Latest ArticlesWith the rapid development of the nuclear industry, more-stringent requirements are proposed for high-level radioactive waste liquid treatment and the enrichment of isotope products. High-pressure ion exchange chromatography has been widely accepted for the fine separation of elements and nuclides due to its advantages, such as high efficiency, environmental friendliness, ease of operation, and feasibility for large-scale industrial applications. Here, we summarized the evolution of high-pressure ion exchange chromatography and the relevant research progress in ion exchange equilibrium and related separation technology. The prospects for application of high-pressure ion exchange chromatography to rare earth elements, actinide elements and isotope separation were discussed. High-pressure ion exchange chromatography represents a promising strategy for the extraction of rare earth elements and actinide elements from high-level radioactive waste liquid, as well as being an effective method for the automated production of high purity isotope products with great environmental benefits.
Hepatocellular carcinoma (HCC) is the most common primary malignant tumor of the liver, but early diagnosis and effective treatment are still difficult. With the development of radionuclide applications in medicine, nuclear medicine is playing an increasingly important role in the diagnosis and treatment of HCC. Radionuclide-based positron emission tomography-computed tomography and single-photon emission computed tomography-computed tomography molecular imaging are indispensable for assessing progression, staging, differentiation, preoperative planning, postoperative prediction, and evaluation of HCC in clinical applications. Moreover, radionuclide-based endoradiotherapy provides an objective therapeutic strategy for patients with unresectable advanced HCC. This review highlights the application and development of radionuclides in the diagnosis and treatment of HCC. More efforts are warranted for the development of advanced radionuclides to make significant contributions in the treatment of HCC.
A simple and convenient method has been developed for the pre-concentration and separation of inorganic selenium species from environmental water samples using anion exchange chromatographic column combined with high resolution inductively coupled plasma mass spectrometry (HR-ICP-MS) measurement. 75Se(Ⅳ) and 75Se(Ⅵ) were prepared and used as tracers during the experiments. The volatility of selenium during solution evaporation was investigated to establish a reliable water samples pretreatment procedure. The parameters which affect the uptake of Se(Ⅳ) and Se(Ⅵ) on Dowex1 × 8 resin was optimized and the procedure for Se(Ⅳ) and Se(Ⅵ) separation was proposed. Both Se(Ⅳ) and Se(Ⅵ) are retained on the column in natural or alkaline solution with high distribution coefficient. The successive gradient elution of pre-concentrated species of selenium with HNO3 solution allows to differentiate between them. Se(Ⅳ) and Se(Ⅵ) finally were eluted with 0.05 mol/L HNO3 and 5.0 mol/L HNO3, respectively. The proposed method has been successfully verified using the certified reference materials (CRMs) of real water samples, and spiked recoveries for real samples were 98%-104% with 5% relative standard deviations (RSDs). The developed procedure is proved to be reliable and can be used for the rapid determination of selenium species in environmental water samples.
The extraction complexes of uranyl(Ⅵ) in HNO3 to a hydroxyl-functionalized ionic liquid (IL) phase, HOEtmimNTf2 bearing CMPO, were investigated. Three possibly successive extraction complexes, UO2L2+ (L = CMPO), UO2L22+ and UO2L32+, were detected based on variable U/L ratios. Uranyl(Ⅵ) prefers to be extracted as complex UO2L32+, combining with the ions from HOEtmimNTf2 to construct a solid material through self-assembly. The thermodynamics of complexes, UO2L2+ (j = 1-3), were studied by spectrophotometry and microcalorimetry. All the formation reactions are principally driven by entropy, although a small part of the driving force of complexes UO2L22+ and UO2L32+ comes from enthalpy. Based on the thermodynamic properties for complex UO2L32+, we provide a possible coordination mode in HOEtmimNTf2: the first CMPO molecule coordinates with UO22+ in a bidentate fashion while the others do in a monodentate fashion. The results offer a thermodynamic insight into the formation behaviors of the uranyl(Ⅵ)/CMPO complexes involving the special IL HOEtmimNTf2, which is of significance to advance the novel IL extraction strategy.
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.
Astatine-211 (211At, t1/2 = 7.21 h) emitting two α particles with energies of 5.87 and 7.45 MeV, can lead to a high linear energy transfer (LET = 98.84 keV/µm) and short tissue range (50~90 µm). Since the 1950s, 211At had stepped into endoradiotherapy and has always been regarded as one of the most promising α-emitters for targeted-alpha therapy (TAT) in various malignancies. In the past two decades, 211At related radiopharmaceuticals have achieved great progress in the studies of basic physicochemical properties of astatine, 211At labeling strategies, preclinical and clinical studies, producing profound effects in nuclear medicine. This work will give a panorama of 211At-related researches in the recent 20 years, which will cover both the fundamental insights of 211At radiochemistry and applied labeling compounds. It can provide some important hints for the studies of TAT and other radiopharmaceuticals applied in tumor radiotherapy.
Based on the outstanding application advantages of nitrogen-rich materials with regular porous frameworks in the capture of gaseous radioactive iodine, a series of covalent organic frameworks (COFs) with dual channels and abundant tertiary-amine active sites were constructed herein via a unique multi-nitrogen node design. The high density of up-to-six nitrogen adsorption sites in a single structural unit of the products effectively improved the adsorption capacities of the materials for iodine. Moreover, the adsorption affinity of the active sites can be further regulated by charge-induced effect of different electron-donating groups introduced into the COFs. Adsorption experiments combined with DFT theoretical calculations confirmed that the introduction of electron-donating groups can effectively increase the electron density around the active sites and enhance the binding energy between the materials and iodine, and thus improve the iodine adsorption capacity to 5.54 g/g. The construction strategy of multi-nitrogen node and charge-induced effect proposed in this study provides an important guidance for the study of the structure-activity relationship of functional materials and the design and preparation of high-performance iodine adsorption materials.
The radionuclide (RN) migration study is not only helpful to understand environmental behavior of RNs, but also can establish the basis for the safety assessment of geological disposal of high-level radioactive waste (HLW). In the context of China's HLW disposal, this review briefly summaries the progress of China's RN migration studies over the past decade regarding three aspects, RN sorption, RN transport and radioactive colloid. Domestic studies from other disciplines (such as geology and environmental science) are also included in this review because they can provide references for the RN migration study. Overall, China has achieved clear progress in RN migration study over the past decade, although large-scaled field experiments are lacked and a gap still exists comparing with the international advanced level. Finally, several suggestions are proposed for future RN migration research in China.
Photocatalytic removal of uranium has attracted much attention in nuclear wastewater treatment and it is highly needed to develop functional photocatalyst with excellent removal performance. In this work, seven kinds of carbon dots/carbon nitride (CDs/CN) composites were synthesized and SerCDs/CN with the best photo-assisted uranium removal performance was screened out. It was found that the introduction of CDs could bring in higher photocurrent density, lower interfacial charge transfer impedance and narrower band gap, resulting in a much-improved removal performance. SerCDs/CN had shown a removal capacity as high as 1690 mg/g and the reaction could be operated under air atmosphere which is promising in real application.
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