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high energy resolution XAFSYamamoto, 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)Okamoto, Yoshihiro; Shiwaku, Hideaki; Shimamura, Keisuke*; Kobayashi, Hidekazu; Nagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
Journal of Nuclear Materials, 570, p.153962_1 - 153962_13, 2022/11
Simulated nuclear waste glass samples containing phosphorus, which increase the solubility of molybdenum, were prepared and analyzed using synchrotron X-ray Absorption Fine Structure (XAFS) analysis for some constituent elements and Raman spectroscopic analysis of their complex structure. Changes in local structure and chemical state due to different phosphorus additions and waste loading rates were systematically studied. Consequently, no crystalline phase due to the molybdate compound was observed even at a maximum waste content of 30 wt% (corresponding to 1.87 mol% MoO
). Oxidation proceeded when the waste-loading rate was increased, whereas the reduction proceeded when phosphorus was added. In some cases, the effects of oxidation and reduction were offset. The local structure around specific elements can be classified as follows; Zn that is affected mainly by the waste-loading rate, Ce that is affected by both the waste-loading rate and phosphorus addition, and Zr element that is not affected by either of them. From the comparison between the analytical results of Mo and other elements, it was considered that the added phosphorus exists as a free PO
structural unit and may deprive the alkali metal coordinated to the molybdate ion.
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)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)Murakami, Tsuyoshi*; Hayashi, Hirokazu
Journal of Nuclear Materials, 558, p.153330_1 - 153330_7, 2022/01
Times Cited Count：0 Percentile：0.01(Materials Science, Multidisciplinary)Excess amounts of dissolution agents, CdCl
and ZrCl, are required to dissolve transuranium (TRU: Pu and minor actinides) nitrides into LiCl-KCl melts at the chemical dissolution step, which is the first step in the reprocessing of used nitride fuels. We propose an electrochemical process where the remaining Zr and Cd are recovered from the melts to be recycled as dissolution agents for the chemical dissolution step, leaving TRU in the melts. Since the initial concentration ratio of CdCl/ZrCl remaining in the melts would depend on the condition of the chemical dissolution step and would vary during the proposed electrochemical recovery process, electrochemical behaviors of Zr and Cd were investigated in LiCl-KCl melts with various concentration ratios of CdCl/ZrCl at 723 K to confirm the basic feasibility of the proposed process. Potentiostatic electrolysis was performed using a liquid Cd cathode at -1.05 V (vs. Ag/AgCl), which was a more positive potential than the redox potentials of TRU on the liquid Cd electrode. The obtained results showed that the current efficiency for recovering Zr and Cd from the melts was as high as 100% regardless of the CdCl/ZrCl concentration ratio in the melts.
Yomogida, Takumi; Saeki, Morihisa*; Morii, Shiori; Oba, Hironori*; Kitatsuji, Yoshihiro
Analytical Sciences, 37(12), p.1843 - 1846, 2021/12
Times Cited Count：0 Percentile：0(Chemistry, Analytical)In this study, we developed a simple and one-step Pd separation technique based on photoreduction with Xe lamp irradiation for the determination of 
Pd in highly radioactive samples. A simulated high-level radioactive liquid wastes (HLLW) solution, which consists of 14 major elements (Rb, Sr, Zr, Mo, Ru, Rh, Pd, Cs, Ba, La, Ce, Pr, Nd, Sm) in a 3 mol L
HNO
solution, was used to evaluate the separation performance. The Pd precipitate were formed by Xe lamp irradiation and recovered by centrifugation. The results showed that the recovery of Pd from a simulated HLLW solution depend on the irradiation time and concentration of ethanol. By optimizing the conditions at photo irradiation, the Pd recovery from the simulated HLLW solution reached up to 50 %, while 99.5 % of the other 13 elements were separated. The Pd precipitate could be separated from the elements that are the main source of radioactivity (Sr, Cs, and Ba) and the source of spectral interference for the determination of Pd (Zr, and Ru). These results indicate that selective separation of Pd is achieved with the proposed method, showing the applicability of the proposed separation technique to HLLW samples.
Wakai, Satoshi*; Hirano, Shinichi*; Ueno, Fumiyoshi; Okamoto, Akihiro*
Zairyo To Kankyo, 70(12), p.491 - 496, 2021/12
After Fukushima Daiichi Nuclear Power Station accident, various corrosion mitigating activities have been treated, and severe corrosion incident have never taken placed. On the other hand, the facilities were exposed sea water, and some of them have continuously exposed to ground water. The exposure of metal materials to environmental water has a risk of microbiologically influenced corrosion (MIC). In this paper, we summarize the latest knowledge of MIC and the task of MIC in the decommissioning of Fukushima Daiichi Nuclear Power Station.
Nagai, Takayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Okamoto, Yoshihiro
2020-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Oyobi "Hito, Kankyo To Busshitsu O Tsunagu Inobeshion Soshutsu Dainamikku, Araiansu" Kenkyu Seika, Katsudo Hokokusho (CD-ROM), 1 Pages, 2021/11
no abstracts in English
Ogawa, Shuichi*; Taga, Ryo*; Yoshigoe, Akitaka; Takakuwa, Yuji*
Journal of Vacuum Science and Technology A, 39(4), p.043207_1 - 043207_9, 2021/07
Times Cited Count：1 Percentile：7.45(Materials Science, Coatings & Films)Nickel (Ni) is used as a catalyst for nitric oxide decomposition and ammonia production but it is easily oxidized and deactivated. Clarification of the reduction process of oxidized Ni is essential to promote more efficient use of Ni catalysts. In this study, the reduction processes were investigated by in situ time-resolved photoelectron spectroscopy. We propose a two-step reduction reaction model. The rate-limiting process for the first step is surface precipitation of O atoms and that of the second step is dissociation of H
molecules.
Nakashima, Nobuaki*; Yatsuhashi, Tomoyuki*; Sakota, Kenji*; Iwakura, Izumi*; Hashimoto, Sena*; Yokoyama, Keiichi; Matsuda, Shohei
Chemical Physics Letters, 752, p.137570_1 - 137570_5, 2020/08
Times Cited Count：1 Percentile：4.85(Chemistry, Physical)Photo-redox reactions between Eu
and Eu
ions are induced by laser irradiation in alcoholic solution. Efficiency, wavelength dependence, and laser-power dependence are investigated with three different lasers. Nano second laser pulses at a wavelength of 308 nm is found to cause one-photon redox reactions with a quantum yield around 0.5. Nano second laser pulses at a wavelength of 394 nm induces two-photon reduction of Eu to form Eu. When the pulse energy is 5 mJ, the quantum yield is measured to be 0.015. Although the quantum yield is one order of magnitude lower than that of the one photon reduction, reduction phenomena can be easily observed under the moderate laser field strength. Because of the two-photon nature, there should be a room to improve the efficiency by increasing the laser field strength.
Kato, Chiaki
Comprehensive Nuclear Materials, 2nd Edition, Vol.4, p.528 - 563, 2020/08
In spent fuel reprocessing plants, various nitric media are encountered throughout the PUREX process, used in the separation of fission products, uranium, and plutonium. The PUREX process is thus highly corrosive as it takes place at high temperatures under high concentrations of nitric acid solution containing oxidizing metal ions from spent fuel. In this review, the unique chemical properties of nitric acid are first described. Secondly, the process of oxidizing power generation in boiling nitric acid under heat transfer is described using the redox potential and a thermodynamic model of boiling nitric acid. Finally, the corrosion behavior and corrosion acceleration mechanism specific to the reprocessing environments are described from the perspective of solution chemistry.
Itoi, Hiroyuki*; Ninomiya, Takeru*; Hasegawa, Hideyuki*; Maki, Shintaro*; Sakakibara, Akihiro*; Suzuki, Ryutaro*; Kasai, Yuto*; Iwata, Hiroyuki*; Matsumura, Daiju; Owada, Mao*; et al.
Journal of Physical Chemistry C, 124(28), p.15205 - 15215, 2020/07
Times Cited Count：8 Percentile：39.3(Chemistry, Physical), Zn
+, and CoKato, Tomoaki*; Yu, Q.*; Tanaka, Kazuya; Kozai, Naofumi; Saito, Takumi*; Onuki, Toshihiko
Journal of Environmental Sciences, 86, p.78 - 86, 2019/12
Times Cited Count：2 Percentile：8.23(Environmental Sciences)This paper investigated the fate of the dissolved permanganate in aqueous solution after contact with bacterial cells and metal accumulation during precipitation of Mn oxides. When Mn(VII) was contacted with bacterial cells, cells were damaged and Mn(VII) was reduced by cells to lower valence and precipitated as Mn oxides (biomass Mn oxides). When Co ions were present, Co was incorporated into Mn oxides as Co. These results suggest that Mn(VII) can be used to remove metal ions when introduced to wastewater as disinfectant.
Saeki, Morihisa*; Matsumura, Daiju; Yomogida, Takumi; Taguchi, Tomitsugu*; Tsuji, Takuya; Saito, Hiroyuki*; Oba, Hironori*
Journal of Physical Chemistry C, 123(1), p.817 - 824, 2019/01
Times Cited Count：14 Percentile：53.24(Chemistry, Physical)Reaction kinetics of laser-induced particle formation in an aqueous solution of PdCl
was investigated by transmission electron microscope (TEM) and dispersive X-ray absorption fine structure (DXAFS). The Pd particle was generated by irradiation of nanosecond pulsed 266-nm laser. The TEM observation showed dependence of the particle size on the laser fluence and promotion of the particle growth by irradiation of high-fluence laser. The DXAFS data give us the Pd concentration. Temporal changes of the Pd concentration analyzed based on Finke-Watzky two step mechanism. The analysis elucidates that the laser photon contributes to the reduction of the PdCl ion by the one-photon process and to the autocatalytic growth of the Pd particles by the multi-photon process.
Kusaka, Ryoji
Bunko Kenkyu, 67(6), p.239 - 240, 2018/12
A spectroscopic technique for analysis developed by collaboration between Japan Atomic Energy Agency (JAEA) and Quantum and Radiological Science and Technology (QST) is discussed for readers outside the field of nuclear energy. This paper introduces a quantitative analysis for Pd radioisotope contained in a spent nuclear fuel by using laser-induced photoreduction and inductively coupled plasma mass spectrometry (ICP-MS). The importance and problems of quantitative analysis for radioisotopes in spent nuclear fuels are described, and the principle, advantages, and future applications of the spectroscopic technique are discussed.
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.
Hayashida, Kazuki; Kato, Toshihiro*; Kubota, Mitsuru*; Murakami, Hiroaki; Amano, Yuki; Iwatsuki, Teruki
Chikyu Kagaku, 52(1), p.55 - 71, 2018/03
In this study, the simulated experimental drift was constructed in the granite of 500 m depth at Mizunami Underground Research Laboratory, and the hydrochemical process after the drift closure was observed. The groundwater chemistry around the drift changed with the change of the groundwater flow in the fractures when the gallery was constructed. The redox potential increased due to the infiltration of oxygen from the drift into the rock. After closing the drift, the redox potential of the groundwater plunged due to microbial activity, while the groundwater became alkalized conditon due to the influence of cement material such as shotcrete. The amount of cement material consumed for this alkalization was small, and it was considered that its influence would last long in accordance with the amount of cement used.
Pd by ICP-MS; The Relation between separation conditions and Pd recoveryYomogida, Takumi; Asai, Shiho; Saeki, Morihisa*; Hanzawa, Yukiko; Horita, Takuma; Esaka, Fumitaka; Oba, Hironori*; Kitatsuji, Yoshihiro
Bunseki Kagaku, 66(9), p.647 - 652, 2017/09
Times Cited Count：2 Percentile：6.85(Chemistry, Analytical)Palladium-107 is a long-lived fission product, which can be found in high-level radioactive liquid wastes (HLLW). Determination of the Pd contents in HLLW is essential to evaluate the long-term safety of HLLW repositories. However, the Pd content in HLLW has not been reported because of difficulties in pretreatment for the measurement. In this study, we investigated applicability of laser-induced photoreduction to HLLW solution: it enables a simple and non-contact separation of Pd. The results showed the recovery of 60% was achieved at the conditions: 40% ethanol, 20 min irradiation, 100 mJ of pulse energy. Additionally, major radionuclides and potentially interfering components in ICP-MS were removed from the simulated HLLW over a wide concentration range of Pd from 0.24 to 24 mg L, showing the applicability of the proposed separation technique to HLLW samples.
Saeki, Morihisa*; Taguchi, Tomitsugu*; Oba, Hironori*; Matsumura, Daiju; Tsuji, Takuya; Yomogida, Takumi
Denki Gakkai Kenkyukai Shiryo, Denshi Zairyo Kenkyukai (EFM-17-010
021), p.15 - 18, 2017/09
Irradiation of nanosecond pulsed UV laser into a solution of palladium ion leads to formation of palladium particles with sub-micron size particles by time-resolved X-ray absorption spectroscopy.
Yamasaki, Shinya*; Tanaka, Kazuya; Kozai, Naofumi; Onuki, Toshihiko
Applied Geochemistry, 78, p.279 - 286, 2017/03
Times Cited Count：4 Percentile：18.31(Geochemistry & Geophysics)This study examined the rate constant for the U(VI) reduction process by three flavin analogues, which are redox-active biomolecules secreted from anaerobic bacteria, to elucidate their substituent group effect on the U(VI) reduction rate by electrochemical methods. The formation of the U(IV) was monitored by UV-vis spectrometry in the presence of the flavins. The rate constant for the U(VI) reduction by the flavins was determined. The apparent reduction potential of U(VI) increased about 0.2 V in the presence of the mediators, which strongly suggests that the biological electron mediator makes the U(VI) reduction possible even under more oxidative conditions.
