三价锕系和镧系元素与水溶性和 CHON 相容配体的络合和萃取研究用于选择性萃取镅,Inorganic Chemistry

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三价锕系和镧系元素与水溶性和 CHON 相容配体的络合和萃取研究用于选择性萃取镅
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-10-23 , DOI: 10.1021/acs.inorgchem.2c02871
Patrik Weßling _{1,

2} , Melina Maag ₂ , Giana Baruth _{1,

2} , Thomas Sittel ₁ , Fynn S Sauerwein ₃ , Andreas Wilden ₃ , Giuseppe Modolo ₃ , Andreas Geist ₁ , Petra J Panak _{1,

2}

Affiliation

合成了用于选择性分离 Am(III) 的新型亲水配体：3,3'-([2,2'-bipyridine]-6,6'-diylbis(1 H -1,2,3-triazole-4,1-) diyl))bis(propan-1-ol) (PrOH-BPTD) 和 3,3'-([2,2'-bipyridine]-6,6'-diylbis(1 H -1,2,3-triazole-) 4,1-二基））双（乙醇-1-醇）（EtOH-BPTD）。通过时间分辨激光荧光光谱研究了 An(III) 和 Ln(III) 与 PrOH- 和 EtOH-BPTD 的络合。[ML ₂ ] ³⁺存在于 Cm(III) 和 Eu(III) 中，而 [ML] ³⁺仅与 Cm(III) 形成。稳定性常数显示 Cm(III) 优先于 Eu(III) 配位，而 PrOH-BPTD 是更强的配体。Am(III)、Cm(III) 和 Ln(III) 在含有萃取剂的有机相之间的分布N、N、N '、N'-四正辛基-3-氧杂戊二胺 (TODGA) 和含有 PrOH-BPTD 的水相作为时间和温度以及 TODGA、BPTD 和 HNO ₃浓度的函数进行了研究. 由 0.2 mol/L TODGA 和 0.04 mol/L PrOH-BPTD 在 0.33–0.39 mol/L HNO ₃中组成的系统允许选择性 Am(III) 反萃取到水相中，同时保持 Cm(III) 和 Ln(III) ) 在有机相中，将 PrOH-BPTD 标记为优化 AmSel 工艺（Am(III) 选择性萃取）的出色络合剂。

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Complexation and Extraction Studies of Trivalent Actinides and Lanthanides with Water-Soluble and CHON-Compatible Ligands for the Selective Extraction of Americium

Novel hydrophilic ligands to selectively separate Am(III) are synthesized: 3,3′-([2,2′-bipyridine]-6,6′-diylbis(1H-1,2,3-triazole-4,1-diyl))bis(propan-1-ol) (PrOH-BPTD) and 3,3′-([2,2′-bipyridine]-6,6′-diylbis(1H-1,2,3-triazole-4,1-diyl))bis(ethan-1-ol) (EtOH-BPTD). The complexation of An(III) and Ln(III) with PrOH- and EtOH-BPTD is studied by time-resolved laser fluorescence spectroscopy. [ML₂]³⁺ is found for both Cm(III) and Eu(III), while [ML]³⁺ is only formed with Cm(III). Stability constants show a preferential coordination of Cm(III) over Eu(III) with PrOH-BPTD being the stronger ligand. The distribution of Am(III), Cm(III), and Ln(III) between an organic phase containing the extracting agent N,N,N′,N′-tetra-n-octyl-3-oxapentanediamide (TODGA) and aqueous phases containing PrOH-BPTD is studied as a function of time and temperature as well as the TODGA, BPTD, and HNO₃ concentrations. A system composed of 0.2 mol/L TODGA and 0.04 mol/L PrOH-BPTD in 0.33–0.39 mol/L HNO₃ allows for selective Am(III) back-extraction into the aqueous phase while keeping Cm(III) and Ln(III) in the organic phase, marking PrOH-BPTD as an excellent complexant for an optimized AmSel process (Am(III) selective extraction).

更新日期：2022-10-23

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