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Journal Articles

The Kinetics and mechanism of H$$_{2}$$O$$_{2}$$ decomposition at the U$$_{3}$$O$$_{8}$$ surface in bicarbonate solution

McGrady, J.; Kumagai, Yuta; Watanabe, Masayuki; Kirishima, Akira*; Akiyama, Daisuke*; Kitamura, Akira; Kimuro, Shingo

RSC Advances (Internet), 11(46), p.28940 - 28948, 2021/08

 Times Cited Count:0

Journal Articles

Synthesis and characterization of iodovanadinite using PdI$$_{2}$$, an iodine source for the immobilisation of radioiodine

Johnstone, E. V.*; Bailey, D. J.*; Lawson, S.*; Stennett, M. C.*; Corkhill, C. L.*; Kim, M.*; Heo, J.*; Matsumura, Daiju; Hyatt, N. C.*

RSC Advances (Internet), 10(42), p.25116 - 25124, 2020/07

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

Journal Articles

Complexation and bonding studies on [Ru(NO)(H$$_{2}$$O)$$_{5}$$]$$^{3+}$$ with nitrate ions by using density functional theory calculation

Kato, Akane*; Kaneko, Masashi; Nakashima, Satoru*

RSC Advances (Internet), 10(41), p.24434 - 24443, 2020/06

 Times Cited Count:5 Percentile:62.74(Chemistry, Multidisciplinary)

Complexation reactions of ruthenium-nitrosyl complexes in HNO$$_{3}$$ solution were investigated by density functional theory (DFT) calculations in order to predict the stability of Ru species in high-level radioactive liquid waste (HLLW) solution. Equilibrium structure of [Ru(NO)(NO$$_{3}$$)$$_{3}$$(H$$_{2}$$O)$$_{2}$$] obtained by DFT calculations reproduced the experimental Ru-ligands bond lengths and IR frequencies reported previously. Comparison of the Gibbs energies among the geometrical isomers revealed that the complexation reactions of the ruthenium-nitrosyl complexes with NO$$_{3}$$$$^{-}$$ proceed via the NO$$_{3}$$$$^{-}$$ coordination to the equatorial plane toward the Ru-NO axis. We also estimated Gibbs energy differences on the stepwise complexation reactions to succeed in reproducing the fraction of Ru-NO species in 6 M HNO$$_{3}$$ solution, such as in HLLW, by considering the association energy between the Ru-NO species and the substituting ligands. Electron density analyses of the complexes indicated that the strength of the Ru-ligands coordination bonds depends on the stability of the Ru species and the Ru complex without NO$$_{3}$$$$^{-}$$ at the axial position is more stable than that wit NO$$_{3}$$$$^{-}$$, which might attribute to the difference in the trans influence between H$$_{2}$$O and NO$$_{3}$$$$^{-}$$. Finally, we demonstrated the complexation kinetics in the reactions $$x = 1 rightarrow x = 2$$. The present study is expected to enable us to model the precise complexation reactions of platinum-group metals in HNO$$_{3}$$ solution.

Journal Articles

Hydrogen absorption and desorption on Rh nanoparticles revealed by ${it in situ}$ dispersive X-ray absorption fine structure spectroscopy

Song, C.*; Seo, O.*; Matsumura, Daiju; Hiroi, Satoshi*; Cui, Y.-T.*; Kim, J.*; Chen, Y.*; Tayal, A.*; Kusada, Kohei*; Kobayashi, Hirokazu*; et al.

RSC Advances (Internet), 10(34), p.19751 - 19758, 2020/05

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

Journal Articles

Time-controlled synthesis of the 3D coordination polymer U(1,2,3-Hbtc)$$_{2}$$ followed by the formation of molecular poly-oxo cluster {$rm U$_{14}$$} containing hemimellitate uranium(IV)

Dufaye, M.*; Martin, N. P.*; Duval, S.*; Volkringer, C.*; Ikeda, Atsushi; Loiseau, T.*

RSC Advances (Internet), 9(40), p.22795 - 22804, 2019/07

AA2019-0270.pdf:1.14MB

 Times Cited Count:8 Percentile:60.04(Chemistry, Multidisciplinary)

Two coordination compounds bearing tetravalent uranium (UIV)) were synthesized in the presence of tritopic hemimellitic acid in acetonitrile with a controlled amount of water (H$$_{2}$$O/U $${approx}$$ 8) and structurally characterized. The slow hydrolysis reaction together with the partial decomposition of the starting organic reactants into oxalate and acetate molecules induces the generation of such a large poly-oxo cluster with fourteen uranium centers. Structural comparisons with other closely related uranium-containing clusters, such as the {$rm U$_{12}$$}$ cluster based on the association of inner core [U$_{6}$$O$$_{8}$$] with three dinuclear sub-units {$rm U$_{2}$$}, were performed.

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:7 Percentile:42.43(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

Role of Tf$$_{2}$$N$$^{-}$$ anions in the ionic liquid-water distribution of europium(III) chelates

Okamura, Hiroyuki; Aoyagi, Noboru; Shimojo, Kojiro; Naganawa, Hirochika; Imura, Hisanori*

RSC Advances (Internet), 7(13), p.7610 - 7618, 2017/01

 Times Cited Count:14 Percentile:55.9(Chemistry, Multidisciplinary)

The role of bis(trifluoromethanesulfonyl)imide (Tf$$_{2}$$N$$^{-}$$) anions in the ionic liquid-water distribution systems of the Eu(III) chelates with 2-thenoyltrifluoroacetone (Htta) was investigated by the liquid-liquid distribution and time-resolved laser-induced fluorescence spectroscopy (TRLFS). The effect of the ionic liquids on the distribution constant of Eu(tta)$$_{3}$$ was evaluated by the regular solution theory. The distribution constant of Eu(tta)$$_{3}$$ in 1-alkyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide ([C$$_{n}$$mim][Tf$$_{2}$$N]) was increased dramatically by the solvation effects of Eu(tta)$$_{3}$$ in [C$$_{n}$$mim][Tf$$_{2}$$N]. TRLFS for [Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$] synthesized revealed that the Eu(tta)$$_{3}$$ chelate was almost completely dehydrated in a series of [C$$_{n}$$mim][Tf$$_{2}$$N]. The Eu(tta)$$_{3}$$ chelate exists as di- or tri-hydrates in 1-ethyl-3-methylimidazolium perchlorate ([C$$_{2}$$mim][ClO$$_{4}$$]) containing 20 M water, whereas mono-hydrated chelate was formed in [C$$_{2}$$mim][Tf$$_{2}$$N, ClO$$_{4}$$] in the presence of 0.50 M Tf$$_{2}$$N$$^{-}$$ and 20 M water. These results show that the coordinated water molecules of [Eu(tta)$$_{3}$$(H$$_{2}$$O)$$_{3}$$] were replaced by the Tf$$_{2}$$N$$^{-}$$ anions. In fact, an anionic adduct, [Eu(tta)$$_{3}$$(Tf$$_{2}$$N)]$$^{-}$$, was observed by electrospray ionization mass spectrometry in the presence of [C$$_{4}$$mim][Tf$$_{2}$$N].

Journal Articles

Effect of storage environment on hydrogen generation by the reaction of Al with water

Wang, Y.-Q.*; Gai, W.-Z.*; Zhang, X.-Y.*; Pan, H.-Y.*; Cheng, Z.-X.*; Xu, P. G.; Deng, Z.-Y.*

RSC Advances (Internet), 7(4), p.2103 - 2109, 2017/01

AA2016-0521.pdf:1.55MB

 Times Cited Count:18 Percentile:66.56(Chemistry, Multidisciplinary)

Journal Articles

Kinetics study of the Al-water reaction promoted by an ultrasonically prepared Al(OH)$$_{3}$$ suspension

Liang, G.-H.*; Gai, W.-Z.*; Deng, Z.-Y.*; Xu, P. G.; Cheng, Z.*

RSC Advances (Internet), 6(42), p.35305 - 35314, 2016/04

AA2016-0023.pdf:1.41MB

 Times Cited Count:13 Percentile:52.59(Chemistry, Multidisciplinary)

Journal Articles

Sequential radiation chemical reactions in aqueous bromide solutions; Pulse radiolysis experiment and spur model simulation

Yamashita, Shinichi*; Iwamatsu, Kazuhiro; Maehashi, Yuki*; Taguchi, Mitsumasa; Hata, Kuniki; Muroya, Yusa*; Katsumura, Yosuke*

RSC Advances (Internet), 5(33), p.25877 - 25886, 2015/02

 Times Cited Count:11 Percentile:42.31(Chemistry, Multidisciplinary)

Pulse radiolysis experiments were carried out to observe transient absorptions of reaction intermediates produced in N$$_{2}$$O$$^{-}$$ and Ar-saturated aqueous solutions containing 0.9-900 mM NaBr. The most important species among the reaction intermediates are BrOH $$^{cdot -}$$ and Br$$_{2}$$ $$^{cdot -}$$, which commonly have absorption peaks around 360 nm. The experimental results were compared with the results of simulation based on a spur diffusion model. Each of several complicated sequential radiation-induced chemical reactions was carefully considered, optimizing its rate constant within a range of reported values. All the experimental results were able to be universally reproduced by the simulation, assuming a reaction not yet reported, 2BrOH$$^{cdot -}$$ $$rightarrow$$ Br$$_{2}$$ + 2OH$$^{-}$$, with a rate constant of 3.8 $$times$$ 10$$^{9}$$ M$$^{-1}$$ s$$^{-1}$$, which is significant only within 10 micro-s for rather high bromide concentrations ($$>$$ 10 mM). Primary $$G$$ values, which are yields after sufficient diffusion from the spur to the perimeter region during 100 ns, of major water decomposition products, as well as of the reaction intermediates, were calculated for N$$_{2}$$O$$^{-}$$ and Ar-saturated conditions as a function of NaBr concentration.

Journal Articles

Monte Carlo simulation studies of cation selectivity in ion exchange of zeolites

Nakamura, Hiroki; Okumura, Masahiko; Machida, Masahiko

RSC Advances (Internet), 4(95), p.52757 - 52761, 2014/10

 Times Cited Count:6 Percentile:23.25(Chemistry, Multidisciplinary)

In order to evaluate the selectivity for specific cations in ion-exchange of zeolites, we calculate the ion-exchange isotherms in various zeolites using Monte Carlo simulation techniques. The calculation results agree well with experiments. Furthermore, we examine the Si/Al-ratio dependence on the cation selectivity and find that the Cs selectivity once increases with the Si/Al ratiobut saturates above a certain value. These results reveal that the selectivity for Cs is enhanced cooperatively by microporous structure and the Si/Al ratio of the zeolite framework. The present simulation scheme is promising in selecting useful materials for Cs decontamination in waste treatments.

Journal Articles

Origin of the enhancement of electrocatalytic activity and durability of PtRu alloy prepared from a hetero binuclear Pt-Ru complex for methanol oxidation reactions

Okawa, Yukihisa*; Masuda, Takuya*; Uehara, Hiromitsu*; Matsumura, Daiju; Tamura, Kazuhisa; Nishihata, Yasuo; Uosaki, Kohei*

RSC Advances (Internet), 3(35), p.15094 - 15101, 2013/09

 Times Cited Count:9 Percentile:39.22(Chemistry, Multidisciplinary)

Journal Articles

Formation of an Fe-H complex anion in YFe$$_{2}$$; Adjustment of imbalanced charge by additional Li as an electron donor

Matsuo, Motoaki*; Saito, Hiroyuki; Machida, Akihiko; Sato, Ryutaro*; Takagi, Shigeyuki*; Miwa, Kazutoshi*; Watanuki, Tetsu; Katayama, Yoshinori; Aoki, Katsutoshi; Orimo, Shinichi*

RSC Advances (Internet), 3(4), p.1013 - 1016, 2013/01

 Times Cited Count:16 Percentile:53.51(Chemistry, Multidisciplinary)

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