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Technology for Reprocessing Mother–Wash Solution after Crystallization Purification of Spent Nuclear Fuel from High Temperature Gas-Cooled Reactor 高温气冷堆乏核燃料结晶净化后母液再处理技术
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020061
L. I. Tkachenko, V. L. Vidanov, E. V. Kenf, N. Yu. Volodina, Ya. O. Pleshakov, A. Yu. Shadrin

Abstract

The extractants diphenyl-N,N-dioctylcarbamoylmethylphosphine oxide and diphenyl-N,N-diisobutylcarbamoylmethylphosphine oxide for the SNF reprocessing were tested. The conditions for extraction and separation of uranium and TPE–REE were determined. A flowsheet was proposed for reprocessing SNF from high-temperature gas-cooled reactors. Upon dynamic testing, at least 99.9% of uranium and plutonium and at least 99.5% of americium and rare earth elements were separated. The TPE + REE and U + Pu fractions were recovered. The U + Pu fraction contained approximately 5% Am, while the TPE + REE fraction had less than 0.1% U and Pu.

摘要 试验了用于 SNF 后处理的萃取剂二苯基-N,N-二辛基氨基甲酰基甲基氧化膦和二苯基-N,N-二异丁基氨基甲酰基甲基氧化膦。确定了铀和 TPE-REE 的提取和分离条件。提出了高温气冷堆 SNF 后处理流程图。经动态测试,至少分离出 99.9% 的铀和钚以及至少 99.5% 的镅和稀土元素。回收了 TPE + REE 和 U + Pu 部分。铀+钚馏分含有大约 5%的镅,而热塑性聚乙烯+稀土元素馏分中的铀和钚含量低于 0.1%。
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引用次数: 0
The Influence of the Sizes of Nanodiamond Aggregates in Suspensions on the Efficiency of Sorption of 90Y and 177Lu Isotopes for Further Use in Nuclear Medicine 悬浮液中纳米金刚石聚集体的尺寸对进一步用于核医学的 90Y 和 177Lu 同位素吸附效率的影响
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020097
A. G. Kazakov, J. S. Babenya, T. Y. Ekatova, S. E. Vinokurov, E. Y. Khvorostinin, I. A. Ushakov, V. V. Zukau, E. S. Stasyuk, E. A. Nesterov, V. L. Sadkin, A. S. Rogov, B. F. Myasoedov

Abstract

Nanodiamonds (NDs) are promising carriers of radionuclides in radiopharmaceuticals for the use in nuclear medicine. In this work, we investigated the influence of the properties of NDs suspensions, including the sizes of their aggregates, in aqueous solutions with different pH on their binding of medical isotopes 90Y and 177Lu and determination of conditions for fabricating promising conjugates for further in vivo studies. It was shown that sorption is influenced by the composition of the solution, which determines the properties of the NDs surface, while the forms of cations of the studied nuclides in the solution do not affect the sorption value.

摘要 纳米金刚石(NDs)是放射性药物中很有前途的放射性核素载体,可用于核医学。在这项工作中,我们研究了不同 pH 值的水溶液中纳米金刚石悬浮液的性质(包括其聚集体的大小)对其与医用同位素 90Y 和 177Lu 结合的影响,并确定了为进一步的体内研究制造有前景的共轭物的条件。研究表明,吸附力受溶液成分的影响,溶液成分决定了玖龙表面的特性,而所研究的核素在溶液中的阳离子形式并不影响吸附值。
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引用次数: 0
Obtaining of Nanodiamond Conjugates with Scandium Isotopes for the Use in Nuclear Medicine 获得用于核医学的钪同位素纳米金刚石共轭物
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020103
A. G. Kazakov, T. Y. Ekatova, S. E. Vinokurov, E. Y. Khvorostinin, I. A. Ushakov, V. V. Zukau, E. S. Stasyuk, E. A. Nesterov, V. L. Sadkin, A. S. Rogov, B. F. Myasoedov

Abstract

In this work, we studied the sorption of scandium, whose isotopes 44Sc and 47Sc are explored for diagnostics and therapy in nuclear medicine, by aggregates of commercial (TAN, STP) and oxidized nanodiamonds (ox-STP) from aqueous solutions. The sorption capacity of the studied NDs for scandium was determined; 100 μg of NDs is found to be sufficient for the sorption of 1 GBq of 47Sc, which is equivalent to the activity of isotopes used in therapy. It was shown that the supposed mechanism for the binding of Sc(III) to nanodiamond aggregates is chemisorption, and the chemical composition of the nanodiamond surface affects the sorption efficiency to a greater extent than the speciation of scandium in solution. The obtained data on Sc(III) sorption are correlated with the sizes of nanodiamond aggregates; it is shown that sorption under experimental conditions does not depend on the size of the aggregates. For the further development of radiopharmaceuticals based on 47Sc, optimal carriers for this isotope—TAN and ox-STP—were suggested.

摘要 在这项工作中,我们研究了商用纳米金刚石(TAN、STP)和氧化纳米金刚石(ox-STP)聚集体从水溶液中吸附钪的情况,钪的同位素 44Sc 和 47Sc 在核医学中被用于诊断和治疗。测定了所研究的纳米金刚石对钪的吸附能力;发现 100 μg 的纳米金刚石足以吸附 1 GBq 的 47Sc,这相当于用于治疗的同位素的活性。研究表明,Sc(III)与纳米金刚石聚集体结合的假定机制是化学吸附,纳米金刚石表面的化学成分对吸附效率的影响程度大于溶液中钪的种类。所获得的 Sc(III) 吸附数据与纳米金刚石聚集体的大小相关;实验表明,实验条件下的吸附与聚集体的大小无关。为进一步开发基于 47Sc 的放射性药物,提出了该同位素的最佳载体--TAN 和 ox-STP。
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引用次数: 0
Dynamic Tests of Cesium-137 Recovery from the Mayak Model Alkaline HLW with p-Isononylcalix[6]arene-based Extractant 用对-壬基钙[6]烯萃取剂从马雅克模型碱性 HLW 中回收铯-137 的动态测试
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s106636222402005x
A. Z. Yumaguen, E. S. Babitova, M. V. Logunov, M. D. Karavan, P. V. Kozlov, A. V. Konnikov, I. V. Smirnov

Abstract

The article presents the results of studies on composition optimization, properties, and laboratory dynamic tests of extraction mixtures based on p-isononylcalix[6]arene for the alkaline HLW purification to remove 137Cs. The distribution of 137Cs among the products of the technological scheme is presented and the raffinate purification factor to remove 137Cs are determined. It was revealed that, in the case of using nitric acid as a stripping solution, nitrosation of p-isononylcalix[6]arene is possible in the technological process. The composition of the resulting product was determined. To prevent nitrosation of p-isononylcalix[6]arene, formic acid was used in the stripping stage, which ensured stable operation of the extraction setup for 48 h while 137Cs extraction from model alkaline HLW was at a level of 99.7%.

摘要 本文介绍了基于对异壬基癸氧[6]炔的萃取混合物的成分优化、特性和实验室动态测试研究结果,该混合物用于碱性高放废物净化以去除 137Cs。介绍了 137Cs 在技术方案产物中的分布情况,并确定了去除 137Cs 的萃取物净化系数。研究发现,在使用硝酸作为汽提溶液的情况下,对异壬基萼[6]炔有可能在技术过程中发生亚硝基化反应。对由此产生的产品的成分进行了测定。为防止对-异壬基萼[6]炔发生亚硝酸盐化,在汽提阶段使用了甲酸,这确保了萃取装置稳定运行 48 小时,而从模型碱性 HLW 中萃取的 137Cs 达到了 99.7%的水平。
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引用次数: 0
Determination of the Thermal Stability of Impregnated Type Solid Extractant Based on Dibenzo-21-crown-7 and Organic Matrix MN-200 基于二苯并-21-冠醚-7 和有机基质 MN-200 的浸渍型固体萃取剂热稳定性的测定
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020140
A. V. Rodin, A. M. Koscheeva, K. V. Shelamov, L. V. Gezalyan, A. V. Ponizov, A. V. Ananiev

Abstract

The thermal stability of dibenzo-21-crown-7 and of MN-200 organic matrix based on styrene–divinylbenzene in inert and oxidizing atmosphere at temperatures of up to 600°С was studied. Solid extractants (SEs) were prepared from these components. These SEs are stable up to 300°С in inert atmosphere and up to 180–250°С in oxidizing atmosphere, depending on the presence of an additional diluent, fluorinated alcohol, in the SE. At higher temperatures, the SEs undergo exothermic processes accompanied by the formation of such major gaseous products as toluene, styrene, benzaldehyde, 1-ethyl-4-methylbenzene, and 1,3-dioxolane. Their yield depends on the type of the gaseous atmosphere used.

摘要 研究了二苯并-21-冠醚-7 和基于苯乙烯-二乙烯基苯的 MN-200 有机基质在惰性和氧化气氛中的热稳定性。用这些成分制备了固体萃取剂(SE)。这些固体萃取剂在惰性气氛中的稳定性可达 300°С,在氧化气氛中的稳定性可达 180-250°С,具体取决于萃取剂中是否含有额外的稀释剂--氟化醇。在较高温度下,SE 会发生放热过程,并形成甲苯、苯乙烯、苯甲醛、1-乙基-4-甲基苯和 1,3-二氧戊环等主要气态产物。它们的产量取决于所用气体环境的类型。
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引用次数: 0
Preparation of High-Labeled Graphene Oxide by Tritium Thermal Activation Method for Application in the Betavoltaic Cell of a Nuclear Battery 利用氚热活化法制备高标记氧化石墨烯,并将其应用于核电池的光伏电池中
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020073
G. A. Badun, V. A. Bunyaev, M. G. Chernysheva

Abstract

The possibility of tritium introduction into graphene oxide (GO) by tritium thermal activation method was demonstrated. It was established that, in order to produce the highest possible specific radioactivity, thin films of GO with a thickness of 5.6 mg/m2 must be treated with tritium atoms. The experiment conducted at 77 K showed a number of advantages. GO was processed with tritium atoms, the resulting specific activity of [3H]GO reached 2.6 Ci/mg in term of the weight of the initial GO (0.7 Ci/mg after removal of the labile tritium). Specific energy release of [3H]GO with this specific activity is 22.3 W/kg, which is quite sufficient for its application as a component of a nuclear battery.

摘要 通过氚热激活法证明了将氚引入氧化石墨烯(GO)的可能性。实验证明,为了产生尽可能高的比放射性,必须用氚原子处理厚度为 5.6 mg/m2 的氧化石墨烯薄膜。在 77 K 温度下进行的实验显示了许多优点。用氚原子处理 GO 后,[3H]GO 的比放射性活度达到 2.6 Ci/mg(按初始 GO 重量计算)(去除易变氚后为 0.7 Ci/mg)。具有这种比活度的[3H]GO 的比能量释放为 22.3 W/kg,这足以将其用作核电池组件。
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引用次数: 0
Diffusion of Radioactive Waste Elements from Underground Water and Leachates of Phosphate Waste Forms in Pore Solution of Clay Materials 粘土材料孔隙溶液中地下水和磷酸盐废物浸出液中放射性废物元素的扩散
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020115
K. V. Martynov, E. V. Zakharova

Abstract

Using through diffusion method at room temperature, migration of simulants of RW elements (P, Se, Br, Mo, Cs, U) in compacted samples of clay materials of various mineral compositions was studied during porous diffusion from model solutions: underground water and leachates of phosphate waste forms having a total salt content of up to 500 mg/L. Based on the results of experiments, effective diffusion coefficients and sorption distribution coefficients of elements in barrier materials were determined. Numerical models are proposed to describe diffusion transfer of selenium, cesium, and uranium depending on porosity, mineral composition of materials, and concentration of elements in pore solution. Patterns of diffusion of elements from solutions of different salt composition were revealed.

摘要 通过室温下的扩散法,研究了各种矿物成分的粘土材料压实样品中 RW 元素(P、Se、Br、Mo、Cs、U)模拟物从模型溶液(地下水和总盐含量高达 500 mg/L 的磷酸盐废物浸出液)中进行多孔扩散时的迁移情况。根据实验结果,确定了元素在屏障材料中的有效扩散系数和吸附分布系数。根据孔隙率、材料的矿物成分以及孔隙溶液中元素的浓度,提出了描述硒、铯和铀扩散转移的数值模型。揭示了元素从不同盐成分溶液中扩散的模式。
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引用次数: 0
Evaluation of Natural Radioactivity in Soil Samples Collected from the Khasa River Banks in Kirkuk, Iraq 对从伊拉克基尔库克哈萨河岸采集的土壤样本中天然放射性的评估
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020139
A. M. Shaker, A. H. Taqi, A. El-Taher

Abstract

The natural radioactivity in soil samples collected from the Khasa River, which flows in the Kirkuk city of Iraq, was studied using a high-purity germanium (HPGe) detector and a spectroscopy system. The activity concentrations (Bq kg−1) of 214Pb, 226Ra, 212Pb, 228Ac, and 40K varied from 10.1 ± 0.6 to 27.5 ± 3.2, from 23.4 ± 2.8 to 44.1 ± 6.1, from 13.2 ± 0.7 to 26.4 ± 1.8, from 12.5 ± 0.9 to 28.1 ± 4.3, and from 206.5 ± 12.8 to 332.2 ± 7.2, respectively. The results have been compared to the average worldwide values. The hazard indices have also been calculated. The average of radium equivalent activity (Raeq) was 81.2 Bq kg−1; the absorbed gamma dose rate (D) was 42.8 nGy h−1; the annual effective dose rates (AEDE) outdoor and indoor were 0.05 and 0.2 mSv year−1, respectively; the external hazard (Hex) was 0.2; the internal hazard (Hin) was 0.3; the gamma radiation representative level index (Iγ) was 0.5. Our results for some sites were found to be higher than the worldwide values.

摘要 使用高纯锗(HPGe)探测器和光谱系统对从流经伊拉克基尔库克市的卡萨河采集的土壤样本中的天然放射性进行了研究。214Pb、226Ra、212Pb、228Ac 和 40K 的放射性浓度(Bq kg-1)分别为 10.1 ± 0.6 至 27.5 ± 3.2、23.4 ± 2.8 至 44.1 ± 6.1、13.2 ± 0.7 至 26.4 ± 1.8、12.5 ± 0.9 至 28.1 ± 4.3 和 206.5 ± 12.8 至 332.2 ± 7.2。这些结果与全球平均值进行了比较。还计算了危害指数。镭当量活度(Raeq)的平均值为 81.2 Bq kg-1;吸收伽马剂量率(D)为 42.8 nGy h-1;室外和室内的年有效剂量率(AEDE)分别为 0.05 和 0.2 mSv year-1;外部危害(Hex)为 0.2;内部危害(Hin)为 0.3;伽马辐射代表水平指数(Iγ)为 0.5。我们发现某些地点的结果高于全球数值。
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引用次数: 0
Speciation of Uranium in Trace Concentrations in Aqueous Solutions of Complex Chemical Composition 化学成分复杂的水溶液中痕量浓度铀的标示
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020164
F. F. Faizrakhmanov

Abstract

Speciation of uranium in trace concentrations in water of complex chemical composition was studied using ultrafiltration and sorption methods in a wide range of solution acidity. As shown by the experiments and computations, uranium in trace concentrations in aqueous solutions identical to wastewater from the facilities occurs at pH 1–3 in the truly dissolved state in the form of UO22+ and UO2OH+ ions. At pH ≥ 4, uranium(VI) mainly occurs in the pseudocolloidal form due to sorption on hydroxides of iron, aluminum, or other impurity elements. The decrease in the fraction of uranium colloids at pH ≥ 7 is due to the formation of stable, negatively charged uranyl carbonate complexes in the solution.

摘要 采用超滤和吸附方法研究了复杂化学成分水体中痕量浓度铀在较大溶液酸度范围内的分布情况。实验和计算表明,与设施废水相同的水溶液中的痕量铀在 pH 值为 1-3 时以 UO22+ 和 UO2OH+ 离子的形式真正溶解。当 pH 值≥4 时,铀(VI) 主要以假胶体形式存在,这是由于吸附在铁、铝或其他杂质元素的氢氧化物上。pH≥7 时,铀胶体的比例下降,这是由于溶液中形成了稳定的、带负电荷的碳酸铀酰络合物。
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引用次数: 0
Statistical Evaluation of the Tritium Content of Aquatic Ecosystems at NPP Sites 核电厂厂址水生生态系统氚含量的统计评估
IF 0.9 Q4 Chemistry Pub Date : 2024-05-16 DOI: 10.1134/s1066362224020174
L. G. Bondarenko, V. N. Dushin, A. D. Sadykin, S. I. Shabalev

Abstract

The lognormal statistical distribution was used to present the reliable integrated data on the content of various physicochemical forms of tritium in air, natural water, and components of aquatic ecosystems at nuclear facility sites. Statistics of lognormal distributions took into account the left truncation, which reflects the effect of finite sensitivity of measurements. The statistics of lognormal distributions were used to obtain estimates for ecosystems of NPP sites at limited sets of data. Specific activities were estimated for various forms of tritium such as HTO (free water), TFWT (tissue free water tritium), and OBT (organically bound tritium). The measurement results show that the specific activity of tritium in the body in bound forms was, as a rule, higher than its specific activity in free water in the ambient environment. Equilibrium concentration ratios (CRs) (partition coefficients of hydrogen) ranged from 1 to about 20. The results obtained by the Radium Institute research team agree with those obtained by the researchers from Canada and France for the specific activity of tritium in different chemical forms in environmental samples.

摘要 采用对数正态分布统计方法,给出了核设施所在地空气、天然水和水生生态系统成分中各种物理化学形式的氚含量的可靠综合数据。对数正态分布统计考虑了左截断,这反映了测量的有限灵敏度的影响。对数正态分布统计用于在有限的数据集上获得核电厂所在地生态系统的估计值。对 HTO(自由水)、TFWT(组织自由水氚)和 OBT(有机结合氚)等各种形式的氚的比活度进行了估算。测量结果表明,人体内结合态氚的比活度通常高于环境中自由水中氚的比活度。平衡浓度比(CRs)(氢的分配系数)从 1 到 20 左右不等。镭研究所研究小组获得的结果与加拿大和法国研究人员获得的环境样本中不同化学形态氚的比活度结果一致。
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引用次数: 0
期刊
Radiochemistry
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