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Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate
Solvent Extraction and Ion Exchange ( IF 2 ) Pub Date : 2020-01-20 , DOI: 10.1080/07366299.2019.1710918
Peter Zsabka 1, 2 , Karen Van Hecke 1 , Andreas Wilden 3 , Giuseppe Modolo 3 , Michelle Hupert 4 , Vincent Jespers 5 , Stefan Voorspoels 5 , Marc Verwerft 1 , Koen Binnemans 2 , Thomas Cardinaels 1, 2
Affiliation  

Radiolytic stability of the extractants N,N,N’,N’-tetraoctyl diglycolamide (TODGA) and 2,9-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-1,2,4-benzotriazin-3-yl)-1,10-phenanthroline (CyMe4BTPhen) in the ionic liquid tri-n-octylmethylammonium nitrate ([N1888][NO3]) was studied via the combination of a steady-state irradiation by cobalt-60 gamma-radiation, followed by solvent extraction and identification of radiolysis products by High-Performance Liquid Chromatography coupled to Electro Spray Ionisation Mass Spectrometry (HPLC-ESI-MS). The observed trend for the distribution ratios of trivalent minor actinides and Eu(III) showed a decrease as a function of absorbed dose in the case of the TODGA solvent. The gamma irradiations were conducted in the presence or absence of an acidic aqueous phase. The determined dose constants for TODGA under neutral or acidic conditions were up to four times lower than the values reported in aliphatic diluents under comparable conditions. The degradation patterns were similar to those found by former studies on TODGA diluted in n-dodecane; only de-alkylation and bond ruptures within the diglycolamide core were observed. The presence of an acidic aqueous phase during irradiation resulted in a different relative abundance of certain radiolysis products of both the diluent and TODGA and a higher dose constant compared to the neutral irradiation conditions. A quantification of CyMe4BTPhen in irradiated samples with the [N1888][NO3] diluent was not possible, but the effect on its extraction properties was evaluated. The distribution ratios slightly increased under the effect of absorbed dose, indicating the formation of radiolysis products that are efficient extractants as well.



中文翻译:

离子液体硝酸三正辛基甲基铵中TODGA和CyMe4BTPhen的γ辐解

萃取剂N,N,N',N'-四辛基二甘醇酰胺(TODGA)和2,9-双(5,5,8,8-四甲基-5,6,7,8-四氢-1,2)的辐射稳定性,4-苯并三嗪-3-基)-1,10菲咯啉(CYME 4在离子液体三BTPhen)ñ -octylmethylammonium硝酸盐([N 1888 ] [NO 3])的研究方法是结合使用钴60γ射线进行稳态辐照,然后通过高效液相色谱-电喷雾电离质谱联用(HPLC-ESI-MS)进行溶剂萃取和放射性分解产物的鉴定。在TODGA溶剂的情况下,观察到的三价次act系元素和Eu(III)分布比的趋势随吸收剂量的变化而降低。在有或没有酸性水相的情况下进行γ辐射。在中性或酸性条件下,TODGA的确定剂量常数比在类似条件下脂族稀释剂中报道的值低四倍。降解模式与以前在TODGA中稀释n的研究发现的降解模式相似。-十二烷; 仅观察到二甘醇酰胺核心内的脱烷基化和键断裂。与中性辐照条件相比,辐照过程中酸性水相的存在导致稀释剂和TODGA的某些放射分解产物的相对相对丰度不同,并且剂量常数更高。不可能用[N 1888 ] [NO 3 ]稀释剂对照射样品中的CyMe 4 BTPhen进行定量,但是评估了对其提取性能的影响。在吸收剂量的作用下,分配比略有增加,表明也形成了有效的萃取剂的放射分解产物。

更新日期:2020-04-20
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