Using CO Reactions to Achieve Mass-spectrometric Discrimination in Simultaneous Plutonium-isotope Speciation with Inductively Coupled Plasma-Tandem Mass Spectrometry

Matsueda, Makoto; Kawakami, Tomohiko*; Koarai, Kazuma; Terashima, Motoki; Fujiwara, Kenso; Iijima, Kazuki; Furukawa, Makoto*; Takagai, Yoshitaka*

Chemistry Letters, 51(7), p.678 - 682, 2022/07

https://doi.org/10.1246/cl.220160

New methodology for a simultaneous isotope speciation of various Pu isotopes without complicated isobaric interferences is developed by using inductively coupled plasma-mass spectrometry (ICP-MS). In analyzing ICP tandem MS (ICP-MS/MS), CO gas reactions in a dynamic reaction cell (DRC) almost eliminated the background noise intensity produced by isobaric interference from isotopes originating from actinides such as Am, Cm, and U at the locations (m/z) of significant Pu isotopes (Pu, Pu, Pu, Pu, Pu).

Rapid analysis of Sr in cattle bone and tooth samples by inductively coupled plasma mass spectrometry

Koarai, Kazuma; Matsueda, Makoto; Aoki, Jo; Yanagisawa, Kayo*; Terashima, Motoki; Fujiwara, Kenso; Kino, Yasushi*; Oka, Toshitaka; Takahashi, Atsushi*; Suzuki, Toshihiko*; et al.

Journal of Analytical Atomic Spectrometry, 36(8), p.1678 - 1682, 2021/08

https://doi.org/10.1039/D1JA00086A

Rapid analysis of Sr in bone and tooth samples of cattle were achieved by an inductively coupled plasma mass spectrometry (ICP-MS) coupled with mass shift and solid phase extraction techniques. Limit of detection (LOD) in the ICP-MS measurement of 0.1 g samples was lower than that of the radioactivity measurement. Analytical time of the ICP-MS method was reduced from 20 days to 11 hours, compared with the radiometric method. Therefore, the ICP-MS method can be rapid and useful procedure of Sr in small bone and tooth samples derived from terrestrial animals.

Development of solid-phase extraction technique for ICP-MS analysis of iodine-129 in environmental samples; Comparative study of anion-exchange and silver ion-supported resins on isolation of Iodine-129 from interference elements

Aoki, Jo; Matsueda, Makoto; Koarai, Kazuma; Terashima, Motoki; Fujiwara, Kenso; Abe, Hironobu

JAEA-Research 2021-002, 20 Pages, 2021/05

JAEA-Research-2021-002.pdf:2.75MB

In order to analyze extremely low concentrations of I in environmental samples by ICP-MS with high sensitivity and rapidity, it is necessary to remove interfering elements (Na, Mg, K, Ca, Mo, Cd and In) using a pretreatment method with Solid-phase Extraction Resin. Anion Exchange Resins with amino groups have been widely used as Solid-phase Extraction Resins, while Ag+ Supported Resins have also been widely used in recent years. It is necessary to optimize the pretreatment technique based on characteristics of the resins. In this study, we compared in terms of separation of I from matrix elements (Na, Mg, K, Ca, Mo, Cd and In) for DOWEX1-X8, AG 1-X8 and CL Resin, and investigated their suitability for ICP-MS analysis of I in environmental samples. The results of adsorption and elution experiments showed that all resins examined uptake and elute I quantitatively. CL Resin showed the highest removal performance of interfering elements, with 3.1% of Mo remaining, but other interfering elements were removed below the detection limit of ICP-MS. However, the Mo remained after the CL Resin treatment could interfere the ICP-MS measurement of I, based on the consideration of ratio of I and Mo. The eluate from CL Resin was treated with a Cation exchange resin (DOWEX 50WX8). As a result, Mo in the eluate was removed by up to 98% and the interference from Mo was reduced to measurable level. Therefore, the pretreatment method using CL Resin in combination with DOWEX 50WX8 is effective for ICP-MS analysis of I at extremely low concentrations (background level).

Applicability of Sr resin for ICP-MS measurement of Sr in hard tissue samples

Koarai, Kazuma; Matsueda, Makoto; Aoki, Jo; Yanagisawa, Kayo*; Fujiwara, Kenso; Terashima, Motoki; Kitamura, Akihiro; Abe, Hironobu

KEK Proceedings 2020-4, p.180 - 185, 2020/11

Strontium-90 and Y, its daughter nuclide, adverse effects on the bone marrow. Monitoring of Sr in the bones have been required after the Fukushima-Daiichi Nuclear Power Plant accident. However, conventional radioactivity measurement method for Sr requires a complicated separation of Y and a time-consuming measurement. ICP-MS system has been applied to Sr concentration survey of water, soil, and edible part of fish. We applied the ICP-MS system for the bones for the first time. In this study, reference bone (JSAC 0785 fish bone) was used as measurement samples. Sample preparation of the bone was performed using a microwave digestion instrument. After sample preparation, Sr was determined using ICP-MS system with cascade separation steps based on on-line column separation and oxygen reaction. Strontium-90 in the bones was successfully separated from Ca, Ba, Y, Zr, Fe, Se, and Ge, which interfered in ICP-MS measurement, in the separation steps.

Determination of humic substances in deep groundwater from sedimentary formations by the carbon concentration-based DAX-8 resin isolation technique

Terashima, Motoki; Endo, Takashi*; Miyakawa, Kazuya

Journal of Nuclear Science and Technology, 57(4), p.380 - 387, 2020/04

https://doi.org/10.1080/00223131.2019.1688730

Physicochemical and ion-binding properties of highly aliphatic humic substances extracted from deep sedimentary groundwater

Saito, Takumi; Terashima, Motoki; Aoyagi, Noboru; Nagao, Seiya*; Fujitake, Nobuhide*; Onuki, Toshihiko

Environmental Science; Processes & Impacts, 17(8), p.1386 - 1395, 2015/08

https://doi.org/10.1039/C5EM00176E

The deep groundwater HSs were different from surface HSs, having high aliphaticities, sulfur contents, and small molecular sizes. The amounts of their acidic functional groups were comparable to or slightly larger than those of surface HSs; however, the magnitude of Cu binding to the deep groundwater HSs was smaller. The NICA-Donnan model attributed this to the binding of Cu to chemically homogeneous carboxylic-type sites via mono-dentate coordination at relatively low pH. The binding mode tended to shift to multi-dentate coordination with carboxylic-type and probably more heterogeneous alcoholic hydroxide-type groups at higher pH. This study shows the particularity of the deep groundwater HSs in terms of their physicochemical and ion-binding properties, compared with surface HSs.

Sorption and diffusion of Eu in sedimentary rock in the presence of humic substance

Seida, Yoshimi; Terashima, Motoki; Tachi, Yukio; Iijima, Kazuki; Nakazawa, Toshiyuki*; Yamada, Norikazu*; Yui, Mikazu

Radiochimica Acta, 98(9-11), p.703 - 709, 2010/11

https://doi.org/10.1524/ract.2010.1771

Diffusion and sorption behaviors of Eu in sedimentary rock were investigated in the presence of humic substance in the present study. Sedimentary rock obtained from Horonobe URL test site in Hokkaido, Japan, (accessible pore diameter is around several to several ten nanometer) was used. The Diffusion behaviors of Eu were examined based on reservoir depletion method coupled with analysis of inner distribution of the radioactive elements in the rock. Time sequence of concentration of each radioactive element as well as the humic substance in the reservoir was obtained as a function of concentration and molecular size of humic substance. Coexistence of humic substance reduced the depletion of Eu in the reservoir, indicating complexation between the radioactive elements and the humic substance. On the contrary, obvious decrease of humic substance in the reservoir was not observed in the system. This observation suggests that the radioactive elements became hard to diffuse into the sedimentary rock due to an increase of their size through complexation with the humic substance. The sorption of Eu was reduced with increase of the humic substance although the sorption of the humic substance was not influenced by the existence of Th or Eu. The diffusion and sorption of Eu were found to be reduced in the presence of humic substance.

Eu(III) binding abilities of dissolved humic substances isolated from deep groundwater in Horonobe area, Hokkaido, Japan

Terashima, Motoki; Seida, Yoshimi; Iwatsuki, Teruki; Iijima, Kazuki; Yoshikawa, Hideki; Yui, Mikazu; Nagao, Seiya*

no journal, , 

Eu(III) binding abilities of dissolved humic substances (HSs), which were extracted from deep groundwater in the Horonobe Underground Research Center, Hokkaido, Japan, were investigated by fluorescence quenching technique. In the synthetic groundwater condition, the fluorescence quenching due to the binding with Eu(III) was not observed for the groundwater HSs, while that was observed for the Aldrich humic acid (HA). This result indicates that the binding ability of the groundwater HSs are different from that of Aldrich HA. Based on structural characteristics of the groundwater HSs, the differences in the binding ability are discussed.

In situ experiment for redox buffer capacity in the subsurface environment

Amano, Yuki; Nanjo, Isao; Iwatsuki, Teruki; Sasaki, Yoshito; Asano, Takahiro; Terashima, Motoki; Nagaoka, Toru*; Nakamura, Takamichi*; Yoshikawa, Hideki; Aoki, Kazuhiro

no journal, , 

In-situ experiment of redox reaction was conducted to assess the redox buffur capacity of water-rock-microbes system in the subsurface environment at 140 m depth of Horonobe Underground Research Laboratory. Dissolved oxygen was injected into a borehole, and the physico-chemical parameters (i.e. pH, ORP, DO, EC, etc.) and geochemical composition, microbial cell number, and microbial community structure were monitored continuously during the groundwater circulation. DO concentration could not detected after 10 hours from the injection. The concentration of Fe(II) was decreased with time, then the injected oxygen could be consumed by Fe(II). The rate of oxygen consumption during the experiment was 9.64 mg/L/day. The Eh value become stable at -208 mV after 5 days, then it showed that the reducing condition would be recovered quickly after closed condition.

Application of NICA-Donnan model to modelling of Eu(III) solubility in the presence of deep groundwater humic substances

Terashima, Motoki; Okazaki, Mitsuhiro; Iijima, Kazuki; Yui, Mikazu

no journal, , 

no abstracts in English