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Journal Articles

Effect of oxygen-donor charge on adjacent nitrogen-donor interactions in Eu$$^{3+}$$ complexes of mixed N,O-donor ligands demonstrated on a 10-fold [Eu(TPAMEN)]$$^{3+}$$ chelate complex

Schnaars, K.; Kaneko, Masashi; Fujisawa, Kiyoshi*

Inorganic Chemistry, 60(4), p.2477 - 2491, 2021/02

https://doi.org/10.1021/acs.inorgchem.0c03405
 Times Cited Count：6 Percentile：59.03(Chemistry, Inorganic & Nuclear)

To reduce high-level radiotoxic waste generated by nuclear power plants, highly selective separation agents for minor actinides are mandatory. The mixed N,O-donor ligand ${it N,N,N',N'}$-tetrakis[(6-carboxypyridin-2-yl)methyl]ethylenediamine (H$$_{4}$$TPAEN) has shown good performance as a masking agent in Am$$^{3+}$$/Eu$$^{3+}$$ separation studies. In this work, we examine whether a decrease in O-donor basicity can promote the M$$^{3+}$$-N$$_{am}$$ interactions. Therefore, we replace the deprotonated "charged" carboxylic acid groups of TPAEN$$^{4-}$$ by neutral amide groups and introduce ${it N,N,N',N'}$-tetrakis[(6-${it N",N"}$-diethylcarbamoylpyridin-2-yl)methyl]ethylenediamine (TPAMEN) as a new ligand. TPAMEN was crystallized with Eu(OTf)$$_{3}$$ and Eu(NO$$_{3}$$)$$_{3}$$ 6H$$_{2}$$O to form positively charged 1:1 [Eu(TPAMEN)]$$^{3+}$$ complexes in the solid state. Alterations in the M-O/N bond distances are compared to [Eu(TPAEN)]$$^{-}$$ and investigated by DFT calculations to expose the differences in charge/energy density distributions at europium(III) and the donor functionalities of the TPAEN$$^{4-}$$ and TPAMEN. On the basis of estimations of the bond orders, atomic charges spin populations, and density of states in the Eu and potential Am and Cm complexes, the specific contributions of the donor-metal interaction are analyzed. The prediction of complex formation energy differences for the [M(TPAEN)]$$^{-}$$ and [M(TPAMEN)]$$^{3+}$$ (M$$^{3+}$$ = Eu$$^{3+}$$, Am$$^{3+}$$) complexes provide an outlook on the potential performance of TPAMEN in Am$$^{3+}$$/Eu$$^{3+}$$ separation.

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

http://doi.org/10.15261/serdj.23.151

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.

JAEA Reports

Two-dimensional analysis for a scrapeoff and divertor regions with an MHD model; Conceptual design study of FY86 FER

*; *; Hitoki, Shigehisa*; Fujisawa, Noboru; Sugihara, Masayoshi; Yamamoto, Shin; Mizoguchi, Tadanori*; Abe, Mitsushi*; *; *; et al.

JAERI-M 87-119, 19 Pages, 1987/08

JAERI-M-87-119.pdf:0.5MB

no abstracts in English

JAEA Reports

Preliminary analysis on plasma equilibrium control; Conceptual design study of FY86 FER

Abe, Mitsushi*; *; *; *; *; *; Shinya, K.*; Sugihara, Masayoshi; Hatayama, Akiyoshi*; Hitoki, Shigehisa*; et al.

JAERI-M 87-116, 13 Pages, 1987/08

JAERI-M-87-116.pdf:0.49MB

no abstracts in English

JAEA Reports

Effect of discrete RF spectrum on fast wave current drive; Conceptual design study of FY86 FER

*; *; Sugihara, Masayoshi; Yamamoto, Shin; Mizoguchi, Tadanori*; Hitoki, Shigehisa*; Abe, Mitsushi*; *; *; *; et al.

JAERI-M 87-110, 11 Pages, 1987/08

JAERI-M-87-110.pdf:0.38MB

no abstracts in English

JAEA Reports

Consistency between current ramp-up/recharging scenario by non-inductive current drive and dense and cold divertor plasma; Conceptual design study of FY86 FER

Hitoki, Shigehisa*; Sugihara, Masayoshi; Yamamoto, Shin; Abe, Mitsushi*; *; *; *; *; Shinya, K.*; Hatayama, Akiyoshi*; et al.

JAERI-M 87-109, 33 Pages, 1987/08

JAERI-M-87-109.pdf:0.81MB

no abstracts in English

JAEA Reports

Plasma physics design and major specifications of candidate reactors for FER design studies; Conceptual design study of FY86 FER

Sugihara, Masayoshi; Mizoguchi, Tadanori*; Hatayama, Akiyoshi*; Shinya, K.*; Yamamoto, Shin; Abe, Mitsushi*; *; *; *; *; et al.

JAERI-M 87-108, 49 Pages, 1987/08

JAERI-M-87-108.pdf:1.42MB

no abstracts in English

JAEA Reports

Main physics features driving design concept and physics design constraints; Conceptual design study of FY86 FER

Fujisawa, Noboru; Sugihara, Masayoshi; Yamamoto, Shin; Mizoguchi, Tadanori*; Hitoki, Shigehisa*; Abe, Mitsushi*; *; *; *; *; et al.

JAERI-M 87-093, 64 Pages, 1987/07

JAERI-M-87-093.pdf:1.45MB

no abstracts in English

Oral presentation

Decomposition of chlorinated phenol, benzoic acid and benzylamine by $$gamma$$-ray irradiation in zeolite-water mixture

Sugawara, Atsushi*; Kumagai, Yuta; Watanabe, Masayuki; Kimura, Atsushi*; Taguchi, Mitsumasa*; Fujisawa, Kiyoshi*

no journal, , 

Radiation-induced decomposition of three chlorinated aromatic compounds in zeolite-water mixture was studied, in order to evaluate decomposition yields of the aromatics adsorbed on the zeolite. The adsorption and condensation in zeolite pore structure has a possibility to improve the decomposition yield of aqueous organics in treatments of environmental water using ionizing radiations. In this study, the decomposition yields of 4-chlorophenol (4-ClPh), 4-chlorobenzoic acid (4-ClBAc), 4-chlorobenzylamine(4-ClBAm) were examined. The decomposition yield of adsorbed 4-ClBAm was lower than that in pure water. On the other hand, adsorbed 4-ClPh decomposed at a yield as high as in pure water. Moreover, a slight increase in the yield was overserved for 4-ClBAc. These results suggest that the decomposition yields of adsorbed aromatics are dependent on the reactivity with carriers of energy transfer from solid zeolite framework to water in the pore.

Oral presentation

Synthesis of rare-earths complex with MA separation reagent, TPEN and its derivatives

Murayama, Tatsuya*; Watanabe, Masayuki; Fujisawa, Kiyoshi*

no journal, , 

In this presentation, N,N,N',N'-Tetrakis(2-pyridylmethyl)ethylenediamine(TPEN) and the derivative, N,N,N',N'-Tetrakis(2-pyridylmethyl)-1,2-propanediamine(MeTPEN) which methylene chain was substituted by methyl group were used as ligand to synthesize europium complexes and which molecular structures and properties were compared by using spectroscopic methods.

Oral presentation

Synthesis of rare earth complexes using minor actinides separation reagent TPEN and derivatives

Murayama, Tatsuya*; Watanabe, Masayuki; Aoyagi, Noboru; Fujisawa, Kiyoshi*

no journal, , 

In this study, we synthesized Eu(III) complex using N,N,N',N'-tetrakis(2-pyridylmethyl)-ethylenediamine (TPEN) and TPEN derivatives, N,N,N',N'-tetrakis(2-pyridylmethyl)-propylenediamine(MeTPEN) which has methyl group into the ethylenediamine framework, the structure and physical properties of these complexes investigated. The crystal structure of Eu(TPEN) and Eu(MeTPEN), the geometry of these structures indicate pseudo-bicapped square antiprism (10 coordination) with two bidentate NO$$_{3}$$$$^{-}$$; ions. As the result of investigation of fluorescence spectrum and lifetime in organic solution, the fluorescence of Eu (MeTPEN) was enhanced more intensity than that of Eu(TPEN) by addition of OAc$$^{-}$$; ion.

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