Evaluation of Thermodynamic Model of Pd(II) Complex Formation with Isosaccharinic Acid

IF 16.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Accounts of Chemical Research Pub Date : 2024-01-17 DOI:10.1007/s10953-023-01352-6

Shingo Kimuro, Yayoi Taneichi, Hajime Iwata, Takamitsu Ishidera, Akira Kitamura, Yukio Tachi, Takeru Tanaka, Kana Hirano, Manami Hieda, Shunsuke Miyabe, Daisuke Kawamoto

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Abstract

Palladium-107 is one of the selected radionuclides in the safety assessment of geological disposal of radioactive waste. Although isosaccharinic acid (ISA) forms strong complexes with many elements and enhances element solubility, the thermodynamic evaluation of the complex of Pd with ISA has not been conducted. In this study, the solubility of Pd(OH)₂ at pH 8.5–12.5 in the presence of ISA was investigated under inert gas (N₂) atmosphere. Furthermore, the coordination state of aqueous Pd and ISA was investigated by X-ray absorption and Fourier transform infrared spectroscopy, respectively. According to experimental results, the number of OH ligands in the mixed complex depends on pH. The thermodynamic model and conditional equilibrium constants of the Pd-ISA complex were estimated by slope analyses of solubility experiments at different pH levels and ionic strengths based on the specific ion interaction theory. Hence, the impact of complexation with ISA on Pd(II) solubility under disposal conditions could be quantified using the proposed thermodynamic models in this study.

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评估 Pd(II) 与异糖精酸形成络合物的热力学模型

摘要钯-107 是放射性废物地质处置安全评估中选定的放射性核素之一。虽然异糖精酸（ISA）能与许多元素形成强络合物并提高元素的溶解度，但尚未对钯与 ISA 的络合物进行热力学评价。本研究在惰性气体（N2）环境下考察了 Pd(OH)2 在 pH 值为 8.5-12.5 的 ISA 存在下的溶解度。此外，还分别通过 X 射线吸收和傅立叶变换红外光谱法研究了水溶液中 Pd 和 ISA 的配位状态。实验结果表明，混合复合物中 OH 配体的数量取决于 pH 值。根据比离子相互作用理论，通过对不同 pH 值和离子强度下的溶解度实验进行斜率分析，估算出了 Pd-ISA 复合物的热力学模型和条件平衡常数。因此，利用本研究中提出的热力学模型，可以量化与 ISA 的络合对 Pd(II) 在弃置条件下溶解度的影响。

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来源期刊

Accounts of Chemical Research 化学-化学综合

CiteScore

31.40

自引率

1.10%

发文量

312

审稿时长

2 months

期刊介绍： Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.

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