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Journal Articles

Unusually kinetically inert monocationic neptunyl complex with a fluorescein-modified 1,10-phenanthroline-2,9-dicarboxylate ligand; Specific separation and detection in gel electrophoresis

Yamagata, Kazuhito*; Ouchi, Kazuki; Marumo, Kazuki*; Tasaki-Handa, Yuiko*; Haraga, Tomoko; Saito, Shingo*

Inorganic Chemistry, 62(2), p.730 - 738, 2023/01

 Times Cited Count:1 Percentile:81.75(Chemistry, Inorganic & Nuclear)

The inert NpO$$_{2}$$$$^{+}$$ complex with a fluorescein-modified phenanthroline-2,9-dicarboxylic acid was found by kinetic selection using polyacrylamide gel electrophoresis (PAGE) from a small chemical library. The small spontaneous dissociation rate constant of 8$$times$$10$$^{-6}$$ s$$^{-1}$$ (the half-life of 23 hours) was determined. This is the singly-charged NpO$$_{2}$$$$^{+}$$ complex exhibiting unusual kinetic inertness in aqueous solution, one million times slower than widely accepted fast kinetics of neptunyl complexes. Selective fluorescence detection of NpO$$_{2}$$$$^{+}$$ was achieved in PAGE with a detection limit of 68 pmol dm$$^{-3}$$(17 fg). This system was successfully applied to simulated spent nuclear fuel and high-level radioactive waste samples.

Journal Articles

Stoichiometry between humate unit molecules and metal ions in supramolecular assembly induced by Cu$$^{2+}$$ and Tb$$^{3+}$$ 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

 Times Cited Count:4 Percentile:36.59(Engineering, Environmental)

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$$^{2+}$$ and Tb$$^{3+}$$ 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$$^{2+}$$ and Tb$$^{3+}$$ 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.

Journal Articles

Advanced gel electrophoresis techniques reveal heterogeneity of humic acids based on molecular weight distributions of kinetically inert Cu$$^{2+}$$-humate complexes

Marumo, Kazuki*; Matsumoto, Atsumasa*; Nakano, Sumika*; Shibukawa, Masami*; Saito, Takumi*; Haraga, Tomoko; Saito, Shingo*

Environmental Science & Technology, 53(24), p.14507 - 14515, 2019/12

 Times Cited Count:7 Percentile:29.54(Engineering, Environmental)

Humic acids (HA) are responsible for the fate of metal ions in the environment. We developed a polyacrylamide gel electrophoresis (PAGE) technique to investigate the MW distributions of metal ion (copper ion). Combining contaminant-metal-free and high-resolution PAGE systems for HA provided accurate MW distributions for the metal ions. Coupling this system with UV-Vis spectrometry and the excitation-emission matrix (EEM) spectrometry-parallel factor analysis (PARAFAC) method revealed new insights into metal-HA complex. Interestingly, the MW distributions of the three metal ions were entirely different, indicating that the presence of specific binding environments in HA for the metal ions depending its MW. The MW distributions of five fluorescent components were associated with the metal ion distributions. Our PAGE-based methodology suggests that metal binding sites and fluorescent components in HA exhibit heterogeneity in terms of metal binding affinity and MW.

Oral presentation

Supramolecular formation of humic acids via complexation with metal ion investigated by two dimensional gel electrophoresis

Marumo, Kazuki*; Saito, Takumi*; Haraga, Tomoko; Shibukawa, Masami*; Saito, Shingo*

no journal, , 

no abstracts in English

Oral presentation

Aggregation reaction analysis of humic acids via complexation with lanthanide and actinide ions by means of two dimensional gel electrophoresis

Marumo, Kazuki*; Saito, Takumi*; Haraga, Tomoko; Shibukawa, Masami*; Saito, Shingo*

no journal, , 

no abstracts in English

Oral presentation

Evaluation for molecular weight distribution of actinide ions complexed with humic acid by gel electrophoresis

Haraga, Tomoko; Marumo, Kazuki*; Saito, Takumi*; Shibukawa, Masami*; Saito, Shingo*

no journal, , 

no abstracts in English

Oral presentation

Molecular weight distribution of actinide ions complexed with humic acid measured by gel electrophoresis techniques

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

no journal, , 

no abstracts in English

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