JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2024
·Vol. 333
·期 3
·1357-1365
·
IF 1.5
Mei Lingzi,Shao Hui,Cui Lingzhi,Yang Jinmin,Zhang Lei
A novel method for rapid radioanalytical measurement of uranium and plutonium in 100ml emergency urine samples was developed, through optimized selection of the separation and purification process and a combined measurement with ICP-TOF-MS and alpha spectrometry. The typical analytical time is within 6 h, the recovery rates are more than 80%, and the minimum detection activity concentrations are 3.4 × 10 −4 Bq/L for 238 U and 2.5 × 10 −3 Bq/L for 239 Pu respectively. The spiked test shows that this method can be used for quantitative evaluation of the activity concentration of 238 U and 239 Pu in urine samples accurately.
研究领域:
放射化学
·
环境科学
·
医学检测
✓ 已验证
DOI
高影响因子
ACS Earth and Space Chemistry
·
2021
·
IF 3.475
Yang Wu,Xiongxin Dai,Marcus Christl,Hans-Arno Synal,Shan Xing,Shaochun Hou
Plutonium-244 could be the heaviest primordial nuclide existing on earth since the early formation of the solar system. However, the controversial results on the detection of 244Pu in bastnaesite samples require a reassessment. An extremely sensitive analytical method has been developed for the analysis of total 244Pu in completely digested bastnaesite samples by accelerator mass spectrometry. As no true signal of 244Pu was observed, an upper limit for the 244Pu content in the bastnaesite concentrate sample from the Bayan Obo rare-earth deposit (China) was estimated to be 5.4 × 10–19 g/g at 99% confidence level. This result does not agree with the detection of 244Pu at a concentration of 1.0 × 10–18 g/g in bastnaesite reported by Hoffman et al. [Nature1971,234, 132–134] but confirms the latest measurement for an upper limit of 1.5 × 10–19 g 244Pu/g bastnaesite by Lachner et al. [Phys. Rev. C: Nucl. Phys.2012,85, 015801]. Thus, the direct search for primordial 244Pu on earth still remains an open question.
研究领域:
地球化学
·
核物理学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2014
·Vol. 21
·期 11
·7219-7226
·
IF 2.757
Xie Jinchuan,Lin Jianfeng,Zhou Xiaohua,Li Mei,Zhou Guoqing
Low-solubility contaminants with high affinity for colloid surfaces may form colloid-associated species. The mobile characteristics of this species are, however, ignored by the traditional sorption/distribution experiments in which colloidal species contributed to the immobile fraction of the contaminants retained on the solids as a result of centrifugation or ultrafiltration procedures. The mobility of the contaminants in subsurface environments might be underestimated accordingly. Our results show that colloidal species of 239 Pu in three-phase systems remained the highest percentages in comparison to both the dissolved species and the immobile species retained on the granite grains (solid phase), although the relative fraction of these three species depended on the colloid types. The real solid/liquid distribution coefficients ( K
s/d ) experimentally determined were generally smaller than the traditional K
s/d (i.e., the K
s+c/d in this study) by ~1,000 mL/g for the three-phase systems with the mineral colloids (granite particle, soil colloid, or kaolinite colloid). For the humic acid system, the traditional K
s/d was 140 mL/g, whereas the real K
s/d was approximately zero. The deviations from the real solid/liquid K
s/d were caused by the artificially increased immobile fraction of Pu. One has to be cautious in using K
s/d -based transport models to predict the fate and transport of Pu in the environment.
研究领域:
环境科学
·
放射生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Yangchun Leng,Qintang Li,Qiang Tian,Xiaoyuan Chen,László Almásy,Yuliang Liu,Guangai Sun,Xianguo Tuo,Minhao Yan,Mark J. Henderson
The ability of bentonite and montmorillonite pillared by Al-oxide and mixed (Ln-Al)-oxides (Ln = La, Ce) to remove 239 plutonium solution species from water is comparatively investigated at pH 7 and pH 4. Small-angle scattering and neutron contrast variation with H 2 O/D 2 O mixtures is used to verify the ingress of water in the calcined products after hydrophilicity was introduced by an NH 3 -H 2 O vapor treatment. The size and shape of the (La/Ce)-Al oxo-hydroxy pillaring cations (2 nm spheres) is determined by small-angle x-ray scattering from the pillaring solutions. Not all of the oxide pillars improved Pu uptake compared with sodium montmorillonite. At neutral and acidic pH only (Ce-Al)-oxide pillared clays showed the ability to remove Pu over the concentration range studied (1.35 × 10 −8 –8 × 10 −8 mol dm −3 ) with distribution coefficient ( K D ) values >10 4 . XPS analysis of the (Ce-Al)-oxide pillared clays indicates the presence of Ce 4+ as cerium dioxide. The progressive improvement in sorption performance in the order of pillar type Al 2 O 3 < La 2 O 3 -Al 2 O 3 << CeO 2 -Al 2 O 3 reflects the increasing access of Pu solution species to the clay mineral layers by changes to the basal spacing and specific surface area, and also to the higher stability of the (Ce-Al)-oxide pillars.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2021
·Vol. 328
·期 1
·137-147
·
IF 1.371
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
✓ 已验证
DOI
高影响因子
Separations
·
2025
·Vol. 12
·期 5
·106
·
IF 2.7
Xiaoyun Guo,Junli Wang,Yao Liu,Haojun Zhao,Hui Wang,Wentao Wang,Baole Li,Taihong Yan
Developing a new efficient separation ligand based on the “CHON” principle to address the limitations of phosphorus containing extractants in nuclear fuel reprocessing can help further simplify the process flow and reduce the amount of secondary waste. Building upon this critical need, a novel ligand was developed through a strategic application of the Hard and Soft Acids and Bases (HSAB) theory, integrating a soft donor nitrogen atom into the linear architecture of bis-diglycolamide. This groundbreaking ligand, named N,N′-bis[2-(2-(N,N-dioctylcarbamoyl)ethoxy)ethylacetamido]-N″-diethylenetriamine (TOMDEA-BisDGA), has demonstrated remarkable potential in the extraction of Pu(IV). The study unveils that the ligand demonstrates remarkable selectivity and separation efficiency towards Pu(IV) ions while maintaining an exceptionally low extraction capacity for U(VI) across a wide acidity spectrum of 0.1~6 mol/L. To explain the structure properties of complex formed by the ligand and Pu(IV), a systematic analysis was performed, including slope analysis, proton nuclear magnetic resonance (NMR) titration, and Fourier-transform infrared (FT-IR) spectroscopy. This study explores the coordination and separation behavior of diglycolamide ligands with actinide. This work is expected to provide important information and theoretical bases upon which advanced design and optimization of ligands for high-performance processes for the separation of plutonium might be carried out. Such findings will contribute to the understanding of actinide chemistry and further the design of improved separation methods for nuclear applications.
研究领域:
核化学
·
配体设计
·
放射化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 4
·999-1005
·
IF 1.6
Luo Maoyi,Liu Daqian,Dai Xiongxin,Wu Yang,Yuan Ni
A simple and sensitive method was developed for 239, 240 Pu determination of sub-femtogram level in grass/vegetable sample using compact accelerator mass spectrometry (AMS). Pu was leached with HNO 3 -H 2 O 2 after ashing, and purified with AGMP-1 M resin column from grass matrix. After target preparation using mixed titanium/iron oxides, the final sample was measured by 300 kV AMS. The average recovery was higher than 80% for large-size (> 20 g ) grass sample in the entire procedure. 20 g environmental grass samples spiked with known amounts of 239 Pu standard solution or certified reference materials were measured for method evalution, good agreement between the expected values and measured results has been achieved. The detection limits were estimated to be 1.5 × 10 –16 g (0.34 µBq) for 239 Pu and 9 × 10 –17 g (0.8 µBq) for 240 Pu, demonstrating the feasibility of AMS for the determination of the sub-femtogram level of 239,240 Pu in environmental grass with global fallout signatures. Grass samples collected from China natural environment were successfully analyzed, and 239+240 Pu concentration down to 1.6 × 10 − 4 Bq/kg were measured in these samples. This improvement can stimulate environmental monitoring, ecological migration process and biological availability studies of Pu in the biosphere.
研究领域:
环境科学
·
核化学
·
分析化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL RADIOACTIVITY
·
2023
·
IF 2.3
Yao Yang,Maoyi Luo,Yang Wu,Ni Yuan,Jingjing He,Hongmei Guo,Quan an
A reliable and stable method was developed to accurately analyze neptunium ( 237 Np) and plutonium isotopes in environmental samples using 242 Pu or 236 Pu as a tracer. Key parameters, including the valence adjustment conditions and the stabilities of Pu and Np in the different resins, were investigated using TK200 and TEVA resin. It was found that Pu and Np could be efficiently extracted simultaneously using TK200 resin under the optimal loading conditions (6–12 M HNO 3 ) with the addition of 0.01–0.12 M NaNO 2 for valence adjustment. These isotopes were subsequently stripped out using a solution containing 0.1 M HCl , 0.05 M HF, and 0.01 M NH 2 OH·HCl. The separation efficiencies of Pu and Np were >93%, and the chemical yield ratio between Np and Pu was maintained steady at an average of 1.00 ± 0.03 (n > 50) under the optimal conditions. The analytical method was validated by analyzing environmental soil samples spiked with known amounts of 239 Pu and 237 Np standard solutions or certified reference materials. The measured values of 237 Np, 239 Pu, and 240 Pu obtained by inductively coupled plasma tandem mass spectrometry were consistent with their International Atomic Energy Agency literature values within a 95% confidence interval. These results confirm the reliability and high analytical precision (<6%) of this developed method using Pu as a non-isotopic tracer for monitoring the chemical yield of 237 Np. The developed method can also be used for environmental pollutant monitoring and for tracer studies of the 237 Np and Pu isotopes.
研究领域:
环境科学
·
核化学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Zhongtang Wang,Zhaoya Huang,Yun Xie,Zhaoyi Tan
Plutonium has been extensively studied in the environment, for the purpose of radiological assessment, environmental behavior study and nuclear emergency response. To determine Pu isotopes in environmental soil and sediment, a novel analytical method was established in this study using a new type of extraction resin, TK200 resin. Firstly an investigation was performed to study the extraction behaviors of Pu, U, Th, Hg, Tl, Pb, Bi and Hf on TK200 resin. On the basis of the results, a new chromatographic procedure was then proposed to separate Pu from the elements that interfere the accurate determination of Pu isotopes by mass spectrometry. Owing to the excellent separation efficiency between Pu and interfering elements (IEs) of the developed procedure, high decontamination factors (DFs) were obtained for IEs, e.g. the DF(U) (>7.5 × 10 7 ) was the highest reported value. The separation procedure was finally combined with HNO 3 leaching, CaF 2 /LaF 3 coprecipitation and sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) measurement to establish a complete method. The established method was evaluated by analyzing four standard reference materials (soil, sediment), and the results showed that both 239+240 Pu activity and 240 Pu/ 239 Pu isotopic ratio were accurately determined, with stable and high Pu chemical recoveries (81–91%). The whole analytical method only took about 15 h, and the limits of detection were calculated to be 0.13–0.24 fg g −1 for Pu isotopes (for 2 g soil or sediment), guaranteeing the rapid determination of ultra-trace level Pu in soil and sediment samples.
研究领域:
环境科学
·
核化学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2025
·
IF 1.6
Xin Futao,Luo Min,Li Chun,Ma Lingling,Xu Diandou,Xu Gang,Li Xi,Shao Yang
A rapid method has been developed for determining ultra-low level Pu isotopes in atmospheric particulate matter samples using SF-ICP-MS and TEVA resin. The Pu purification, ashing conditions and microwave digestion, were optimized to achieve high decontamination factor of U (4.1 × 10 4 ) and stably high Pu recovery (80–90%). The method detection limits were estimated to be 0.83 fg/g for 239 Pu and 0.70 fg/g for 240 Pu. Four IAEA certified reference materials were used for method evaluation. Finally, the method was successfully applied to determine the source of Pu in atmospheric particulate matter samples. The method can be performed within 16 h.
研究领域:
环境科学
·
核化学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2018
·Vol. 316
·期 1
·411-417
·
IF 1.181
Wang Zhongtang,Wen Wei,Quan Wei,Du Liang,Wang Ping,Lin Jinxian,Xie Yun,Tan Zhaoyi
Plutonium is one of the key radionuclides in nuclear decommission. In this study, a rapid method was developed to analyze Pu for concrete samples using total digestion, CaF 2 /LaF 3 coprecipitation, extraction chromatography using TEVA and DGA resins, and ICP-MS measurement. The whole analytical process can be achieved within 2 days, with sufficiently high decontamination factors of interfering elements and high Pu chemical recovery (57–93%). The high throughput (22 samples/2 days) and low LODs (0.008 mBq g −1 for 239 Pu and 0.02 mBq g −1 for 240 Pu) allow this method to effectively detect low level Pu contamination in concrete samples.
研究领域:
分析化学
·
核科学与技术
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Huidi Zhang,Shuai Wang,Jipan Yu,Zijie Li,Jianhui Lan,Lirong Zheng,Siyan Liu,Liyong Yuan,Taoyuan Xiu,Jindong Wang,Xinpeng Wang,Weiqun Shi
Uranium and plutonium are typical actinides tightly associated with nuclear fuel cycle. In this work we rationally design and fabricate a phosphonic group-decorated covalent organic framework, TzDa-Phos, for highly selective removal of uranium [U(VI)] and plutonium [Pu(IV)]. The saturation adsorption capacity for U(VI) can reach 394 mg/g at pH 4.0, and even maintains 40 mg/g in 1–4 M HNO 3 solutions. The distribution coefficient of Pu(IV) with TzDa-Phos is recorded up to 9.7 × 10 3 mL/g at 3 M HNO 3 . The excellent adsorption performance of TzDa-Phos for U(VI) and Pu(IV) is reasonably attributed to phosphonic groups decorated in TzDa. Specifically, the strong complexation of P O with uranium nitrate species (e.g., UO 2 (NO 3 ) + , UO 2 (NO 3 ) 2 0 ) is indicated at high acidities, in contrary to the coordination of P-O − with uranium at pH 4.0 as evidenced by FT-IR, XPS and EXAFS analyses. This work provides a promising adsorbent to recover uranium and plutonium from various wastewaters via a solid-phase extraction approach.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）