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Journal Articles

Weakened oxygen adsorbing the Pt-O bond of the Pt catalyst induced by vacancy introduction into carbon support

Okazaki, Hiroyuki*; Idesaki, Akira*; Koshikawa, Hiroshi*; Matsumura, Daiju; Ikeda, Takashi*; Yamamoto, Shunya*; Yamaki, Tetsuya*

Journal of Physical Chemistry C, 127(49), p.23628 - 23633, 2023/12

 Times Cited Count:0 Percentile:0(Chemistry, Physical)

Journal Articles

Investigation of hydrogen superoxide adsorption during ORR on Pt/C catalyst in acidic solution for PEFC by ${it in-situ}$ high energy resolution XAFS

Yamamoto, Naoki*; Matsumura, Daiju; Hagihara, Yuto*; Tanaka, Kei*; Hasegawa, Yuta*; Ishii, Kenji*; Tanaka, Hirohisa*

Journal of Power Sources, 557, p.232508_1 - 232508_10, 2023/02

 Times Cited Count:2 Percentile:26.88(Chemistry, Physical)

Journal Articles

Formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd and chlorination of MPd$$_{3+x}$$ using cadmium chloride

Hayashi, Hirokazu; Shibata, Hiroki; Sato, Takumi; Otobe, Haruyoshi

Journal of Radioanalytical and Nuclear Chemistry, 332(2), p.503 - 510, 2023/02

 Times Cited Count:0 Percentile:0.01(Chemistry, Analytical)

The formation of MPd$$_{3+x}$$ (M = Gd, Np) by the reaction of MN with Pd at 1323 K in Ar gas flow was observed. Cubic AuCu$$_3$$-type GdPd$$_{3.3}$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) and NpPd$$_3$$ (${it a}$ = 0.4081 $$pm$$ 0.0001 nm) were identified, respectively. The product obtained from the reaction of NpN with Pd contained additional phases including the hexagonal TiNi$$_3$$-type NpPd$$_3$$. Chlorination of the MPd$$_{3+x}$$ (M = Gd, Np) samples was accomplished by the solid-state reaction using cadmium chloride at 673 K in a dynamic vacuum. Pd-rich solid solution phase saturated with Cd and an intermetallic compound PdCd were obtained as by-products of MCl$$_3$$ formation.

Journal Articles

Synergistic hybrid electrocatalysts of platinum alloy and single-atom platinum for an efficient and durable oxygen reduction reaction

Liu, B.*; Feng, R.*; Busch, M.*; Wang, S.*; Wu, H.*; Liu, P.*; Gu, J.*; Bahadoran, A.*; Matsumura, Daiju; Tsuji, Takuya; et al.

ACS Nano, 16(9), p.14121 - 14133, 2022/09

 Times Cited Count:51 Percentile:98.66(Chemistry, Multidisciplinary)

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:1 Percentile:11.64(Engineering, Chemical)

no abstracts in English

Journal Articles

Activity enhancement of platinum oxygen-reduction electrocatalysts using ion-beam induced defects

Kimata, Tetsuya*; Kakitani, Kenta*; Yamamoto, Shunya*; Shimoyama, Iwao; Matsumura, Daiju; Iwase, Akihiro*; Mao, W.*; Kobayashi, Tomohiro*; Yamaki, Tetsuya*; Terai, Takayuki*

Physical Review Materials (Internet), 6(3), p.035801_1 - 035801_7, 2022/03

 Times Cited Count:7 Percentile:68.86(Materials Science, Multidisciplinary)

Journal Articles

Extraction behavior of a novel functionalized ionic liquid for separation of platinum group metals from aqueous nitric acid solution

Ito, Tatsuya; Osugi, Haruka*; Osawa, Naoki*; Takahashi, Tadayuki*; Kim, S.-Y.*; Nagaishi, Ryuji

Analytical Sciences, 38(1), p.91 - 97, 2022/01

 Times Cited Count:2 Percentile:29.37(Chemistry, Analytical)

A novel ionic liquid (IL) functionalized with thiodiglycol amic acid containing a soft S donor was synthesized for the effective and efficient extraction of platinum group metals (Ru, Rh, and Pd) from aqueous nitric acid solutions, such as high-level radioactive liquid waste (HLLW). The IL allowed a rapid extraction of Pd(II) with an extraction ratio of approximately 100%. The extractions of Ru(III) and Rh(III) by the IL were slower than that of Pd(II), but the rates were accelerated by temperature elevation. The extractions of Ru(III) and Rh(III) at 50$$^{circ}$$C reached equilibrium within 4 and 8 h, respectively, with the extraction ratios of over 90% without assisting agents or other methods for the extraction system. Furthermore, the IL could extract more than 90% of Ru(III), Rh(III), and Pd(II) from the simulated HLLW within 2 h at 50$$^{circ}$$C.

Journal Articles

Effective extraction of Pt(IV) as [PtCl$$_{6}$$]$$^{2-}$$ from hydrochloric acid using a simple urea extractant

Ueda, Yuki; Morisada, Shintaro*; Kawakita, Hidetaka*; Wenzel, M.*; Weigand, J. J.*; Oto, Keisuke*

Separation and Purification Technology, 277, p.119456_1 - 119456_8, 2021/12

 Times Cited Count:5 Percentile:29.15(Engineering, Chemical)

no abstracts in English

Journal Articles

Density functional theory study on the $$^{193}$$Ir M$"o$ssbauer spectroscopic parameters of Vaska's complexes and their oxidative adducts

Kaneko, Masashi; Nakashima, Satoru*

Inorganic Chemistry, 60(17), p.12740 - 12752, 2021/09

 Times Cited Count:3 Percentile:31.46(Chemistry, Inorganic & Nuclear)

In the present study, density functional theory (DFT) calculation was applied to Vaska's complexes of formula ${it trans}$-[IrCl(CO)(PPh$$_{3}$$)$$_{2}$$], and their oxidative adducts with small molecules (YZ) including H$$_{2}$$, i.e., ${it trans}$-[IrCl(YZ)(CO))(PPh$$_{3}$$)$$_{2}$$], to successfully correlate the electronic states of the complexes with the corresponding $$^{193}$$Ir M$"o$ssbauer spectroscopic parameters. After confirming the reproducibility of the DFT methods for elucidating the equilibrium structures and $$^{193}$$Ir M$"o$ssbauer isomer shifts of the octahedral Ir complexes, the isomer shifts and quadrupole splitting values of Vaska's complexes and their oxidative adducts were calculated. A bond critical point analysis revealed that the tendency in the isomer shifts was correlated with the strength of the covalent interaction in the coordination bonds. In an electric field gradient (EFG) analysis of the oxidative adducts, the sign of the principal axis was found to be positive for the complex with YZ = Cl$$_{2}$$ and negative for the complex with YZ = H$$_{2}$$. This reversal of the sign of the EFG principal axis was caused by the difference in the electron density distribution for the coordination bonds between Ir and YZ, according to a density of states analysis.

Journal Articles

Selective extraction of platinum(IV) from the simulated secondary resources using simple secondary amide and urea extractants

Ueda, Yuki; Morisada, Shintaro*; Kawakita, Hidetaka*; Oto, Keisuke*

Separations (Internet), 8(9), p.139_1 - 139_15, 2021/09

 Times Cited Count:9 Percentile:62.42(Chemistry, Analytical)

no abstracts in English

Journal Articles

Sorption properties of aluminum hexacyanoferrate for platinum group elements

Mishima, Ria; Inaba, Yusuke*; Tachioka, Sotaro*; Harigai, Miki*; Watanabe, Shinta*; Onoe, Jun*; Nakase, Masahiko*; Matsumura, Tatsuro; Takeshita, Kenji*

Chemistry Letters, 49(1), p.83 - 86, 2020/01

 Times Cited Count:4 Percentile:20.61(Chemistry, Multidisciplinary)

Separation of platinum group metals (PGMs) from high-level liquid waste generated from the reprocessing of spent nuclear fuels is important to produce good quality vitrified glass for final disposal. A new sorbent, Aluminum hexacyanoferrate (AlHCF), was synthesized and the general sorption behavior of PGMs from concentrated nitric acid was examined. Nitric acid caused substantial elution of AlHCF but the sorption of Pd stabilized the structure. Consequently, Rh was sorbed in the presence of Pd, whereas single Rh sorption caused complete dissolution of AlHCF. Relation between sorbed mount of Pd vs eluted Al and Fe revealed that the elution ratio of Al and Fe was not the same as molar ratio of synthesized AlHCF, indicating the re-sorption of Fe resulted in formation of new structure. The sorption mechanism of PGMs by this new sorbent, AlHCF, not only the simple ion exchange, but also oxidation reduction reaction as well as kinetics play important rule. Understanding the general sorption and dissolution behavior will help improve the sorption performance of PGMs by AlHCF.

Journal Articles

Enhancement of Fe-N-C carbon catalyst activity for the oxygen reduction reaction; Effective increment of active sites by a short and repeated heating process

Yasuda, Satoshi; Uchibori, Yosuke*; Wakeshima, Makoto*; Hinatsu, Yukio*; Ogawa, Hiroaki; Yano, Masahiro; Asaoka, Hidehito

RSC Advances (Internet), 8(66), p.37600 - 37605, 2018/11

 Times Cited Count:12 Percentile:42.2(Chemistry, Multidisciplinary)

We present a quantitative study on the effect of a newly obtained thermal history on the formation of Fe-N-C catalytic sites. A short and repeated heating process is employed as the new thermal history, where short heating (1 min) followed by quenching is applied to a sample with arbitrary repetition. Through electrochemical quantitative analysis, it is found that the new process effectively increases the Fe-N-C mass-based site density (MSD) to almost twice that achieved using a conventional continuous heating process, while the turn-over frequency (TOF) is independent of the process. Elemental analysis shows that the new process effectively suppresses the thermal desorption of Fe and N atoms during the initial formation stage and consequently contributes to an increase in the Fe-N-C site density. The resultant catalytic activity (gravimetric kinetic current density (0.8 V vs. RHE)) is 1.8 times higher than that achieved with the continuous heating process.

Journal Articles

Effect of water for the oxygen adsorption on surface of PtCo catalysts

Cui, Y.-T.*; Harada, Yoshihisa*; Niwa, Hideharu*; Oshima, Masaharu*; Hatanaka, Tatsuya*; Nakamura, Naoki*; Ando, Masaki*; Yoshida, Toshihiko*; Ishii, Kenji*; Matsumura, Daiju

NanotechJapan Bulletin (Internet), 11(4), 6 Pages, 2018/08

no abstracts in English

Journal Articles

Development of separation technique for platinum group metals from radioactive liquid waste utilizing laser-induced particulate formation

Saeki, Morihisa*; Asai, Shiho; Oba, Hironori*

Bunseki, 2018(4), p.138 - 143, 2018/04

Platinum group metal (PGM) has attracted much attention in light of increasing demands in the industrial sector. A wide variety of techniques specialized for PGM separation, such as, solvent extraction, solid phase extraction, and molten salt electrolysis have been developed so far. Among such techniques, a newly developed separation technique based on laser-induced particulate formation can be a promising alternative to conventional ones. It enables non-contact and highly-selective separation with a simple operation. In this review, the research history and the basic mechanism of laser-induced particulate formation were outlined. Several applications were also mentioned, focusing on our latest research progress which achieved a world first quantitation of radioactive palladium in a spent nuclear fuel sample.

Journal Articles

Adsorption of platinum-group metals and molybdenum onto aluminum ferrocyanide in spent fuel solution

Onishi, Takashi; Sekioka, Ken*; Suto, Mitsuo*; Tanaka, Kosuke; Koyama, Shinichi; Inaba, Yusuke*; Takahashi, Hideharu*; Harigai, Miki*; Takeshita, Kenji*

Energy Procedia, 131, p.151 - 156, 2017/12

 Times Cited Count:11 Percentile:98.82(Energy & Fuels)

no abstracts in English

Journal Articles

Chemical state analysis of rhodium in simulated waste glass by synchrotron-radiation-based XAFS and imaging XAFS techniques

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Inose, Takehiko*; Sato, Seiichi*

Nihon Genshiryoku Gakkai Wabun Rombunshi, 16(4), p.180 - 190, 2017/12

X-ray absorption fine structure (XAFS) and imaging XAFS analyses were performed to elucidate chemical state of rhodium in the simulated waste glass. The chemical forms of Rh in the glass were evaluated to be 84% RhO$$_{2}$$ and 16% metal/alloy as the result of linear combination analysis of EXAFS data. According to the imaging XAFS analysis, the chemical form of Rh which was located together with Ru was mainly oxide (RhO$$_{2}$$). It suggests that stable (Ru,Rh)O$$_{2}$$ solid solution exists in the simulated glass. On the other hand, that of Rh of which distribution did not accord with Ru in the glass was mainly metallic. In the case of metallic Rh in the glass, it tended to become an aggregation form. It can be concluded that the chemical state of Rh was much affected by the existence and distribution of Ru element.

Journal Articles

Recent research in solvent extraction of platinum group metals

Narita, Hirokazu*; Suzuki, Tomoya*; Motokawa, Ryuhei

Nihon Kinzoku Gakkai-Shi, 81(4), p.157 - 167, 2017/04

 Times Cited Count:17 Percentile:62.47(Metallurgy & Metallurgical Engineering)

Journal Articles

Selective extraction of Pt(IV) over Fe(III) from HCl with an amide-containing tertiary amine compound

Maeda, Motoki*; Narita, Hirokazu*; Tokoro, Chiharu*; Tanaka, Mikiya*; Motokawa, Ryuhei; Shiwaku, Hideaki; Yaita, Tsuyoshi

Separation and Purification Technology, 177, p.176 - 181, 2017/04

 Times Cited Count:22 Percentile:58.37(Engineering, Chemical)

Journal Articles

Separation of Ru(III), Rh(III) and Pd(II) from nitric acid solutions using ion-exchange resins bearing carboxylic betaine

Suzuki, Tomoya; Morita, Keisuke; Sasaki, Yuji; Matsumura, Tatsuro

Separation Science and Technology, 51(17), p.2815 - 2822, 2016/09

 Times Cited Count:8 Percentile:26.31(Chemistry, Multidisciplinary)

To understand the adsorption properties of styrene-divinylbenzene copolymer functionalized with ${it N,N,N}$-trimethylglycine, AMP03, the adsorption behaviors for platinoid ions (Ru(III), Rh(III), and Pd(II)) were examined. Furthermore, we performed adsorption experiments using sample solutions with adding triethylamine, thiourea, and ${it N,N,N}$-trimethylglycine. Based on the adsorption data obtained in this study, we performed chromatographic experiments. The results indicated that all platinoid ions in the feed solution completely adsorbed on AMP03, and almost 80% of the adsorbed platinoid ions were recovered. These results show that AMP03 has the potential to recover Ru(III), Rh(III), and Pd(II) from high-level liquid waste.

Journal Articles

Chemical composition of insoluble residue generated at the Rokkasho Reprocessing Plant

Yamagishi, Isao; Odakura, Makoto; Ichige, Yoshiaki; Kuroha, Mitsuhiko; Takano, Masahide; Akabori, Mitsuo; Yoshioka, Masahiro*

Proceedings of 21st International Conference & Exhibition; Nuclear Fuel Cycle for a Low-Carbon Future (GLOBAL 2015) (USB Flash Drive), p.1113 - 1119, 2015/09

The characteristics of insoluble residues in fine suspension at the Rokkasho Reprocessing Plant were analyzed. The insoluble residues were washed with oxalic acid solution to dissolve zirconium molybdate residues. XRD profiles of unwashed residues showed the presence of a noble metal alloy, zirconium molybdate, and zirconia, but zirconium molybdate was not found after washing. More than 50% of the Sb-125 and Pu in thee residues was washed out as well. The noble metal alloy composed of Mo, Tc, Ru, Rh, and Pd occupied more than 90% of the total weight of 12 elements (Ca, Cr, Fe, Ni, Zr, Mo, Tc, Ru, Rh, Pd, Te, and U) found in the residues. In consideration of the chemical forms of 12 elements, the alloy-to-residue weight ratio was evaluated to be 64% and 78% with and without 18% of an unknown component, respectively.

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