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PROGRESS IN NUCLEAR ENERGY · 2015 · IF 1.119

Adsorption and immobilization of actinides using novel SiO2–ZrO2-calcium alginate aerogels from high level liquid waste

Junchuan Zhao,Xingeng Ding,Cheng Meng,Chunrong Ren,Huiqin Fu,Hui Yang

The novel SiO 2 –ZrO 2 -calcium alginate aerogels were prepared by Sol–Gel process with phase separation method for investigating the adsorption and immobilization performance of the plutonium and minor actinides from high-level liquid waste (HLLW). The materials contained porous network structure with high surface area (233.44–481.08 m 2 /g) and pore volume (0.50–1.26 m 3 /g). The aerogels were superior adsorbents for the removal of plutonium and minor actinides, the maximum adsorption capacity and adsorption rate (35 °C, 75 rpm) reached 231.5 mg/g and 99.2%. For all the waste forms, SiO 2 , ZrO 2 and Ca 2 SiO 4 phases were simultaneously observed in the matrix. Moreover, Ce entered into Ca sites of Ca 2 SiO 4 and Zr sites of ZrO 2 . The substitution of Ca and Zr by Ce in the Ca 2 SiO 4 and ZrO 2 implies a promising disposal measure of actinides.

CAS / MDL: 25322-68-3 7699-43-6
研究领域: 材料科学 · 核化学与放射化学 · 环境科学
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RSC Advances · 2012 ·Vol. 3 ·期 5 ·1572-1582 · IF 0

Bisactinyl halogenated complexes: relativistic density functional theory calculation and experimental synthesis

Qing-Jiang Pan,Yong-Ming Wang,Run-Xue Wang,Hong-Yue Wu,Weiting Yang,Zhong-Ming Sun,Hong-Xing Zhang

Relativistic density functional theory was used to explore a series of bisactinyl complexes, [(phen)(AnVIO2)(μ2-F)(F)]2 (An = U (1), Np (2) and Pu (3); phen = phenanthroline; μ2 = doubly bridged), [(phen)(UVO2)(μ2-F)(F)]22− (4), [(phen)(UVIO2)(μ2-X)(X)]2 (X = Cl (5), Br (6) and I (7)), [(L)(UVIO2)(μ2-F)(F)]2 (L = bpy (8), 2NH3 (9) and 2F (10); bpy = 2,2′-bipyridine) and [NH4]4[(F)2(UVIO2)(μ2-F)(F)]2 (11). The effects of varying actinyl ions (UO22+, NpO22+ and PuO22+), oxidation states of uranium (VI and V) and equatorial ligands (phen → bpy → 2NH3 → 2F and F → Cl → Br → I) on the structures and electronic properties of complexes were examined. The calculated distances and bond orders of AnO indicate the partial triple bonding character, and agree with the trends in the AnO stretching vibrational frequencies. The free energies of formation reactions of 1–11 calculated in the aqueous solution demonstrate that 1, 8 and 11 are thermodynamically stable. In this work, we have successfully synthesized 1 and [Me2NH2]4[(F)2(UVIO2)(μ2-F)(F)]2 (12), which is represented by theoretical model complex 11. Their characterizations of the single crystal X-ray diffraction and infrared are consistent with the calculated results; the measured fine-structured fluorescent emissions were assigned as transitions from the UO bonding to the U (f) orbital by analyzing the electronic structure and absorption spectra.

CAS / MDL: 68-12-2
研究领域: 化学 · 材料科学 · 理论计算
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS · 2025 · IF 4.6

Speed and precision: unveiling an ICP-MS method for ultra-trace 239Pu quantification in food

Yinjie Zou,Hong Ren,Lei Zhou,Peng Wang,Yiyao Cao

A rapid, accurate, and sensitive inductively coupled plasma mass spectrometry (ICP-MS) method has been developed and validated for the determination of ultra-trace levels of Plutonium-239 ( 239 Pu) in food. After ashing, samples were digested with lefort aqua regia and treated with FeCl 3 to mask phosphorus (P) interference, thereby preventing it from inhibiting the adsorption of Pu by the resin column. Subsequently, a two-stage TK200 resin column was employed for separation and purification, followed by ICP-MS analysis using kinetic energy discrimination (KED) mode. By combining a chromatographic column with ICP-MS, this method achieved an overall decontamination factor (DF) of 3.53×10 12 for uranium hydride ions ( 238 UH + ) and demonstrated excellent linearity within the given concentration range, with a correlation coefficient ( r ) exceeding 0.999. The limit of detection (LOD) was 3.6 fg/g (ash), with an average recovery of over 74% and a relative standard deviation below 6.6%. Furthermore, the proposed method's applicability was evaluated by quantifying 239 Pu in food. The results indicate that this method is rapid, accurate, and sensitive, making it ideal for 239 Pu detection.

研究领域: 分析化学 · 核化学 · 食品安全 · 环境监测 · 放射性同位素检测 · 质谱学
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

Selective coordination behaviors of Uranium(VI) with novel asymmetrical tetra-alkylcarbamides

Qi Chen,Baole Li,Junli Wang,Haowei Zhu,Xiwen Chen,Yifu Hu,Jia Zhou,Wentao Wang,Weifang Zheng,Taihong Yan

In this work, the solvent extraction and complexation behaviors of U(VI) by two novel asymmetrical tetra-alkylcarbamides, N,N’-butyl-N,N’-hexylurea ( L1 : SBHU ) and N,N’-butyl-N,N’-pentylurea ( L2 : SBPU ) in HNO 3 media were systematically investigated. Both two ligands extract U(VI) more effectively than other metals such as Pu(IV), Np(IV), and Th(IV) in a wide range of acidity. Under 5 mol/L HNO 3 , D U reached 5.25, while D Pu  = 1.08, D Np  = 0.11, D Th  = 0.13.. Additionally, no third-phase was present by the extraction of highly uranium concentration solution with SBHU even under 7 mol/L HNO 3 after four cycles demonstrating good acid resistance and resistance to the formation of the third phase. Slope analyses and FT-IR indicate that the U(VI) complexes are a form of UO 2 (NO 3 ) 2 ·2 L for the two ligands during the extraction. Additionally, based on the DFT calculations, the NBO analysis, and topological analysis were analyzed in detail. The results demonstrate that the interactions between ligands and U(VI) are shown mainly as ionic characteristics, and the ligand-to-metal charge transfer was also observed. This study enriches the coordination chemistry of actinides: Th(IV), U(VI), Np(IV), Am(III), and Pu(IV) by tetra-alkylcarbamides, which may shed light on the design and synthesis of novel U(VI) selective ligands.

研究领域: 配位化学 · 锕系元素化学 · 溶剂萃取 · 理论化学
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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
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