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Nanocrystalline Ce(OH)4-based materials: ruthenium selective adsorbent for highly alkaline radioactive liquid waste 基于 Ce(OH)4 的纳米晶材料:用于高碱性放射性废液的钌选择性吸附剂
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-02-13 DOI: 10.1515/ract-2023-0194
Jayaprakasam Selvakumar, Kumari Anshul, Padala A. Nishad, Bhaskarapillai Anupkumar, Subramanian Srinivasan, Nethapakkam R. Jawahar, Appadurai L. Rufus, Jayantha K. Gayen, Tulasi V. Krishna Mohan
Cerium hydroxide, Ce(OH)4 (Ce), has been synthesised and assessed as a Ru-selective adsorbent for treating alkaline radioactive liquid waste. Infrared spectroscopy, thermal analysis, scanning electron microscopy, and energy-dispersive X-ray spectroscopy investigations confirmed the successful formation of nanocrystalline Ce from Ce(NO3)3·6H2O. Selective removal of 106Ru from the ion-exchange effluent of intermediate-level liquid waste (ILW) by Ce was assessed using a high-pure germanium (HPGe) gamma-ray spectrometer. The calculated average distribution coefficient (k D) was ∼200 mL/g. The percentage removal of 106Ru using Ce by varying time, [106Ru] and [Ce] was calculated. The adsorption of 106Ru on Ce follows pseudo-second-order and Freundlich isotherms. The calculated Q max was 93,584 Bq/g. Accelerated leaching studies of the Ru-laden Ce cement product were carried out and found suitable for transport and disposal. Further, Ce-Polyether sulphone (Ce-PES) and Ce-Chitosan (CeC) composites were prepared and assessed for their Ru-uptake capacity for engineering scale application.
氢氧化铈(Ce(OH)4 (Ce))已被合成并评估为一种处理碱性放射性液体废物的 Ru 选择性吸附剂。红外光谱、热分析、扫描电子显微镜和能量色散 X 射线光谱研究证实,Ce(NO3)3-6H2O 成功地形成了纳米晶 Ce。使用高纯锗(HPGe)伽马射线光谱仪评估了 Ce 从中级液体废物(ILW)离子交换流出物中选择性去除 106Ru 的情况。计算得出的平均分布系数(k D)为 200 mL/g。通过改变时间、[106Ru]和[Ce],计算了利用 Ce 去除 106Ru 的百分比。106Ru 在 Ce 上的吸附遵循伪二阶和 Freundlich 等温线。计算得出的最大 Q 值为 93,584 Bq/g。对含有 Ru 的 Ce 水泥产品进行了加速沥滤研究,发现其适合运输和处置。此外,还制备了 Ce 聚醚砜(Ce-PES)和 Ce 壳聚糖(CeC)复合材料,并对其在工程规模应用中的 Ru 吸收能力进行了评估。
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引用次数: 0
An LSC approach for tritium determination in gaseous mixtures optimized with respect to handling, reaction parameters and miniaturization towards microfluidic analysis 用于测定气态混合物中氚含量的 LSC 方法,在处理、反应参数和微型化方面进行了优化,以实现微流控分析
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-02-12 DOI: 10.1515/ract-2023-0262
Alexandra Becker, Holger Lippold, Jantje Pauline Bäcker, Detlev Belder, Cornelius Fischer
The handling and analysis of gaseous tritium is of interest for hydrogen isotope separation experiments. In this work, we present an easy-to-handle setup for catalytic oxidation to HTO, recovering all of the initially dosed gaseous tritium as determined by LSC, using CuO as a catalyst at a reaction temperature of 900 °C. Aiming to reduce cocktail waste, the LSC determination was downscaled to a microfluidic setup. The performance was evaluated based on the counting efficiency, which was shown to decrease significantly, as the sample volume was reduced to µl amounts, while no changes were observed over a wide range of sample-to-cocktail ratios.
气态氚的处理和分析对氢同位素分离实验很有意义。在这项工作中,我们介绍了一种易于处理的催化氧化成 HTO 的装置,利用 CuO 作为催化剂,在 900 °C 的反应温度下,通过 LSC 测定回收了所有初始剂量的气态氚。为了减少鸡尾酒的浪费,将 LSC 测定缩小到微流控装置中。根据计数效率对其性能进行了评估,结果表明,当样品量减少到微升量时,计数效率会显著降低,而在样品与鸡尾酒比率的大范围内没有观察到任何变化。
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引用次数: 0
Application of thin boron deposit by electrophoresis as neutron detectors 将电泳薄硼沉积物用作中子探测器
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-02-12 DOI: 10.1515/ract-2023-0226
Mohamed Fares, Mohammed Messaoudi, Mohamed Yacine Debili, Kassida Negara
Detecting nuclear radiation presents a distinctive challenge, particularly with neutrons, which are neutral particles. The method of direct detection involves the utilization of a converter material, acting as an intermediary. Boron plays a pivotal role in this process, reacting with thermal neutrons to generate alpha particles and lithium, with a notable energy release of 2.314 MeV during the 10B (n,α) 7Li reaction. This facilitates effective identification and measurement of neutrons in radiation detection systems. The paths of the particles α (for E = 1.474 MeV) and Li (for E Li = 0.842 MeV). The active medium of the nuclear detector, typically a gas, undergoes ionization by these highly charged particles, or they form ion pairs that are subsequently collected by electrodes to produce the signal at the detector’s output. Various deposit methods can be used for this purpose, electrophoresis offers a distinct advantage in terms of both simplicity and precision. This study details the utilization of the electrophoresis technique for the deposition of boron on the tube walls of prototype detectors developed within our laboratory.
检测核辐射是一项独特的挑战,尤其是中子这种中性粒子。直接探测的方法需要利用一种转换材料作为中介。硼在这一过程中起着关键作用,它与热中子反应生成α粒子和锂,在 10B (n,α) 7Li 反应中释放出 2.314 MeV 的显著能量。这有助于在辐射探测系统中有效识别和测量中子。粒子 α(E = 1.474 MeV)和 Li(E Li = 0.842 MeV)的运动轨迹。核探测器的活性介质(通常是气体)会被这些高电荷粒子电离,或形成离子对,然后被电极收集,在探测器的输出端产生信号。有多种沉积方法可用于此目的,其中电泳在简便性和精确性方面具有明显优势。本研究详细介绍了利用电泳技术在我们实验室开发的原型探测器管壁上沉积硼的情况。
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引用次数: 0
Observations regarding the synthesis and redox chemistry of heterobimetallic uranyl complexes containing Group 10 metals 有关含有第 10 族金属的杂多金属铀酰络合物的合成和氧化还原化学的观察结果
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-02-09 DOI: 10.1515/ract-2023-0237
Emily R. Mikeska, Natalie M. Lind, Alexander C. Ervin, Celine Khalife, Joseph P. Karnes, James D. Blakemore
Literature reports have demonstrated that Schiff-base-type ligands can serve as robust platforms for the synthesis of heterobimetallic complexes containing transition metals and the uranyl dication (UO2 2+). However, efforts have not advanced to include either synthesis of complexes containing second- or third-row transition metals or measurement of the redox properties of the corresponding heterobimetallic complexes, despite the significance of actinide redox in studies of nuclear fuel reprocessing and separations. Here, metalloligands denoted [Ni], [Pd], and [Pt] that contain the corresponding Group 10 metals have been prepared and a synthetic strategy to access species incorporating the uranyl ion (UO2 2+) has been explored, toward the goal of understanding how the secondary metals could tune uranium-centered redox chemistry. The synthesis and redox characterization of the bimetallic complex [Ni,UO2] was achieved, and factors that appear to govern extension of the chosen synthetic strategy to complexes with Pd and Pt are reported here. Infrared and solid-state structural data from X-ray diffraction analysis of the metalloligands [Pd] and [Pt] show that the metal centers in these complexes adopt the expected square planar geometries, while the structure of the bimetallic [Ni,UO2] reveals that the uranyl moiety influences the coordination environment of Ni(II), including inducement of a puckering of the ligand backbone of the complex in which the phenyl rings fold around the nickel-containing core in an umbrella-shaped fashion. Cyclic voltammetric data collected on the heterobimetallic complexes of both Ni(II) and Pd(II) provide evidence for uranium-centered redox cycling, as well as for the accessibility of other reductions that could be associated with Ni(II) or the organic ligand backbone. Taken together, these results highlight the unique redox behaviors that can be observed in multimetallic systems and design concepts that could be useful for accessing tunable multimetallic complexes containing the uranyl dication.
文献报道表明,希夫碱配体可以作为合成含有过渡金属和铀酰二价(UO2 2+)的杂二金属络合物的可靠平台。然而,尽管锕系元素的氧化还原反应在核燃料后处理和分离研究中具有重要意义,但在合成含有第二排或第三排过渡金属的络合物或测量相应杂多金属络合物的氧化还原特性方面的工作还没有取得进展。在此,我们制备了含有相应第 10 族金属的金属配体(以[Ni]、[Pd]和[Pt]表示),并探索了获得含有铀酰离子(UO2 2+)的物种的合成策略,目的是了解次级金属如何调节以铀为中心的氧化还原化学。本文报告了双金属络合物 [Ni,UO2] 的合成和氧化还原特性,以及将所选合成策略扩展到与钯和铂的络合物的因素。对金属配体 [Pd] 和 [Pt] 进行 X 射线衍射分析所得到的红外和固态结构数据表明,这些配合物中的金属中心采用了预期的方形平面几何结构,而双金属 [Ni,UO2] 的结构则表明,铀酰分子会影响 Ni(II) 的配位环境,包括诱发配合物配体骨架的皱褶,在皱褶中,苯基环以伞形方式折叠在含镍核心周围。在 Ni(II) 和 Pd(II) 的杂双金属配合物上收集的循环伏安数据证明了以铀为中心的氧化还原循环,以及与 Ni(II) 或有机配体骨架有关的其他还原的可及性。总之,这些结果突出了多金属体系中可以观察到的独特氧化还原行为,以及有助于获得含有铀酰二阳离子的可调多金属复合物的设计理念。
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引用次数: 0
Incorporation of phytic acid into reed straw-derived hydrochar for highly efficient and selective adsorption of uranium(VI) 将植酸掺入芦苇秸秆衍生的水炭中以高效、选择性地吸附铀(VI)
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-02-08 DOI: 10.1515/ract-2023-0250
Hongtao Xia, Yuting Liu, Yang Wang, Zihao Feng, Qi Ren, Jianqi Lv, Yang Li, Yanjun Du, Yun Wang
An innovative phytic acid modified reed straw-derived hydrochar composite (PA-C-RBC) was prepared by using inexpensive reed straw and non-toxic phytic acid for the removal of uranium(VI) from aqueous environment. Several characterization results showed that PA-C-RBC was rough and porous with a large number of hydroxyl, carboxyl, and phosphate groups. The uranium(VI) adsorption process by PA-C-RBC conformed to pseudo-second-order kinetic and Langmuir models, and the theoretical maximal adsorption capacity could attain 418.78 mg/g at pH 5.0. PA-C-RBC had 72.66 % of selectivity and 6772.99 mL/g of distribution coefficient for U(VI). Due to the strong chelating between the hydroxyl and phosphate groups on PA-C-RBC and U(VI), PA-C-RBC had excellent adsorption selectivity. These finding highlighted a high potential for removing U(VI) from aqueous solutions.
利用廉价的芦苇秆和无毒的植酸制备了一种创新的植酸改性芦苇秆衍生水炭复合材料(PA-C-RBC),用于去除水环境中的铀(VI)。多项表征结果表明,PA-C-RBC 具有粗糙的多孔性,含有大量羟基、羧基和磷酸基。PA-C-RBC 对铀(VI)的吸附过程符合假二阶动力学模型和 Langmuir 模型,在 pH 值为 5.0 时,理论最大吸附容量可达 418.78 mg/g。PA-C-RBC 对铀(Ⅵ)的选择性为 72.66%,分布系数为 6772.99 mL/g。由于 PA-C-RBC 上的羟基和磷酸基与 U(VI)具有很强的螯合作用,因此 PA-C-RBC 具有极佳的吸附选择性。这些发现凸显了 PA-C-RBC 从水溶液中去除铀(VI)的巨大潜力。
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引用次数: 0
Characterization of glass composite material by pressureless sintering of soil and its application to uranium contaminated soil as a waste form 土壤无压烧结玻璃复合材料的特性及其在作为废物形式的铀污染土壤中的应用
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-01-24 DOI: 10.1515/ract-2023-0222
Jaewoong Hwang, Jaseung Koo, Kenyoung Lee
When operating and dismantling a nuclear facility that handles uranium, the surrounding soil may be contaminated, emphasizing the need for appropriate treatment and disposal methods for soil waste. This study assessed high-temperature sintering technology for uranium contaminated soil waste to overcome limitations in existing decontamination methods and the volume increase associated with current solidification technology. The sintering process was found to effectively vitrify and re-mineralize complex chemical components in the soil. Sintered bodies were produced under varying conditions, adjusting molding pressure, heating temperature, and time. Optimized conditions resulted in sintered bodies with a volume reduction rate exceeding 30 % and a compressive strength surpassing 10 MPa, indicating a significant impact on the phase conversion and re-mineralization of silt and clay minerals. The soil sintering mechanism was identified through comprehensive microscopic observations and mineral phase change analysis. Leaching evaluations of sintered bodies, made from simulated uranium-contaminated soil, demonstrated their applicability to contaminated soil wastes. Additionally, it was confirmed that the sintering temperature of the soil could be lowered by incorporating a small amount of B2O3, suggesting a means to enhance the economic feasibility of the treatment process. The findings of this study highlight the applicability of pressureless sintering technology, based on glass composite materials, capable of simultaneously reducing and stabilizing uranium-contaminated soil waste.
在运行和拆除处理铀的核设施时,周围的土壤可能会受到污染,因此需要对土壤废物采取适当的处理和处置方法。这项研究评估了铀污染土壤废物的高温烧结技术,以克服现有去污方法的局限性和当前固化技术带来的体积增加问题。研究发现,烧结过程能有效地使土壤中复杂的化学成分玻璃化和再矿化。烧结体是在不同条件下生产的,需要调整成型压力、加热温度和时间。优化条件下烧结体的体积减小率超过 30%,抗压强度超过 10 兆帕,这表明烧结体对淤泥和粘土矿物的相转化和再矿化具有重要影响。通过全面的显微观察和矿物相变分析,确定了土壤烧结机制。对模拟铀污染土壤烧结体的浸出评估表明,烧结体适用于受污染的土壤废物。此外,研究还证实,通过加入少量 B2O3 可以降低土壤的烧结温度,从而提高处理过程的经济可行性。这项研究的结果凸显了基于玻璃复合材料的无压烧结技术的适用性,该技术能够同时减少和稳定铀污染土壤废物。
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引用次数: 0
Obituary: Jae-Il Kim (1936–2023) 讣告金载一(1936-2023)
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-01-19 DOI: 10.1515/ract-2023-2001
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引用次数: 0
Determination of natural radionuclides and heavy metal concentrations in the groundwater and adjacent areas of the Kattakurgan reservoir, Uzbekistan 乌兹别克斯坦卡塔库尔干水库地下水及附近地区天然放射性核素和重金属浓度的测定
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-01-12 DOI: 10.1515/ract-2023-0254
U. Tukhtaev, Shakhboz Khasanov, Jaloliddin Fayzullayev, A. Safarov, Bayramali Togaev, Seyedkarim Afsharipour
Abstract We conducted a comprehensive assessment of the Kattakurgan reservoir, alongside adjacent wells and boreholes, to measure the concentrations of natural radionuclides, heavy metals, and associated radiological hazards. Using NaI(Tl) crystal scintillation gamma spectrometers, we determined radionuclide levels in water and sediment. Inductively coupled plasma mass spectrometry (ICP-MS) was employed for heavy metal analysis. Our results showed radionuclide concentrations in reservoir water for 226Ra (0.8 Bq/L), 232Th (0.4 Bq/L), and 40K (0.4 Bq/L) were within the limits set by the World Health Organization (WHO). In contrast, deep well water samples showed elevated 226Ra concentrations (1.5 Bq/L). Sediment samples’ radionuclide levels were in line with UNSCEAR guidelines. Barium was the most notable heavy metal, with a concentration of 68.08 μg/L. While most radiation hazard indices remained within safety limits, the gamma index recorded a value of 1.057 Bq/kg. Our research provides valuable data for water quality assessment. The methods described can be applied to other reservoir studies. Regular monitoring is recommended for continuous safety evaluation, and further studies on biotic samples are suggested to enhance understanding of the reservoir’s ecosystem health.
摘要 我们对卡塔库尔干水库以及邻近的水井和钻孔进行了全面评估,以测量天然放射性核素、重金属和相关放射性危害的浓度。我们使用 NaI(Tl)晶体闪烁伽马能谱仪测定了水和沉积物中的放射性核素含量。重金属分析则采用了电感耦合等离子体质谱法(ICP-MS)。结果显示,水库水中 226Ra(0.8 Bq/L)、232Th(0.4 Bq/L)和 40K(0.4 Bq/L)的放射性核素浓度均在世界卫生组织(WHO)规定的范围之内。相比之下,深井水样本中的 226Ra 浓度较高(1.5 Bq/L)。沉积物样本的放射性核素水平符合联合国辐射防护委员会的指导方针。钡是最显著的重金属,浓度为 68.08 微克/升。虽然大多数辐射危害指数都保持在安全范围内,但伽马指数却达到了 1.057 Bq/kg。我们的研究为水质评估提供了宝贵的数据。所述方法可用于其他水库研究。建议进行定期监测,以进行持续的安全评估,并建议对生物样本进行进一步研究,以加深对水库生态系统健康状况的了解。
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引用次数: 0
CaO-enhanced polyester for safety: experimental study on fabrication, characterization, and gamma-ray attenuation 氧化钙增强型安全聚酯:关于制造、表征和伽马射线衰减的实验研究
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-01-12 DOI: 10.1515/ract-2023-0265
M. Marashdeh, K. A. Mahmoud
Abstract The current work deals with studying the influence of cheap, widespread CaO on improving the γ ray-protection capacity of the lightweight, sealing polyester. Therefore, polyester composites were filled with different concentrations of CaO fillers. The fabricated CaO-reinforced polyester composites’ density ranged between 1.177 g/cm3 and 1.377 g/cm3, when CaO filler concentrations increased between 0 wt% and 60 wt%, respectively. Fabricated composites’ morphology and chemical composition, as well as CaO fillers’ grain size and distribution, were proved using SEM and EDX spectroscopy. Additionally, the influence of CaO fillers on the gamma-ray shielding properties of the fabricated composites was evaluated using the Monte Carlo simulation and confirmed using the experimental measurements. The recorded results show an enhancement in the synthesized composites’ linear attenuation coefficient from 0.091 cm−1 to 0.106 cm−1 at a gamma ray energy of 0.662 MeV. Moreover, the excess in CaO concentration from 0 wt% and 60 wt% reduces the fabricated composites’ half-value thickness values from 7.64 cm to 6.51 cm, respectively.
摘要 当前的工作是研究廉价、广泛使用的氧化钙对提高轻质密封聚酯的γ射线防护能力的影响。因此,聚酯复合材料中填充了不同浓度的 CaO 填料。当 CaO 填料浓度在 0 wt% 和 60 wt% 之间增加时,制备的 CaO 增强聚酯复合材料的密度在 1.177 g/cm3 和 1.377 g/cm3 之间。利用扫描电镜和乙二胺四乙酸(EDX)光谱法证明了制备的复合材料的形貌和化学成分,以及 CaO 填料的粒度和分布。此外,还利用蒙特卡洛模拟评估了 CaO 填料对所制复合材料伽马射线屏蔽性能的影响,并通过实验测量进行了确认。记录结果显示,在伽马射线能量为 0.662 MeV 时,合成复合材料的线性衰减系数从 0.091 cm-1 提高到 0.106 cm-1。此外,氧化钙浓度从 0 wt% 增加到 60 wt%,复合材料的半值厚度值也从 7.64 cm 减小到 6.51 cm。
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引用次数: 0
Overcoming the obstacle of excess acetonitrile content in the final fluorine-18 radiotracers 克服最终氟-18 放射性标记物中乙腈含量过高的障碍
IF 1.8 3区 化学 Q3 Chemistry Pub Date : 2024-01-09 DOI: 10.1515/ract-2023-0225
Mohammed Al-Qahtani
Abstract Acetonitrile is widely used as a solvent in synthesizing various fluorine-18 positron emission tomography (PET) radiotracers. Acetonitrile is classified as a Class II residual solvent, and due to its inherent toxic properties, the quantity of residual acetonitrile in drug products has to be limited. When working under Good Manufacturing Practices (GMP) during the radiosynthesis of a radiotracer, the aim is to control all solvent concentrations contained in the ready-to-use product. All products must meet predetermined specifications. Rarely, these limits may be exceeded. To avoid eliminating the entire batch, applying a straightforward time-based technique would be desirable to allow the majority of the product to be safely used. This technique should be based on determining a specific time and volume for which the radiotracer can be utilized in the patients after completing quality control analysis. Here, we report a very simple Excel sheet program based on existing mathematical equations that calculates the exact time and volume at which the radiotracer product can be safely administered to a patient.
摘要 乙腈被广泛用作合成各种氟-18 正电子发射断层扫描(PET)放射示踪剂的溶剂。乙腈被列为二类残留溶剂,由于其固有的毒性,药物产品中的乙腈残留量必须加以限制。在放射性示踪剂的放射性合成过程中,按照《药品生产质量管理规范》(GMP)进行操作时,目的是控制即用产品中所有溶剂的浓度。所有产品都必须符合预定的规格。在极少数情况下,可能会超出这些限制。为避免剔除整批产品,最好采用一种直接的基于时间的技术,以便安全地使用大 部分产品。这种技术应基于确定一个特定的时间和数量,在完成质量控制分析后,放射性示踪剂可用于患者。在此,我们报告了一个基于现有数学公式的非常简单的 Excel 表程序,该程序可计算出患者可安全使用放射性示踪剂产品的确切时间和用量。
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引用次数: 0
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Radiochimica Acta
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