$_{2}$$(TOPO)$$_{3}$$$$^{+}$$ and Ln(tta)(TOPO)$$_{3}$$$$^{2+}$$, in [C$$_{4}$$mim][Tf$$_{2}$$N].

Journal Articles

Continuous liquid-liquid extraction of uranium from uranium-containing wastewater using an organic phase-refining-type emulsion flow extractor

Nagano, Tetsushi; Naganawa, Hirochika; Suzuki, Hideya; Toshimitsu, Masaaki*; Mitamura, Hisayoshi*; Yanase, Nobuyuki*; Grambow, B.

Analytical Sciences, 34(9), p.1099 - 1102, 2018/09

 Times Cited Count:12 Percentile:46.41(Chemistry, Analytical)

A previously reported emulsion flow (EF) extraction system does not include a device for refining used solvent. Therefore, the processing of large quantities of wastewater by using the EF extractor alone could lead to the accumulation of wastewater components into the solvent and diminished extraction performance. In the present study, we have developed a solvent-washing-type EF system, which is equipped with a unit for washing used solvent to prevent accumulation, and successfully applied it for treating uranium-containing wastewater.

Journal Articles

Recontamination prevention technologies to prevent radioactive cesium from its runoff from not decontaminated forests to living areas

Nagasu, Ryosuke*; Tanabe, Daijiro*; Yokotsuka, Satoshi*; Kumazawa, Noriyuki*; Ajiki, Takaya*; Aizawa, Yusuke*; Naganawa, Hirochika; Nagano, Tetsushi; Yanase, Nobuyuki*; Mitamura, Hisayoshi*; et al.

Kankyo Joka Gijutsu, 17(2), p.58 - 61, 2018/03

A new technology to suppress cesium migration from forests has been developed collaboratively by Ibaraki University, Kumagai-gumi Co., Ltd. and its group company, Technos, and JAEA. The new technology utilizes polyelectrolytes (polymers with electric charges) and clay minerals to control Cs migration with the aid of natural forces such as rainfall and rainwater runoff. In Imitate-mura, Fukushima, verification tests of the new technology have been performed and its effect on controlling Cs migration from forests to grass farm adjoining the forests has been proven.

Journal Articles

New liquid-liquid extraction apparatus; "Emulsion-flow" extractor

Naganawa, Hirochika

Bunseki Kagaku, 66(11), p.797 - 808, 2017/11


 Times Cited Count:6 Percentile:23.08(Chemistry, Analytical)

A new liquid-liquid extraction method, called the emulsion-flow method, has recently been developed at Japan Atomic Energy Agency (JAEA). The emulsion-flow method, where low cost, simplicity, high efficiency, compactness, safety, and eco-friendly go together, has attracted attention, and has been expected to bring innovation to liquid-liquid extraction technologies. Compared with conventional industrial apparatuses, an emulsion-flow apparatus successfully combines the lowest cost superior to a spray column and the highest performance (the highest efficiency and the highest processing speed) comparable to a centrifugal extractor. Furthermore, the emulsion-flow method can also be used for collecting particulate components by utilizing their aggregation onto a liquid-liquid interface and for purifying water polluted by oil with its remarkable phase-separating ability.

Journal Articles

A Comprehensive extraction study using a mono-alkylated diglycolamic acid extractant; Comparison between a secondary amide group and a tertiary amide group

Sugita, Tsuyoshi; Fujiwara, Iori*; Okamura, Hiroyuki; Oshima, Tatsuya*; Baba, Yoshinari*; Naganawa, Hirochika; Shimojo, Kojiro

Solvent Extraction Research and Development, Japan, 24(2), p.61 - 69, 2017/05

We investigated an influence of amide group in diglycolamic acid-type extractants on extraction property of metal ions. The extraction characteristics of $$N$$-dodecyldiglycolamic acid (C$$_{12}$$DGAA), with a secondary amide group, for 56 metal ions have been investigated, and compared with those of $$N,N$$-dioctyldiglycolamic acid (DODGAA) with a tertiary amide group. Compared with DODGAA, C$$_{12}$$DGAA has a poor extraction performance and separation ability for rare-earth metal ions, except for Sc(III). However, C$$_{12}$$DGAA tended to provide better extraction for relatively small-sized metal ions than DODGAA. In addition, it was found that C$$_{12}$$DGAA enables the selective removal of Hg(II) from aqueous solutions containing various divalent metal ions.

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:18 Percentile:57.24(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

Extraction behavior of rare-earth elements using a mono-alkylated diglycolamic acid extractant

Shimojo, Kojiro; Fujiwara, Iori*; Fujisawa, Kiyoshi*; Okamura, Hiroyuki; Sugita, Tsuyoshi; Oshima, Tatsuya*; Baba, Yoshinari*; Naganawa, Hirochika

Solvent Extraction Research and Development, Japan, 23(2), p.151 - 159, 2016/05

Liquid-liquid extraction of rare-earth (RE) cations has been investigated using $$N$$-dodecyldiglycolamic acid (C$$_{12}$$DGAA) with a secondary amide group, and compared with that using $$N,N$$-dioctyldiglycolamic acid (DODGAA) with a tertiary amide group. C$$_{12}$$DGAA enables quantitative transfer of all RE cations from moderately acidic solution, while being selective toward the heavier RE cations, and performs better than typical carboxylic-acid-type extractants. However, C$$_{12}$$DGAA provides low extraction performance and separation ability for RE cations compared with DODGAA because of the weaker basicity of the amide oxygen. Slope analysis demonstrated that RE$$^{3+}$$ transfer with C$$_{12}$$DGAA proceeded through a proton-exchange reaction, forming a 1:3 complex, RE(C$$_{12}$$DGAA)$$_{3}$$. Structural characterization by X-ray diffraction revealed that three $$N$$-butyldiglycolamic acid (C$$_{4}$$DGAA) molecules coordinated to the La$$^{3+}$$ central ion in a tridentate fashion and the La$$^{3+}$$ primary coordination sphere consisted of three oxygen atoms from the amide group, three oxygen atoms from the ether group, and three oxygen atoms from the carboxy group.

Journal Articles

Decontamination and volume reduction of cesium-contaminated soil by combining soil solidification with interpolyelectrolyte complex and wet classification

Yamashita, Yuji*; Yanase, Nobuyuki; Nagano, Tetsushi; Mitamura, Hisayoshi; Naganawa, Hirochika

Journal of Radioanalytical and Nuclear Chemistry, 305(2), p.583 - 587, 2015/08

 Times Cited Count:5 Percentile:40.2(Chemistry, Analytical)

We propose a method for the decontamination and waste volume reduction of cesium-contaminated soil. The soils were solidified with an interpolyelectrolyte complex solution and classified into several size fractions by wet sieving. $$gamma$$-ray spectrometry of these fractions showed that the distribution ratio of the activity concentration of coarse soil particles decreased, whereas that of soil particles under 0.075 mm increased relative to reference samples. Results show that the fine soil particles, on which radioactive cesium accumulates, were removed from the surface of the coarse soil particles during, and remained in the washing water.

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:40.2(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.

JAEA Reports

The Uranium waste fluid processing examination by liquid and liquid extraction method using the emulsion flow method

Kanda, Nobuhiro; Daiten, Masaki; Endo, Yuji; Yoshida, Hideaki; Mita, Yutaka; Naganawa, Hirochika; Nagano, Tetsushi; Yanase, Nobuyuki

JAEA-Technology 2015-007, 43 Pages, 2015/03


The centrifuge which has the subtlety information concerning the nuclear nonproliferation used for uranium enrichment technical development exists in the uranium enrichment facilities of Ningyo-toge Environmental Engineering Center, Japan Atomic Energy Agency. This centrifugal is performing separation processing of the radioactive material adhering to the surface of parts by wet decontamination of ultrasonic cleaning by dilute sulfuric acid and water, etc. By removing the uranium contained in waste fluid, generated sludge reduces activity concentration. And the possibility of reduction of sludge processing is examined. For this reason, from the 2007 fiscal year, Nuclear Science and Engineering Directorate and cooperation are aimed at, and development of the extraction separation technology of the "uranium" by the emulsion flow method is furthered. The test equipment using the developed emulsion flow method was tested. And dilute sulfuric acid and water were used for the examination as actual waste fluid. The result checked whether the various performances in Basic test carried out in Nuclear Science and Engineering Directorate would be obtained.

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:11 Percentile:64.65(Chemistry, Multidisciplinary)

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

On-site monitoring method of radioactive cesium in water sample using cesium adsorption disk and GM survey meter

Nagano, Tetsushi; Mitamura, Hisayoshi; Yanase, Nobuyuki; Naganawa, Hirochika; Yasuda, Kenichiro; Yamaguchi, Hiroaki*

Hoshasei Busshitsu No Kyuchaku, Josen Oyobi Taihoshasen Gjutsu Ni Okeru Zairyo, Seko, Sokutei No Shin Gijutsu, p.400 - 408, 2014/11

A method for monitoring radioactive cesium concentration in water using a cesium adsorption disk and a GM survey meter has been developed to ascertain whether the water quality meets standards on radiological contaminants in water. This method was successfully applied to monitoring of decontaminated water of an outdoor school swimming pool in Date City after Fukushima Daiichi Nuclear Power Plant accident.

Journal Articles

Intramolecular cooperative effect of a macrocyclic receptor bearing $$beta$$-diketone fragments on the extraction of strontium into an ionic liquid

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

Proceedings of 20th International Solvent Extraction Conference (ISEC 2014), p.1046 - 1051, 2014/09

Journal Articles

Comprehensive extraction separation study of metal ions using $$N,N$$-dioctyldiglycolamic acid DODGAA

Shimojo, Kojiro; Naganawa, Hirochika

Proceedings of 20th International Solvent Extraction Conference (ISEC 2014), p.1052 - 1057, 2014/09

Journal Articles

Comprehensive extraction study using $$N$$,$$N$$-dioctyldiglycolamic acid

Shimojo, Kojiro; Nakai, Ayaka*; Okamura, Hiroyuki; Saito, Takumi*; Ohashi, Akira*; Naganawa, Hirochika

Analytical Sciences, 30(4), p.513 - 517, 2014/04

 Times Cited Count:13 Percentile:48.79(Chemistry, Analytical)

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:46 Percentile:86.36(Chemistry, Analytical)

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:7 Percentile:27.84(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 liquid-liquid extraction of nickel from simulated electroless nickel plating liquid wastes by using a counter current emulsion flow extractor

Nagano, Tetsushi; Mitamura, Hisayoshi; Yamashita, Yuji; Yanase, Nobuyuki; Suzuki, Hideya; Naganawa, Hirochika

Solvent Extraction Research and Development, Japan, 21(1), p.111 - 117, 2014/00

Simulated electroless nickel plating liquid wastes have been processed by using an emulsion flow extractor of a counter current type with a special focus on influences of dilution of the liquid wastes on the extraction performance. The emulsion flow extractor provides an efficient liquid-liquid extraction by sending solutions without additional stirring or shaking. A solvent used in the present study was Shellsol D70 solution containing LIX84-I as an extractant for nickel and PC88A as an accelerating agent. As a result, it was found that increasing degree of dilution with water resulted in improvement of nickel extractabilities obtained from the emulsion flow experiments with a maximum value of 96% as well as those obtained from batch experiments. Droplet sizes at the lower and the upper sides of emulsion phases, estimated by using high-speed microscope, were 214 $$pm$$ 36 $$mu$$m and 415 $$pm$$ 110 $$mu$$m, respectively.

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