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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

2-Carboxamido-6-(1H-pyrazol-3-yl)-pyridines as ligands for efficient separation of americium(III) from europium(III)

Lianjun Song,Xueyu Wang,Dongqi Wang,Qian Xiao,Haowei Xu,Qiuju Li,Lanlan He,Songdong Ding

The synthesis, Eu 3+ complexation, and selective solvent extraction of Am 3+ over Eu 3+ in nitric acid solution by 2-carboxamido-6-(1 H -pyrazol-3-yl)-pyridines (A-PzPy) ligands were described. Without the aid of any lipophilic anion source, A-PzPy ligands in methyl isobutyl ketone (MIBK) diluent demonstrated a more favorable affinity of Am 3+ than Eu 3+ at high acidity levels. Slope analysis showed the formation of 1:2 metal/ligand extracted species. The extraction was a spontaneous exothermic process. The analyses of fluorescence titration, Fourier transform infrared (FT-IR), Raman, time-resolved laser fluorescence spectrum (TRLFS), electrospray ionization mass spectrometry (ESI-MS), conductivity and microcalorimetric titration revealed that the composition of complex is [Eu(NO 3 ) 2 (H 2 O)∙2(Et- p -Tol-A-PzPy)](NO 3 ). Combining the results of solvent extraction and complexation study, the extraction mechanism was proposed. Furthermore, the stability constants (log β ) and thermodynamic parameters (Δ H , Δ S , Δ G ) for complexation of Eu 3+ with Et- p -Tol-A-PzPy were also presented.

研究领域: 化学 · 核化学 · 环境科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2021 ·Vol. 328 ·期 1 ·137-147 · IF 1.371

Rapid method for sequential determination of Pu and Am in soil and sediment samples by sector-field inductively coupled plasma mass spectrometry

Wang Zhongtang,Xie Yun,Lin Jinxian,Li Zejun,Tan Zhaoyi

New method was developed to analyze Pu and Am sequentially for soil and sediment by inductively coupled plasma mass spectrometry (ICPMS). The developed method uses conc. HNO 3 to leach Pu and Am, Fe(OH) 3 coprecipitation to remove alkali and alkaline metals, extraction chromatographic separation using UTEVA, DGA and TEVA resins to remove interfering elements (IEs) and separate Pu and Am from each other, and sector field-ICPMS to measure Pu and Am. The analysis of four standard reference materials showed that both Pu isotopes and 241 Am were accurately determined by this method, as a result of its excellent decontamination ability of IEs. Especially the high decontamination factor of Pu [DF(Pu), 4.2 × 10 2 ] in Am fraction and high DF(Am) (7.0 × 10 3 ) in Pu fraction sufficiently eliminated the cross interference between 241 Pu and 241 Am in ICPMS measurement. In addition, stable and high chemical recoveries were achieved for Pu (71–91%) and Am (70–88%). The low LODs of Pu isotopes, short analytical time (14 h) and high DFs of IEs allows this method to sequentially analyze Pu and Am, for both global fallout and nuclear accident sourced samples.

研究领域: 环境科学 · 分析化学
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ACS Omega · 2021 · IF 3.512

Complexation and Separation of Trivalent Actinides and Lanthanides by a Novel DGA Derived from Macrocyclic Crown Ether: Synthesis, Extraction, and Spectroscopic and Density Functional Theory Studies

Yu Fan,Youzhen Li,Xi Shu,Rulei Wu,Shanyong Chen,Yongdong Jin,Chao Xu,Jing Chen,Chao Huang,Chuanqin Xia

A DGA-arm-grafted macrocyclic aza-crown ether ligand (Cr6DGA) was synthesized, and its solvent extraction behavior toward trivalent americium and europium in nitric acid medium was studied. The effects of various parameters such as the contact time, temperature, concentration of the extractant, and acidity on the extraction by Cr6DGA were investigated. It was found that in 3 mol/L HNO3, the SFEu/Am value was about 2. The complexation energies calculated by DFT showed that the Eu(III) complexes were more stable than the corresponding Am(III) complexes in gas, aqueous, and organic phases. Furthermore, the coordination study showed that the metal/ligand ratio of the extracted species was 1:2 by mass spectrometry (MS) analysis. The time-resolved laser-induced fluorescence spectra (TRLFS) further proved that the extracted species contained one water molecule, and so the composition of the extracted complexes may be [EuL2NO3(H2O)]2+ or [EuL2(NO3)2(H2O)]+. Finally, DFT calculations revealed that [EuL2(NO3)2(H2O)]+ is a more stable species and the binding energy of Eu(III) with the DGA unit is lower than that with the crown unit.

研究领域: 化学 · 核化学与放射化学
✓ 已验证 DOI PubMed 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Diglycolamide with long C-chains combined with ether bonds for high loading of Am(III) and Eu(III): Extraction, aggregation, and third-phase formation studies

Xiaoyang Hu,Haowei Xu,Zhuang Wang,Qiao Yu,Xuanhao Huang,Xingyue Liu,Qiang Tian,Songdong Ding

Diglycolamide (DGA) extractants, especially TODGA ( N , N , N′ , N′ ‐tetraoctyl diglycolamide), show significant potential in high-level liquid waste treatment. However, their limited loading capacity for trivalent lanthanides (Lns) and actinides (Ans) often leads to detrimental emulsification or third phase formation, hindering their practical applicability. Herein, TOOEDGA ( N , N , N’ , N’ -tetra(2-(octyloxy)ethyl)diglycolamide), a new DGA extractant with long C-chains combined with ether bonds, exhibits superior extraction performance towards Am 3+ and Eu 3+ in HNO 3 solution compared to TODGA. The factors influencing the formation of a third phase during the extraction process were investigated. It has been shown that TOOEDGA has a greater loading capacity for Lns 3+ and can tolerate a wider concentration range of HNO 3 . Additionally, the aggregation behavior of DGAs in n -dodecane was also studied using dynamic light scattering and small-angle X-ray scattering, revealing that the reverse micelles formed by TOOEDGA are more stable than those formed by TODGA. Moreover, under similar conditions, TOOEDGA molecules do not aggregate further to generate rod-like reverse micelle aggregates like those observed with TODGA, which is beneficial to inhibit the formation of the third phase. Consequently, our results suggest that TOOEDGA holds great promise as an alternative DGA extractant for practical industrial applications.

CAS / MDL: 13746-96-8 10361-93-0
研究领域: 化学 · 核化学与放射化学 · 环境科学
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CERAMICS INTERNATIONAL · 2025 ·Vol. 51 ·期 27 ·54471-54479 · IF 5.6

Sintering optimization and microscopic alteration mechanism of americium oxide analogues for space energy power

He Chen,Lina Lv,Xiaoyu Li,Tingting Deng,Hao peng,Weicheng Xiang,Fangting Chi

Radioisotope thermoelectric generators (RTGs) produce electrical energy exclusively through the natural decay of radioactive materials, rendering them an ideal power source for space missions and other extreme environments. 241 Am is viewed as a promising substitute for 238 Pu as the heat-generating nuclide in these applications. However, there is currently no consensus on the sintering of 241 Am (Ⅲ) pellets. In this research, Nd (Ⅲ) oxide was used as a surrogate for americium (Ⅲ) oxide, and conventional cold-press-and-sinter methods were employed. Through a systematic investigation of the heating rate, holding time, and maximum temperature during the sintering of Nd (Ⅲ) oxide pellets made from commercial materials, an optimized sintering thermal cycle was developed. This curve enhances sintering efficiency and results in pellets with an open pore network, which is crucial for helium gas release. This work is significant in advancing the research and development of 241 Am nuclear batteries.

CAS / MDL: 1313-97-9
研究领域: 核化学 · 材料科学 · 能源工程 · 空间电源技术 · 固态离子学 · 放射化学
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JOURNAL OF ENVIRONMENTAL RADIOACTIVITY · 2018 · IF 2.263

Sequential analyses of actinides in large-size soil and sediment samples with total sample dissolution

Maoyi Luo,Shan Xing,Yonggang Yang,Lijuan Song,Yan Ma,Yadong Wang,Xiongxin Dai,Steffen Happel

There is a growing demand for the determination of actinides in soil and sediment samples for environmental monitoring and tracing, radiological protection, and nuclear forensic reasons. A total sample dissolution method based on lithium metaborate fusion, followed by sequential column chromatography separation, was developed for simultaneous determination of Pu, Am and Cm isotopes in large-size environmental samples by alpha spectrometry and mass spectrometric techniques. The overall recoveries of both Pu and Am for the entire procedure were higher than 70% for large-size soil samples. The method was validated using 20 g of soil samples spiked with known amounts of 239 Pu and 241 Am as well as the certified reference materials IAEA-384 (Fangataufa Lagoon sediment) and IAEA-385 (Irish Sea sediment). All the measured results agreed very well with the expected values.

研究领域: 环境科学 · 核化学 · 分析化学
✓ 已验证 DOI PubMed 高影响因子
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