Heterogeneous aggregation of humic acids studied by small-angle neutron and X-ray scattering

Saito, Takumi*; Motokawa, Ryuhei; Okubo, Takahiro*; Miura, Daisuke*; Kumada, Takayuki

Environmental Science & Technology, 57(26), p.9802 - 9810, 2023/07

https://doi.org/10.1021/acs.est.3c02028

Outlining zircon growth in a granitic pluton using 3D cathodoluminescence patterns, U-Pb age, titanium concentration, and Th/U; Implications for the magma chamber process of Okueyama granite, Kyushu, Japan

Yuguchi, Takashi*; Ito, Daichi*; Yokoyama, Tatsunori; Sakata, Shuhei*; Suzuki, Satoshi*; Ogita, Yasuhiro; Yagi, Koshi*; Imura, Takumi*; Motai, Satoko*; Ono, Takeshi*

Lithos, 440-441, p.107026_1 - 107026_14, 2023/03

https://doi.org/10.1016/j.lithos.2023.107026

We propose a new method for elucidating zircon growth in granitic plutons, based on variations in three-dimensional 3D cathodoluminescence (CL) patterns, U-Pb ages, titanium concentration, and Th/U ratios. We focused on the zircon growth processes in the Okueyama granite (OKG) in central Kyushu, Japan, to obtain interpretations of magma chamber processes that result in the formation of granitic plutons. The OKG consists of three lithofacies: biotite granite (BG), hornblende granite (HG), and hornblende granodiorite (HGD). To determine the 3D internal structure and growth pattern of a zircon crystal, we performed CL observations for multi-sections of the samples. Simultaneously, we also determined the zircon U-Pb age and titanium concentration of the center sections of the samples. The 3D distribution of the oscillatory zoning can be used to determine the crystal nucleus. The simultaneous determination of zircon U-Pb ages and Ti concentrations of the granite samples indicates the time-temperature (t-T) history of granitic magma before its solidification. The t-T histories of the BG, HG, and HGD represented similar cooling behaviors within the magma chamber: rapid cooling from the zircon crystallization temperature to the closure temperature of the biotite K-Ar system between 16 Ma and 10 Ma. The variations in the Th/U ratios against temperature also demonstrate a different trend at the boundary of approximately 670 C. Fractional crystallization in the magma chamber progressed significantly at temperatures above 670 C; below 670 C, crystallization progressed slowly, indicating only minimal changes in the magma composition. The variations in the Th/U ratio against temperature in the BG, HG, and HGD portrayed common tendencies, indicating the same behavior in the progression of fractional crystallization among the three lithofacies, which in turn, represented the same behavior within the entire magma chamber.

Lanthanide and actinide ion complexes containing organic ligands investigated by surface-enhanced infrared absorption spectroscopy

Hirata, Sakiko*; Kusaka, Ryoji; Meiji, Shogo*; Tamekuni, Seita*; Okudera, Kosuke*; Hamada, Shoken*; Sakamoto, Chihiro*; Honda, Takumi*; Matsushita, Kosuke*; Muramatsu, Satoru*; et al.

Inorganic Chemistry, 62(1), p.474 - 486, 2023/01

https://doi.org/10.1021/acs.inorgchem.2c03618

Current status of Geological disposal by "all-Japan" activities, 6; Post-closure safety assessment (2)

Tachi, Yukio; Saito, Takumi*; Kirishima, Akira*

Nihon Genshiryoku Gakkai-Shi ATOMO, 64(5), p.290 - 295, 2022/05

https://doi.org/10.3327/jaesjb.64.5_290

no abstracts in English

Dispersive XAFS Study on the Laser-Induced Reduction of a Rh ion complex; Presence of a Rh Intermediate in Direct Photoreduction

Saeki, Morihisa*; Matsumura, Daiju; Nakanishi, Ryuzo*; Yomogida, Takumi; Tsuji, Takuya; Saito, Hiroyuki*; Oba, Hironori*

Journal of Physical Chemistry C, 126(12), p.5607 - 5616, 2022/03

https://doi.org/10.1021/acs.jpcc.1c10160

The reaction mechanism of the direct photoreduction of a Rh ion complex to a Rh species induced by pulsed ultraviolet laser irradiation was studied using dispersive X-ray absorption fine structure (DXAFS) spectroscopy. The time-resolved X-ray absorption near edge structure (XANES) showed the absence of isosbestic points and suggested that more than two Rh species contribute toward the direct photoreduction of Rh. Analysis of the time-resolved XANES data by singular value deposition showed that the direct photoreduction involves three Rh species. Multivariate curve resolution by alternating least-squares analysis (MCR-ALS) of the time-resolved XANES data gave pure spectra and concentration profiles of the three Rh species. The Rh species were assigned to Rh, Rh, and Rh species based on the features of the pure XANES spectra. The concentration profiles suggested that the direct photoreduction proceeds in the order of Rh Rh Rh. A reaction mechanism, which was proposed involving photoreductions of Rh and Rh, photoinduced autocatalytic reductions of Rh and Rh, and photooxidation of Rh, well reproduced the concentration profiles of three Rh species.

Stoichiometry between humate unit molecules and metal ions in supramolecular assembly induced by Cu and Tb measured by gel electrophoresis techniques

Nakano, Sumika*; Marumo, Kazuki*; Kazami, Rintaro*; Saito, Takumi*; Haraga, Tomoko; Tasaki-Handa, Yuiko*; Saito, Shingo*

Environmental Science & Technology, 55(22), p.15172 - 15180, 2021/11

https://doi.org/10.1021/acs.est.1c03993

Humic acid (HA) can strongly complex with metal ions to form a supramolecular assembly via coordination binding. However, determining the supramolecular size distribution and stoichiometry between small HA unit molecules constituting HA supramolecule and metal ions has proven to be challenging. Here, we investigated the changes in the size distributions of HAs induced by Cu and Tb ions using a unique polyacrylamide gel electrophoresis (PAGE) for the separation and quantification of HA complexes and metal ions bound, followed by UV-Vis spectroscopy and EEM-PARAFAC. It was found that the supramolecular behaviors of Cu and Tb complexes with HA collected from peat and deep groundwater (HHA) differed. Our results suggest that this supramolecular stoichiometry is related to the abundance of sulfur atoms in the elemental composition of HHA. Our results provide new insights into HA supramolecules formed via metal complexation.

Application of an augmentation method to MCR-ALS analysis for XAFS and Raman data matrices in the structural change of isopolymolybdates

Saeki, Morihisa*; Yomogida, Takumi; Matsumura, Daiju; Saito, Takumi*; Nakanishi, Ryuzo*; Tsuji, Takuya; Oba, Hironori*

Analytical Sciences, 36(11), p.1371 - 1378, 2020/11

https://doi.org/10.2116/analsci.20P147

We measured X-ray absorption fine structure (XAFS) and Raman spectra of isopolymolybdates(VI) in HNO solution (0.15- 4.0 M), which change their geometries depending on acid concentration, and performed simultaneous resolution of the XAFS and Raman data using a multivariate curve resolution by alternating least-squares (MCR-ALS) analysis. In iterative ALS optimization, initial data matrices were prepared by two different methods. The MCR-ALS result of single XAFS data matrix shows large dependence on the preparation method of the initial data matrices. The MCR-ALS result of an augmented matrix of Raman and XAFS data has little dependence on the initial data matrices. It indicates that the augmentation method effectively improves the rotation ambiguities in the MCR-ALS analysis of the XAFS data. Based on the model fitting of the pure EXAFS oscillations, we revealed the change of [MoO(HO)] [MoO(HO)] [HMoO(HO)] in the highly concentrated HNO solution.

Modulation of Dirac electrons in epitaxial BiSe ultrathin films on van der Waals ferromagnet CrSiTe

Kato, Takemi*; Sugawara, Katsuaki*; Ito, Naohiro*; Yamauchi, Kunihiko*; Sato, Takumi*; Oguchi, Tamio*; Takahashi, Takashi*; Shiomi, Yuki*; Saito, Eiji; Sato, Takafumi*

Physical Review Materials (Internet), 4(8), p.084202_1 - 084202_6, 2020/08

https://doi.org/10.1103/PhysRevMaterials.4.084202

Measurement of the angular distribution of -rays after neutron capture by La for a T-violation search

Okudaira, Takuya; Shimizu, Hirohiko*; Kitaguchi, Masaaki*; Hirota, Katsuya*; Haddock, C. C.*; Ito, Ikuya*; Yamamoto, Tomoki*; Endo, Shunsuke*; Ishizaki, Kohei*; Sato, Takumi*; et al.

EPJ Web of Conferences, 219, p.09001_1 - 09001_6, 2019/12

https://doi.org/10.1051/epjconf/201921909001

Parity violating effects enhanced by up to 10 times have been observed in several neutron induced compound nuclei. There is a theoretical prediction that time reversal (T) violating effects can also be enhanced in these nuclei implying that T-violation can be searched for by making very sensitive measurements. However, the enhancement factor has not yet been measured in all nuclei. The angular distribution of the (n,) reaction was measured with La by using a germanium detector assembly at J-PARC, and the enhancement factor was obtained. From the result, the measurement time to achieve the most sensitive T-violation search was estimated as 1.4 days, and a 40% polarized La target and a 70% polarized He spin filter whose thickness is 70 atmcm are needed. Therefore high quality He spin filter is developed in JAEA. The measurement result of the (n,) reaction at J-PARC and the development status of the He spin filter will be presented.

Reduction behaviors of permanganate by microbial cells and concomitant accumulation of divalent cations of Mg, Zn+, and Co

Kato, Tomoaki*; Yu, Q.*; Tanaka, Kazuya; Kozai, Naofumi; Saito, Takumi*; Onuki, Toshihiko

Journal of Environmental Sciences, 86, p.78 - 86, 2019/12

https://doi.org/10.1016/j.jes.2019.05.007

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.