Origin of dissolved organic matter in deep groundwater of marine deposits and its implication for metal binding

Saito, Takumi*; Nishi, Shusaku*; Amano, Yuki; Beppu, Hikari*; Miyakawa, Kazuya

ACS ES&T Water (Internet), 3(12), p.4103 - 4112, 2023/12

https://doi.org/10.1021/acsestwater.3c00505

First-principles simulation of an ejected electron produced by monochromatic deposition energy to water at the femtosecond order

Kai, Takeshi; Toigawa, Tomohiro; Matsuya, Yusuke; Hirata, Yuho; Tezuka, Tomoya*; Tsuchida, Hidetsugu*; Yokoya, Akinari*

RSC Advances (Internet), 13(46), p.32371 - 32380, 2023/11

https://doi.org/10.1039/D3RA05075K

Although scientific knowledge of photolysis and radiolysis of water is widely used in the life sciences and other fields, the formation mechanism of the spatial distribution of hydrated electrons (spur) resulting from energy deposition to water is still not well understood. The chemical reaction times of hydrated electrons, OH radicals, and HO in the spur strongly depend on the spur radius. In our previous study, we elucidated the mechanism at a specific given energy (12.4 eV) by first-principles calculations. In the present study, we performed first-principles calculations of the spur radius at the deposition energies of 11-19 eV. The calculated spur radius is 3-10 nm, which is consistent with the experimental prediction (~4 nm) for the energy range of 8-12.4 eV, and the spur radius gradually increases with increasing energy. The spur radius is a new scientific knowledge and is expected to be widely used for estimating radiation DNA damage.

Comparison of Ichimura-Austern-Vincent and Glauber models for the deuteron-induced inclusive breakup reaction in light and medium-mass nuclei

Liu, H.*; Nakayama, Shinsuke; Lei, J.*; Ren, Z.*

Physical Review C, 108(1), p.014617_1 - 014617_8, 2023/07

https://doi.org/10.1103/PhysRevC.108.014617

In this paper, we study deuteron-induced inclusive breakup reaction and explore the and reactions for light and medium mass nuclei. Using the models of Ichimura, Austern, and Vincent and Glauber, we scrutinize the double differential cross-section of nonelastic breakup and compare the results for various reaction systems. Our findings indicate that the Glauber model, combined with a quantum -matrix, produces remarkable results in the deuteron-induced inclusive breakup reaction. While both models are proficient in predicting the outcomes of light and medium mass nuclei, the reaction showcases higher consistency than the reaction. Nevertheless, there are still significant discrepancies between experimental and theoretical cross-sections that require further investigation and analysis. This study opens up a new realm of possibilities for future research in the field.

Nature of the physicochemical process in water photolysis uncovered by a computer simulation

Kai, Takeshi; Toigawa, Tomohiro; Ukai, Masatoshi*; Fujii, Kentaro*; Watanabe, Ritsuko*; Yokoya, Akinari*

Journal of Chemical Physics, 158(16), p.164103_1 - 164103_8, 2023/04

New insight into water radiolysis and photolysis is indispensable in the dramatic progress of sciences and technologies in various research areas. In the radiation field, reactive hydrated electrons are considerably produced along radiation tracks. Although the formation results from a transient dynamic correlation between ejected electrons and water, the individual mechanisms of electron thermalization, delocalization, and polarization are unknown. Using a dynamic Monte Carlo code, we show herein that the ejected electrons are immediately delocalized by molecular excitations in parallel with phonon polarization and gradually thermalized by momentum transfer with an orientation polarization in a simultaneous manner. Our results show that these mechanisms heavily depend on the intermolecular vibration and rotation modes peculiar to water. We expect our approach to be a powerful technique for connecting physical and chemical processes in various solvents.

Investigation of hydrogen superoxide adsorption during ORR on Pt/C catalyst in acidic solution for PEFC by 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

https://doi.org/10.1016/j.jpowsour.2022.232508

Band gap opening in graphene by hybridization with Au (001) reconstructed surfaces

Terasawa, Tomoo; Matsunaga, Kazuya*; Hayashi, Naoki*; Ito, Takahiro*; Tanaka, Shinichiro*; Yasuda, Satoshi; Asaoka, Hidehito

Physical Review Materials (Internet), 7(1), p.014002_1 - 014002_10, 2023/01

https://doi.org/10.1103/PhysRevMaterials.7.014002

Au(001) surfaces exhibit a complex reconstructed structure [Hex-Au(001)] comprising a hexagonal surface and square bulk lattices, yielding a quasi-one-dimensional corrugated surface. When graphene was grown on this surface, the periodicity of the corrugated surface was predicted to change the electronic structure of graphene, forming bandgaps and new Dirac points. Furthermore, the graphene-Au interface is promising for bandgap generation and spin injection due to band hybridization. Here, we report the angle-resolved photoemission spectroscopy and density functional calculation of graphene on a Hex-Au(001) surface. The crossing point of the original and replica graphene bands showed no bandgap, suggesting that the one-dimensional potential was too small to modify the electronic structure. A bandgap of 0.2 eV was observed at the crossing point of the graphene and Au bands, indicating that the bandgap is generated using hybridization of the graphene and Au bands. We discussed the hybridization mechanism and concluded that the R30 configuration between graphene and Au and an isolated electronic structure of Au are essential for effective hybridization between graphene and Au. We anticipate that hybridization between graphene and Au would result in spin injection into graphene.

Uranium dissolution and uranyl peroxide formation by immersion of simulated fuel debris in aqueous HO solution

Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*; Sasaki, Takayuki*

Journal of Nuclear Science and Technology, 59(8), p.961 - 971, 2022/08

https://doi.org/10.1080/00223131.2021.2023055

We investigated potential degradation of fuel debris caused by HO, which is the oxidant of major impact from water radiolysis. We performed leaching experiments on different kinds of simulated debris comprising U, Fe, Cr, Ni, and Zr in an aqueous HO solution. Chemical analysis of the leaching solution showed that U dissolution was induced by HO. Raman analysis after the leaching revealed that uranyl peroxides were formed on the surface of the simulated debris. These results demonstrate that uranyl peroxides are possible alteration products of fuel debris from HO reaction. However, the sample in which the main uranium-containing phase was a U-Zr oxide solid solution showed much less uranium dissolution and no Raman signal of uranyl peroxides. Comparison of these results indicates that formation of an oxide solid solution of Zr with UO improves the stability of fuel debris against HO reaction.

Theoretical study of deuteron-induced reactions in the nuclear data field

Nakayama, Shinsuke; Iwamoto, Osamu; Watanabe, Yukinobu*; Ogata, Kazuyuki*

Few-Body Systems, 63(1), p.4_1 - 4_6, 2022/03

https://doi.org/10.1007/s00601-021-01712-2

Intensive neutron sources using deuteron accelerators have been proposed for not only science and engineering fields but also medical applications. For the engineering design of such facilities, accurate and comprehensive nuclear data of deuteron-induced reactions are indispensable. However, it is difficult to meet the requirement by employing experimental data alone. Thus, theoretical model calculations play a key role in completing the necessary nuclear data by interpolation and extrapolation of experimental data. Under the above situations, we have been developing a code system dedicated for deuteron-induced reactions, called DEURACS. In the present work, calculations using DEURACS are compared with available experimental data and validation of the present modelling in DEURACS is discussed. Moreover, the importance of consideration of the breakup processes for accurate prediction of deuteron-induced reactions is also presented.

Zeolite-assisted radiolysis of aromatic chlorides mitigating influence of coexisting ions in water matrix

Kumagai, Yuta; Kimura, Atsushi*; Taguchi, Mitsumasa*; Watanabe, Masayuki

Radiation Physics and Chemistry, 191, p.109831_1 - 109831_8, 2022/02

https://doi.org/10.1016/j.radphyschem.2021.109831

In this study, we investigated and compared the effects of a high-silica zeolite (HMOR) on the radiation-induced degradation of three aromatic chlorides, 2-chlorophenol (2-ClPh), 2-chloroaniline (2-ClAn), and 2-chlorobenzoic acid (2-ClBA), in order to examine its potential to reduce the influence of ions in water matrix in the irradiation treatment of water-soluble organic compounds. In the presence of ions reactive to radicals, the degradation of 2-ClPh in water was inhibited, but the combined use of HMOR much improved the degradation yield. This improvement was attributed to high performance of HMOR in adsorption of 2-ClPh. Similarly, HMOR was effective for adsorption of 2-ClAn and facilitated the 2-ClAn degradation by irradiation. In contrast, HMOR was poor at adsorption of 2-ClBA and consistently the degradation of 2-ClBA in the water-HMOR mixture was inhibited by the radical scavenger. These results demonstrate that HMOR can mitigate the influence of radical scavengers in water.

The First application of a GdAlGaO:Ce single-crystal scintillator to neutron radiography

Isegawa, Kazuhisa; Setoyama, Daigo*; Kimura, Hidehiko*; Shinohara, Takenao

Journal of Imaging (Internet), 7(11), p.232_1 - 232_9, 2021/11

https://doi.org/10.3390/jimaging7110232

Neutron radiography is regarded as complementary to X-ray radiography in terms of transmittance through materials, but its spatial resolution is still insufficient. In order to achieve higher resolution in neutron imaging, several approaches have been adopted such as optical magnification and event centroiding, and the authors focused on modification of the scintillator in this paper. A GdAlGaO:Ce single-crystal scintillator was applied to neutron radiography for the first time and was achieved a spatial resolution of 10.5 micrometers. The results indicate that this material can be a powerful candidate for a new neutron scintillator providing a resolution in micrometer order by optimizing the optical system and increasing the scintillator luminosity.