AIで核物質解析の迅速化に挑戦（Scientists Investigate Use of AI to Speed Analysis of Nuclear Materials）

2025-07-22 パシフィック・ノースウェスト国立研究所（PNNL）

Research on nuclear devices and debris is part of a large and ongoing program on nuclear forensics at Pacific Northwest National Laboratory. The Laboratory is a critical component of the nation’s capability to analyze nuclear and radioactive materials and events.　(Illustration by Chris DeGraaf | Pacific Northwest National Laboratory)

＜関連情報＞

• https://www.pnnl.gov/news-media/scientists-investigate-use-ai-speed-analysis-nuclear-materials
• https://pubs.rsc.org/en/content/articlelanding/2025/cp/d4cp04295f

水溶液中の金属-硝酸塩錯体の安定定数について On the stability constants of metal–nitrate complexes in aqueous solutions

Mohammadhasan Dinpajooh, Greta L. Hightower, Richard E. Overstreet, Lori A. Metz, Neil J. Henson, Niranjan Govind,  Andrew M. Ritzmann  and  Nicolas E. Uhnak
Physical Chemistry Chemical Physics  Published:10 Feb 2025
DOI:https://doi.org/10.1039/D4CP04295F

Abstract

Stability constants of simple reactions involving addition of the NO₃⁻ ion to hydrated metal complexes, [M(H₂O)_x]ⁿ⁺ are calculated with a computational workflow developed using cloud computing resources. The computational workflow performs conformational searches for metal complexes at both low and high levels of theories in conjunction with a continuum solvation model (CSM). The low-level theory is mainly used for the initial conformational searches, which are complemented with high-level density functional theory conformational searches in the CSM framework to determine the coordination chemistry relevant for stability constant calculations. In this regard, the lowest energy conformations are found to obtain the reaction free energies for the addition of one NO₃⁻ to [M(H₂O)_x]ⁿ⁺ complexes, where M represents Fe(II), Fe(III), Sr(II), Ce(III), Ce(IV), and U(VI), respectively. Structural analysis of hundreds of optimized geometries at high-level theory reveals that NO₃⁻ coordinates with Fe(II) and Fe(III) in either a monodentate or bidentate manner. Interestingly, the lowest-energy conformations of Fe(II) metal–nitrate complexes exhibit monodentate or bidentate coordination with a coordination number of 6 while the bidentate seven-coordinated Fe(II) metal–nitrate complexes are approximately 2 kcal mol⁻¹ higher in energy. Notably, for Fe(III) metal–nitrate complexes, the bidentate seven-coordinated configuration is more stable than the six-coordinated Fe(II) complexes (monodentate or bidentate) by a few thermal energy units. In contrast, Sr(II), Ce(III), Ce(IV), and U(VI) metal ions predominantly coordinate with NO₃⁻ in a bidentate manner, exhibiting typical coordination numbers of 7, 9, 9, and 5, respectively. Stability constants are accordingly calculated using linear free energy approaches to account for the systematic errors and good agreements are obtained between the calculated stability constants and the available experimental data.