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.

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

Speciation of ruthenium(III) chloro complexes in hydrochloric acid solutions and their extraction characteristics with an amide-containing amine compound

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

Metals, 8(7), p.558_1 - 558_10, 2018/07

AA2018-0670.pdf:2.11MB

https://doi.org/10.3390/met8070558

The refining of platinum group metals is based mainly on solvent extraction methods, whereas Ru is selectively recovered by distillation as RuO. Replacement of distillation byextraction is expected to simplify the purification process. To develop an effective extraction system for Ru, we analyzed the Ru species in HCl with UV-Vis and EXAFS spectroscopies, and we examined the properties of Ru extracted with N-2-ethylhexyl-bis(N-di-2-ethylhexyl-ethylamide) amine (EHBAA). EXAFS and UV-Vis spectra of Ru in HCl solutions revealed that the predominant Ru species in 0.5-10 M HCl solutions changed from [RuCl(HO)] to [RuCl] with the HCl concentration. The extraction percentages of Ru in the EHBAA system increased with increasing HCl concentration, reached 80% at [HCl] = 5 M, and decreased athigher HCl concentrations. EXAFS analysis of the extracted complex indicated that the Ru had 5 Cl and 1 HO in its inner coordination sphere. The similarity of the dependence on HCl concentrations of the extraction in the EHBAA system and the distribution profile of [RuCl(HO)] on [RuCl(HO)] suggested that the EHBAA extracted the pentachlorido species.

Mizunami Underground Research Laboratory Project, Annual report for fiscal year 2006

Nishio, Kazuhisa; Matsuoka, Toshiyuki; Mikake, Shinichiro; Tsuruta, Tadahiko; Amano, Kenji; Oyama, Takuya; Takeuchi, Ryuji; Saegusa, Hiromitsu; Hama, Katsuhiro; Yoshida, Haruo*; et al.

JAEA-Review 2009-001, 110 Pages, 2009/03

JAEA-Review-2009-001.pdf:49.84MB

Japan Atomic Energy Agency (JAEA) at Tono Geoscience Center (TGC) is developing a geoscientific research project named Mizunami Underground Research Laboratory (MIU) project in crystalline rock environment in order to establish scientific and technological basis for geological disposal of HLW. Geoscientific research at MIU is planned to be carried out in three phases over a period of 20 years; Surface-based Investigation Phase (Phase 1), Construction Phase (Phase 2) and Operation Phase (Phase 3). Currently, the project is under the Construction Phase. This document presents the following results of the research and development performed in 2006 fiscal year, as a part of the Construction Phase based on the MIU Master Plan updated in 2002, (1) Investigation at the MIU Construction Site, (2) Construction at the MIU Construction Site, (3) Research Collaboration.

Mizunami Underground Research Laboratory Project Plan for fiscal year 2008

Nishio, Kazuhisa; Oyama, Takuya; Mikake, Shinichiro; Mizuno, Takashi; Saegusa, Hiromitsu; Takeuchi, Ryuji; Amano, Kenji; Tsuruta, Tadahiko; Hama, Katsuhiro; Seno, Yasuhiro; et al.

JAEA-Review 2008-072, 28 Pages, 2009/02

JAEA-Review-2008-072.pdf:11.8MB

Japan Atomic Energy Agency (JAEA) at Tono Geoscience Center (TGC) is developing a geoscientific research project named the Mizunami Underground Research Laboratory (MIU) project in crystalline rock environment in order to establish scientific and technological basis for geological disposal of HLW. Geoscientific research at the MIU project is planned to be carried out in three phases over a period of 20 years; Surface-based Investigation Phase (Phase 1), Construction Phase (Phase 2) and Operation Phase (Phase 3). Currently, the project is under the Construction Phase. This document presents the following 2008 fiscal year plan based on the MIU Master Plan updated in 2002, (1) Investigation Plan, (2) Construction Plan, (3) Research Collaboration Plan, etc.

Mizunami Underground Research Laboratory project program for fiscal year 2006

Nishio, Kazuhisa; Mizuno, Takashi; Oyama, Takuya; Nakama, Shigeo; Saegusa, Hiromitsu; Takeuchi, Ryuji; Amano, Kenji; Tsuruta, Tadahiko; Hama, Katsuhiro; Iyatomi, Yosuke; et al.

JAEA-Review 2007-037, 29 Pages, 2007/12

JAEA-Review-2007-037.pdf:13.06MB

Japan Atomic Energy Agency (JAEA) at Tono Geoscience Center (TGC) is developing a geoscientific research project named Mizunami Underground Research Laboratory (MIU) in crystalline rock environment in order to establish scientific and technological basis for geological disposal of HLW. Geoscientific research at MIU is planned to be carried out in three Phases over a period of 20 years; Surface-based Investigation Phase (Phase 1), Construction Phase (Phase 2) and Operation Phase (Phase 3). Currently, the Project is under the Construction Phase. This document presents the following 2006 fiscal year plan of the Construction Phase based on the MIU Master Plan updated in 2002, (1)Investigation Plan at the MIU Construction Site, (2)Construction Plan at the MIU Construction Site, (3)Research Collaboration Plan.

Assessment of heterogeneous geological environment at Tono; Japanese fiscal year 2004 (Contract research)

Toida, Masaru*; Suyama, Yasuhiro*; Mori, Takayuki*; Inaba, Takeshi*; Sasakura, Takeshi*; Atsumi, Hiroyuki*; Masumoto, Kazuhiko*; Kobayashi, Ichizo*; Iwano, Keita*; Furuichi, Mitsuaki*; et al.

JAEA-Research 2007-065, 210 Pages, 2007/09

JAEA-Research-2007-065-1.pdf:28.82MB
JAEA-Research-2007-065-2.pdf:42.37MB
JAEA-Research-2007-065-3.pdf:24.46MB
JAEA-Research-2007-065-4.pdf:48.78MB

"Geoscientific research" at the Tono Area is developing site investigation, characterization and assessment techniques for understanding of geological environment. Their important goals are to establish a methodology for analyzing uncertainties in heterogeneous geological environment and to develop investigation techniques for efficiently reducing the uncertainties. The current study proposes a new approach where all the possible options in the models and data-sets, which cannot be excluded in the light of the evidences available, are identified. This approach enables uncertainties associated with the understanding at a given stage of the site characterization to be made explicitly using an uncertainty analysis technique based on Fuzzy geostatistics. This approach supports the design of the following investigation stage and reduces the uncertainties efficiently. In FY H16 the technique has been tested through geological modelling and groundwater analyses with Tono Area case based on current knowledge, to demonstrate its applicability and to compile the knowledge / information required to describe the H17 report. This report can be summarized as follows: (1) The knowledge / information required to describe the heterogeneous characteristics was compiled and connected to uncertainties associated with the characterization of a geological environment using a synthesis diagram. (2) Methodologies for assignment and screening of parameters were developed by using Evidential Support Logic (ESL). (3) Applicability of the techniques could be confirmed with Tono Area case. (4) This report proposed a new methodology that integrates the technique into JAEA ordinary technique to good advantage in the geoscientific research project.

None

Inami, Shinichi; Nogami, Takashi; Maki, Akira; Ogata, Yoshiaki; Takeshita, Kenji*; Sazarashi Masami*; Kumagai, Mikio*

Donen Giho, (98), p.32 - 42, 1996/06

https://jopss.jaea.go.jp/pdfdata/PNC-TN1340-96-002.pdf

None

Development of extraction chromatographic agents based on nitrogen-donor ligand for the separation of actinide

Ogata, Takeshi*; Takeshita, Kenji*; Oaki, Hiroshi*; Inaba, Yusuke*; Mori, Atsunori*; Matsumura, Tatsuro; Nakano, Yoshio*

no journal, , 

N,N,N',N'-tetrakis(2-pyridylmethyl)ethylenediamine (TPEN) is one of the podand-type ligands with six nitrogen-donors and recognize the slight difference in the softness between Am(III) and Eu(III). We have tried to synthesize a novel extraction chromatographic agent, which exploit such feature of TPEN. The use of the polymer gel as a support of the extractant can be expect to suppress the elution of the extractant and keep the flexibility of extractant. N,N,N',N'-tetrakis-(4-propenyloxy-2-pyridylmethyl)ethylenediamine (TPPEN) which is TPEN analog introducing polymerizable group to pyridine ring was used as a cross-linker of N-isopropylacrylamide (NIPA). Furthermore, the TPPEN-NIPA gel on highly porous silica was prepared to improve the mechanical strength of the gel. These extraction chromatographic agents have been tested for the separation of Am(III) and Eu(III). Characterization and extraction performance of the extraction chromatographic agents will be described.

Separation of MA and Ln by extraction chromatography using functional gel copolymerized with multidentate inclusion ligands, 3; Recovery of minor actinide from the spent fuel

Suto, Mitsuo; Obayashi, Hiroshi; Koyama, Shinichi; Sekioka, Ken*; Takeshita, Kenji*; Inaba, Yusuke*; Ogata, Takeshi*; Oaki, Hiroshi*

no journal, , 

no abstracts in English