Selective adsorption of Pd(II) over Ag(I) in nitric acid solutions using nitrogen-donor-type adsorbents

Suzuki, Tomoya*; Otsubo, Ukyo*; Ogata, Takeshi*; Shiwaku, Hideaki; Kobayashi, Toru; Yaita, Tsuyoshi; Matsuoka, Mitsuaki*; Murayama, Norihiro*; Narita, Hirokazu*

Separation and Purification Technology, 308, p.122943_1 - 122943_7, 2023/03

https://doi.org/10.1016/j.seppur.2022.122943

HNO leaching is used in recycling Pd metal from spent products that primarily contain Ag, and most Pd residues are separated from solutions containing Ag(I). However, a small amount of Pd(II) often remains in these Ag(I) solutions. Therefore, the separation of Pd(II) and Ag(I) in HNO solutions is essential to promote efficient Pd recycling. In this study, the separation of Pd(II) and Ag(I) in HNO solutions was investigated using four N-donor-type adsorbents functionalized with amine (R-Amine), iminodiacetic acid (R-IDA), pyridine (R-Py), or bis-picolylamine (R-BPA). R-Amine, R-IDA, and R-Py selectively adsorbed Pd(II) over Ag(I), Cu(II), Ni(II), and Fe(III) from HNO solutions (0.3-7 M), but R-Amine exhibited a lower Pd adsorption efficiency. In contrast, 90% of Pd(II), Ag(I), and Cu(II) were adsorbed by R-BPA over the entire range of HNO concentrations. Structural analyses of the adsorbed metal ions using Fourier transform infrared spectroscopy and extended X-ray absorption fine structure spectroscopy revealed the separation mechanisms of the N-donor-type adsorbents. Pd(II) adsorption on R-IDA, R-Py, and R-BPA occurred via Pd(II) coordination of the functional groups (iminodiacetic acid, pyridine, and bis-picolylamine, respectively), whereas that on R-Amine occurred via anion exchange of NO with [Pd(NO)]. The coordinative adsorption mechanisms resulted in the higher Pd(II) adsorption behaviors of R-IDA, R-Py, and R-BPA. HCl (5.0 M) and thiourea (0.1 M) eluents desorbed 83% of Pd(II) from R-IDA and 95% from R-Py, respectively. R-Py was the most effective Pd(II) adsorbent based on adsorption selectivity and desorption efficiency.

Development and validation of fuel stub motion model for the disrupted core of a sodium-cooled fast reactor

Kawada, Kenichi; Suzuki, Toru*

Nuclear Engineering and Technology, 53(12), p.3930 - 3943, 2021/12

https://doi.org/10.1016/j.net.2021.06.018

To improve the capability of the SAS4A code, which simulates the initiating phase of core disruptive accidents for MOX-fueled Sodium-cooled Fast Reactors (SFRs), the authors have investigated in detail the physical phenomena under unprotected loss-of-flow (ULOF) conditions in a previous paper. As the conclusion of the last article, fuel stub motion, in which the residual fuel pellets would move toward the core central region after fuel pin disruption, was identified as one of the key phenomena to be appropriately simulated for the initiating phase of ULOF. In the present paper, a simple model describing fuel stub motion, which was not modeled in the previous SAS4A code, was newly proposed. The applicability of the proposed model was validated through a series of analyses for the CABRI experiments, by which the stub motion would be represented with reasonable conservativeness for the reactivity evaluation of disrupted core.

Manufacture of substitutive assemblies for MONJU reactor decommissioning

Sakakibara, Hiroshi; Aoki, Nobuhiro; Muto, Masahiro; Otabe, Jun; Takahashi, Kenji*; Fujita, Naoyuki*; Hiyama, Kazuhiko*; Suzuki, Hirokazu*; Kamogawa, Toshiyuki*; Yokosuka, Toru*; et al.

JAEA-Technology 2020-020, 73 Pages, 2021/03

JAEA-Technology-2020-020.pdf:8.26MB

The decommissioning is currently in progress at the prototype fast breeder reactor Monju. Fuel assemblies will be taken out of its core for the first step of the great task. Fuel assemblies stand on their own spike plugged into a socket on the core support plate and support with adjacent assemblies through their housing pads each other, resulting in steady core structure. For this reason, some substitutive assemblies are necessary for the purpose of discharging the fuel assemblies of the core. Monju side commissioned, therefore, Plutonium Fuel Development Center to manufacture the substitutive assemblies and the Center accepted it. This report gives descriptions of design, manufacture, and shipment in regard to the substitutive assemblies.

Thermally altered subsurface material of asteroid (162173) Ryugu

Kitazato, Kohei*; Milliken, R. E.*; Iwata, Takahiro*; Abe, Masanao*; Otake, Makiko*; Matsuura, Shuji*; Takagi, Yasuhiko*; Nakamura, Tomoki*; Hiroi, Takahiro*; Matsuoka, Moe*; et al.

Nature Astronomy (Internet), 5(3), p.246 - 250, 2021/03

https://doi.org/10.1038/s41550-020-01271-2

Here we report observations of Ryugu's subsurface material by the Near-Infrared Spectrometer (NIRS3) on the Hayabusa2 spacecraft. Reflectance spectra of excavated material exhibit a hydroxyl (OH) absorption feature that is slightly stronger and peak-shifted compared with that observed for the surface, indicating that space weathering and/or radiative heating have caused subtle spectral changes in the uppermost surface. However, the strength and shape of the OH feature still suggests that the subsurface material experienced heating above 300 C, similar to the surface. In contrast, thermophysical modeling indicates that radiative heating does not increase the temperature above 200 C at the estimated excavation depth of 1 m, even if the semimajor axis is reduced to 0.344 au. This supports the hypothesis that primary thermal alteration occurred due to radiogenic and/or impact heating on Ryugu's parent body.

Analysis of atomistic structural deformation characteristics of calcium silicate hydrate in 53-year-old tricalcium silicate paste using atomic pair distribution function

Bae, S.*; Jee, H.*; Suh, H.*; Kanematsu, Manabu*; Shiro, Ayumi*; Machida, Akihiko*; Watanuki, Tetsu*; Shobu, Takahisa; Morooka, Satoshi; Geng, G.*; et al.

Construction and Building Materials, 237, p.117714_1 - 117714_10, 2020/03

https://doi.org/10.1016/j.conbuildmat.2019.117714

Reconstruction of residents' thyroid equivalent doses from internal radionuclides after the Fukushima Daiichi Nuclear Power Station accident

Oba, Takashi*; Ishikawa, Tetsuo*; Nagai, Haruyasu; Tokonami, Shinji*; Hasegawa, Arifumi*; Suzuki, Gen*

Scientific Reports (Internet), 10(1), p.3639_1 - 3639_11, 2020/02

https://doi.org/10.1038/s41598-020-60453-0

Internal doses of residents after the Fukushima Daiichi Nuclear Power Station accident have been reconstructed. In total 896 behaviour records in the Fukushima Health Management Survey were analysed to estimate thyroid doses via inhalation, using a spatiotemporal radionuclides concentration database constructed by atmospheric dispersion simulations. After a decontamination factor for sheltering and a modifying factor for the dose coefficient were applied, estimated thyroid doses were close to those estimated on the basis of direct thyroid measurement. The median and 95th percentile of thyroid doses of 1-year-old children ranged from 1.2 to 15 mSv and from 7.5 to 30 mSv, respectively.

Unique anion-exchange properties of 3,3'-diaminobenzidine resulting in high selectivity for rhodium(III) over palladium(II) and platinum(IV) in a concentrated hydrochloric acid solution

Suzuki, Tomoya*; Ogata, Takeshi*; Tanaka, Mikiya*; Kobayashi, Toru; Shiwaku, Hideaki; Yaita, Tsuyoshi; Narita, Hirokazu*

Analytical Sciences, 35(12), p.1353 - 1360, 2019/12

https://doi.org/10.2116/analsci.19P204

no abstracts in English

The Surface composition of asteroid 162173 Ryugu from Hayabusa2 near-infrared spectroscopy

Kitazato, Kohei*; Milliken, R. E.*; Iwata, Takahiro*; Abe, Masanao*; Otake, Makiko*; Matsuura, Shuji*; Arai, Takehiko*; Nakauchi, Yusuke*; Nakamura, Tomoki*; Matsuoka, Moe*; et al.

Science, 364(6437), p.272 - 275, 2019/04

https://doi.org/10.1126/science.aav7432

The near-Earth asteroid 162173 Ryugu, the target of Hayabusa2 sample return mission, is believed to be a primitive carbonaceous object. The Near Infrared Spectrometer (NIRS3) on Hayabusa2 acquired reflectance spectra of Ryugu's surface to provide direct measurements of the surface composition and geological context for the returned samples. A weak, narrow absorption feature centered at 2.72 micron was detected across the entire observed surface, indicating that hydroxyl (OH)-bearing minerals are ubiquitous there. The intensity of the OH feature and low albedo are similar to thermally- and/or shock-metamorphosed carbonaceous chondrite meteorites. There are few variations in the OH-band position, consistent with Ryugu being a compositionally homogeneous rubble-pile object generated from impact fragments of an undifferentiated aqueously altered parent body.

Lanthanides complexation properties of O, N-hetero donor ligand PTA

Kobayashi, Toru; Suzuki, Shinichi; Shiwaku, Hideaki; Yaita, Tsuyoshi

Progress in Nuclear Science and Technology (Internet), 5, p.74 - 77, 2018/11

https://doi.org/10.15669/pnst.5.74

Development of extractant, which can efficiently separate actinides, is of increasing importance because it concerns establishment and simplification of separation techniques in nuclear fuel cycle and decontamination of radioactive wastes. In this study, the complexation properties of N-alkyl-N-phenyl-1,10-phenanthroline-2-carboxamide (PTA) with trivalent lanthanides (Ln) were investigated based on structural analysis by using X-ray crystallography and extended X-ray absorption fine structure (EXAFS) methods. As a result, it is revealed that two PTA molecules coordinate with Ln as tridentate ligand via two nitrogen in phenanthroline moiety and one oxygen in amide moiety in both crystal and solution states. The slight difference in coordination bond distances are observed between Eu and Nd complexes, this difference corresponds to the difference in ionic radius between Nd and Eu. This result indicates slight difference in ionic radii of Ln hardly affects coordination properties of PTA.

Sedimentation behavior of mixed solid particles

Sheikh, Md. A. R.*; Son, E.*; Kamiyama, Motoki*; Morioka, Toru*; Matsumoto, Tatsuya*; Morita, Koji*; Matsuba, Kenichi; Kamiyama, Kenji; Suzuki, Toru*

Journal of Nuclear Science and Technology, 55(6), p.623 - 633, 2018/06

https://doi.org/10.1080/00223131.2017.1419888

During core-disruptive accidents in sodium-cooled fast reactors, the sedimentation behavior of fragmented debris is crucial for in-vessel retention. The height of the beds formed may influence both the cooling of the bed and the neutronic characteristics. To develop an experimental database of bed formation behavior, a series of experiments using simulant materials, namely, AlO, ZrO, and stainless steel, were performed under gravity-driven discharge of solid particles from a nozzle into a quiescent cylindrical water pool. The bed height was measured for particles of different size, density, and sphericity, and an injection nozzle with varying diameter, injection velocity, and injection height. From these experiments, an empirical correlation was established to predict the bed height for both homogeneous and mixed particles for the different properties. This correlation reproduces reasonably well the experimental trend in bed height.