Latest ArticlesSeparation and recovery of U(Ⅵ) and Th(Ⅳ) from rare earth minerals is a very challenging work in rare earth industrial production. In the present study, a homemade membrane emulsification circulation (MEC) extractor was used to separate U(Ⅵ) and Th(Ⅳ) from rare earth elements by using Cyphos IL 104 as an extractant. Batch experiments were carried out using a constant temperature oscillator to investigate the extraction parameters of the single element and the results indicated that Cyphos IL 104 could reach the extraction equilibrium within 30 min for all the three elements, i.e., U(Ⅵ), Th(Ⅳ), and Eu(Ⅲ). Besides, the MEC extractor possessed a strong phase separation ability. The extraction efficiencies of U(Ⅵ), Th(Ⅳ), La(Ⅲ), Eu(Ⅲ) and Yb (Ⅲ) increased with the increase of pH. La(Ⅲ), Eu(Ⅲ) and Yb(Ⅲ) were hardly extracted when pH ≤ 1.50, which was beneficial for effectively separating U(Ⅵ) and Th(Ⅳ) from La(Ⅲ), Eu(Ⅲ) and Yb(Ⅲ). In the multi-stages stripping experiments, when the stripping stage number was 3, the effective separation could be achieved by using HCl and H2SO4, since the stripping efficiency reached 80.0% and 100.0% for Th(Ⅳ) and U(Ⅵ), respectively. Slope method and FT-IR spectra showed that Cyphos IL 104 reacted with U(Ⅵ) and Th(Ⅳ) by chelation mechanism. The extraction of multi-elements indicated that U(Ⅵ) and Th(Ⅳ) could be well separated from the solution which contains all rare earth elements, and the extraction efficiencies of U(Ⅵ) and Th(Ⅳ) both were close to 100.0%. Based on the above experimental results, a flowchart for efficient separation of U(Ⅵ) and Th(Ⅳ) from rare earth elements was proposed.
Separation of the minor actinides (Am and Cm) from lanthanides in high-level liquid wastes (HLLW) is one of the most challenging chemical separation tasks known owing to their chemical similarities and is highly significant in nuclear fuel reprocessing plants because it could practically lead to sustainable nuclear energy by closing the nuclear fuel cycle. The solid phase extraction is proposed to be a possible strategy but all reported sorbent materials severely suffer from limited stability and/or efficiency caused by the harsh conditions of high acidity coupled with intense irradiation. Herein, a phenanthroline-based polymeric organic framework (PhenTAPB-POF) was designed and tested for the separation of trivalent americium from lanthanides for the first time. Due to its fully conjugated structure, PhenTAPB-POF exhibits previously unachieved stability under the combined extreme conditions of strong acids and high irradiation field. The americium partitioning experiment indicates that PhenTAPB-POF possesses an ultrahigh adsorption selectivity towards Am(Ⅲ) over lanthanides (e.g., SFAm(Ⅲ)/Eu(Ⅲ) = 3326) in highly acidic simulated HLLW and relatively fast adsorption kinetics in both static and dynamic experiments. Am(Ⅲ) can be almost quantitatively eluted from the PhenTAPB-POF packed-column using a concentrated nitric acid elution. The high stability and superior separation performance endow PhenTAPB-POF with the promising alternative for separating minor actinides over lanthanides from highly acidic HLLW streams.
The in vivo degradation behavior of metallic nanoparticles (NPs) is very important for their biomedical applications and safety evaluation. Here, a method of laser ablation-single particle inductively coupled plasma mass spectrometry (LA-sp-ICP-MS) is shown to have high spatial resolution, sensitivity and accuracy for simultaneous imaging the in situ distribution of particulate Ag (P-Ag) and released ionic Ag (Ion-Ag) in the sub-organs of spleen, liver and kidney after intravenous injection of Ag nanoparticles (50 nm, AgNPs) to mice. Under the optimized parameters of 0.4 J/cm2 laser fluence on a 30 µm spot with dwell time at 100 µs, the signals of P-Ag and Ion-Ag in the organic tissues can be easily distinguished from the mass spectra. The method of iterative threshold algorithm has been used to distract the signals of P-Ag and Ion-Ag and separate each other. The resulting images for the first time provide visualized evidence that a considerable amount of P-Ag accumulated in the splenic marginal zone, but widely distributed in the liver parenchyma at 24 h after injection of AgNPs, and in the meantime, obvious amounts of ionic Ag released and distributed in the organs. In addition, the imaging results indicate that the AgNP excretion in the kidney is mainly in ionic forms. The investigation here demonstrates that the developed LA-sp-ICP-MS method with high spatial resolution, sensitivity and visualization capability can become a powerful tool in the clinical context of metallic NPs.
Due to the rigid Si-O-Si backbone, silicone rubber (SR) have a widespread application in extreme environment such as high temperature and high-level radiation. However, the radiation stability of SR still does not meet the practical needs in special radiation environments. Herein we prepared epoxy POSS(ePOSS)/SR nanocomposites with excellent thermal stability and radiation resistance. As a physical crosslinking point in the SR, addition of small amount of ePOSS not only enhanced the mechanical properties of the matrix, but also improved its thermal stability greatly due to their good compatibility. ePOSS/SR had higher radiation stability in air than SR owing to the inhibition of radiation oxidation by ePOSS, and the yield of main gaseous radiolysis products (CH4, H2, CO and CO2) of SR and ePOSS/SR nanocomposites was determined. By analyzing the changes of chemical structure, thermal properties and mechanical properties of the ePOSS/SR nanocomposite, combined with the characteristics of gas products after γ-irradiation, the radiation induced crosslinking and degradation mechanism of the nanocomposites was proposed comprehensively.
Thioredoxin reductase 1 (TrxR1) is over activity in tumor cell to maintain their redox balance. Although gold clusters have great potential in antitumor drug as they could well inhibit TrxR1, the molecular mechanism has not been disclosed yet. In this work, we revealed gold clusters can well inhibit the activity of TrxR1 in lung tumor cells and further disclosed the inhibition mechanism by using computational simulation methods. We firstly inferred the binding sites of gold in the hydrophobic cavities on TrxR1. The simulation results show that the gold ion (released from Au cluster) interact with –SH of Cys189 in TrxR1, this greatly increase the distance between the C-terminal redox center of TrxR1 and the Trx redox center, thereby destroy the electron transfer pathway between them. Our electron transfer destroying mechanism is different from the previous hypothesis that gold binds to the Sec498 of TrxR1 which has never been proved by experimental and theory studies. This work provides a new understanding of the gold clusters to inhibit TrxR1 activity.
The prevalence of positron emission tomography (PET) imaging has advanced biomedical applications for its ultrahigh sensitivity, deep tissue penetration and quantitative visualization of diseases in vivo. 64Cu with ideal half-life and decay characteristics has been designed as radioactive probes for disease diagnosis. The currently reported 64Cu-labeled nanomaterials have the advantages of long circulation time in serum, good biocompatibility and mature preparation methods, and have been used in vivo PET imaging, biodistribution and pharmacokinetic monitoring, and imaging guided therapy. At the same time, suitable carrier characteristics and radiolabeling strategies are particularly important in the 64Cu PET imaging process. In this review, we summarize different imaging probe designs and 64Cu radiolabeling strategies, as well as their eventual applications in biomedicine. The potential challenges and prospects of 64Cu labeled nanomaterials are also described, which provides broad prospects for radiolabeling strategies and further applications.
During the chemical weathering of the uranium mill tailings, released uranium could be immobilized by the newly formed secondary minerals such as oxyhydroxides. A deeper understanding of the interaction between uranium and common oxyhydroxides under environmental conditions is necessary. In this work, uranium sorption behaviors on Al-, Mn- and Fe-oxyhydroxide minerals (boehmite, manganite, goethite, and lepidocrocite) were investigated by batch experiments. Results showed that the uranium sorption on Al-oxyhydroxide behaved significantly differently from the other three minerals. The sorption edge of the Mn- and Fe-oxyhydroxides located around pH 5, while the sorption edge of boehmite shifted about 1.5 pH unit to near neutral. The sorption isotherms of uranium on manganite, goethite and lepidocrocite at pH 5.0 could be well fitted by the Langmuir model. Instead of surface complexation, sorption on boehmite happened mainly by uranium-bearing carbonates and hydroxides precipitation as illustrated by the characterization results. Both carbonate and phosphate strongly affected the uranium sorption behavior. The removal efficiency of uranium by boehmite exceeded 98% after three sorption-desorption cycles, indicating it may be a potential material for uranium removal and recovery.
The hunt for agents that are suitable for actinide decorporation to reduce the whole-body load of actinide in accidental internal exposure is the ever-lasting goal in radiation protection and medical treatment in nuclear emergency. All current decorporation agents can be categorized as two groups, one is the molecular ligands, and the other is the nanoparticles decorated with molecular ligands. Here in this work, functional nanodiamonds (fNDs) with ssDNA (the endogenous biomacromolecule rich in phosphate groups) loaded on the NDs is reported, which poses good uranyl adsorption selectivity, high cellular uptake, fast excretion, and effective decorporation of uranyl from rat renal proximal tubular epithelial cells (NRK-52E). All those results corroborate that fNDs can potentially serve as a brand new family of chelators for actinide decorporation.
Phototheranostics have attracted tremendous attention in cancer diagnosis and treatment because of the noninvasiveness and promising effectiveness. Developing advanced phototheranostic agents with long emission wavelength, excellent biocompatibility, great tumor-targeting capability, and efficient therapeutic effect is highly desirable. However, the mutual constraint between imaging and therapeutic functions usually hinders their wide applications in biomedical field. To balance this contradiction, we herein rationally designed and synthesized three novel tumor-targeted NIR-II probes (QR-2PEG321, QR-2PEG1000, and QR-2PEG5000) by conjugating three different chain lengths of PEG onto an integrin αvβ3-targeted NIR-II heptamethine cyanine fluorophore, respectively. In virtue of the essential amphiphilic characteristics of PEG polymers, these probes display various degree of aggregation in aqueous buffer accompanying with differential NIR-II imaging and photothermal (PTT) therapeutic performance. Both in vitro and in vivo results have demonstrated that probe QR-2PEG5000 has the best NIR-II imaging performance with prominent renal clearance, whereas QR-2PEG321 possesses excellent photoacoustic signal as well as PTT effect, which undoubtedly provides a promising toolbox for tumor diagnosis and therapy. We thus envision that these synthesized probes have great potential to be explored as a toolkit for precise diagnosis and treatment of malignant tumors.
Exploring efficient materials for capturing radioactive iodine in nuclear waste is of great significance for the progress of nuclear energy as well as the protection of ecological environment. Covalent organic frameworks (COFs) have emerged as promising adsorbents because of their predesignable and functionalizable skeleton structures. However, it remains a grand challenge to achieve large scale preparation of COFs. In this work, we developed a mild and efficient microwave irradiation method instead of the traditional solvothermal method to prepare copper phthalocyanine-based covalent organic frameworks (CuPc-COFs) within only 15 min. The nitrogen-rich 1, 2, 4, 5-tetracarbonitrilebenzene (TCNB) was selected as the solely organic ligand to construct copper phthalocyanine-based 2D conjugated COFs. The resultant CuPc-COFs exhibited excellent iodine enrichment with 2.99 g/g for volatile iodine and 492.27 mg/g for iodine-cyclohexane solution, respectively, outperforming that of many porous materials. As indicated by spectroscopic analysis and DFT calculations, this impressive adsorption performance can be attributed to the charge transfer arising from nitrogen-rich phthalocyanine structures and electron-rich π-conjugated systems with iodine molecules. Moreover, the strong electrostatic interaction between Cu(II) on chelate centers and polyiodide anions (Ix-) also play an important role in the firmly trapping radioactive iodine. Therefore, this study provides a facile and intelligent approach to implement metal-based COFs for the remediation of toxic radioactive iodine.
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