Uranium

  • 文章类型: Journal Article
    牙釉质中碳酸盐羟基磷灰石的电子自旋共振与铀系列测年(ESR/U系列)相结合,是用于从放射性碳测年范围之外的更新世化石中获得年龄测定的主要技术。这些时间信息可以更好地了解古生物学记录的历时变化,特别是关于人属的进化。鉴于古生物学和考古学地区人类牙齿的相对匮乏,ESR/U系列广泛应用于有蹄类动物的牙齿。然而,ESR/U系列年龄的准确性受到埋藏在沉积物中的搪瓷中铀含量的影响。已经表明,铀含量与碳酸盐羟基磷灰石晶体中原子序的增加呈正相关,后者使用红外光谱测定。在这里,我们提供了来自非洲有蹄类动物的牙釉质的参考红外光谱库,基于磨削曲线法,作为基线,以跟踪不同物种中碳酸盐羟基磷灰石的成岩历史,从而选择保存最好的标本进行测年。
    Electron spin resonance coupled with uranium-series dating (ESR/U-series) of carbonate hydroxyapatite in tooth enamel is the main technique used to obtain age determinations from Pleistocene fossils beyond the range of radiocarbon dating. This chronological information allows to better understand diachronic change in the palaeontological record, especially with regard to the evolution of the genus Homo. Given the relative paucity of human teeth at palaeontological and archaeological localities, ESR/U-series is widely applied to the teeth of ungulate species. However, the accuracy of ESR/U-series ages is greatly affected by the incorporation of uranium in the enamel during burial in sediments. It has been shown that uranium content is positively correlated with an increased degree of atomic order in carbonate hydroxyapatite crystals, the latter determined using infrared spectroscopy. Here we present a reference infrared spectral library of tooth enamel from African ungulates, based on the grinding curve method, which serves as baseline to track the diagenetic history of carbonate hydroxyapatite in different species and thus select the best-preserved specimens for dating.
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  • 文章类型: Journal Article
    向日葵(Helianthusannuus)可潜在地用于铀(U)植物修复。然而,影响U的吸收及其随后在植物组织中分布的因素仍不清楚,包括已知增加金属耐受性的硅(Si)的作用。这里,使用水培法,使用基于同步加速器的X射线荧光和荧光X射线吸收近边缘光谱检查了Si对向日葵中U的分布和形态的影响。研究发现,无论如何处理,88%的U都会在根内积累。如果不添加Si,大部分U似乎与根部的表皮结合,而在树叶中,U主要积累在静脉中。添加Si减轻了U的植物毒性,并使向日葵中的U浓度平均降低了60%。在根中,Si增强U在细胞壁中的分布并阻碍其进入细胞,可能是由于call体沉积增加。在树叶中,Si诱导U在毛状体中的螯合。然而,Si没有改变U的形态,U保持六价形式。这些结果提供了向日葵体内U积累和分布的信息,并表明Si可以在高U胁迫下促进植物生长。
    Sunflower (Helianthus annuus) can potentially be used for uranium (U) phytoremediation. However, the factors influencing the absorption of U and its subsequent distribution within plant tissues remain unclear, including the effect of silicon (Si) which is known to increase metal tolerance. Here, using hydroponics, the effect of Si on the distribution and speciation of U in sunflower was examined using synchrotron-based X-ray fluorescence and fluorescence-X-ray absorption near-edge spectroscopy. It was found that ∼88 % of U accumulates within the root regardless of treatments. Without the addition of Si, most of the U appeared to bind to epidermis within the roots, whereas in the leaves, U primarily accumulated in the veins. The addition of Si alleviated U phytotoxicity and decreased U concentration in sunflower by an average of 60 %. In the roots, Si enhanced U distribution in cell walls and impeded its entry into cells, likely due to increased callose deposition. In the leaves, Si induced the sequestration of U in trichomes. However, Si did not alter U speciation and U remained in the hexavalent form. These results provide information on U accumulation and distribution within sunflower, and suggest that Si could enhance plant growth under high U stress.
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  • 文章类型: Journal Article
    水生生态系统中的铀污染对生物构成了威胁。然而,铀沿水生食物链的代谢和毒性仍然未知。这里,我们建立了一个人工水生生态系统,以研究铀沿食物链的命运并揭示其潜在的毒性。结果表明,铀对藻类的毒性具有剂量和时间依赖性,导致细胞变形并阻碍细胞增殖。当接触铀的藻类被鱼摄取时,铀往往集中在鱼的肠道系统和骨骼中。相对而言,直接的水铀暴露导致了铀在头部的显着积累,皮肤,和鱼的肌肉,表明不同的毒性取决于不同的暴露途径。与直接接触水相比,高水平的铀污染(20mgL-1)通过食物摄入加剧了对鱼类的毒性。它还显示,在藻类和鱼类中积累期间,大约25%和20%的U(VI)被还原为低价形式,分别,和超过10%的U(IV,VI)最终转换为U(0),由于较低的溶解度和生物利用度,因此减轻了铀的毒性。总的来说,这项研究为铀在水生食物链中的命运提供了新的见解,并强调了与消费受铀污染的水产品相关的风险。
    Uranium pollution in aquatic ecosystems poses a threat to organisms. However, the metabolism and toxicity of uranium along aquatic food chains remain unknown. Here, we established an artificial aquatic ecosystem to investigate the fate of uranium along the food chain and reveal its potential toxicity. The results displayed a dose- and time-dependent toxicity of uranium on algae, leading to cell deformation and impeding cell proliferation. When uranium-exposed algae are ingested by fish, uranium tends to concentrate in the intestinal system and bones of fish. Comparatively, direct water uranium exposure resulted in a remarkable uranium accumulation in the head, skin, and muscles of fish, suggesting different toxicity depending on distinct exposure pathways. High-level uranium pollution (20 mg L-1) intensifies the toxicity to fish through food intake compared to direct water exposure. It has also revealed that approximately 25 % and 20 % of U(VI) were reduced to lower valence forms during its accumulation in algae and fish, respectively, and over 10 % of U(IV, VI) converted to U(0) ultimately, through which uranium toxicity was mitigated due to the lower solubility and bioavailability. Overall, this study provides new insights into the fate of uranium during its delivery along the aquatic food chain and highlights the risks associated with consuming uranium-contaminated aquatic products.
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  • 文章类型: Journal Article
    Jackpile矿井的地表水和沉积物,圣安东尼矿,RioPaguate,里约·莫基诺,和拉古纳普韦布洛附近的梅西塔水坝地区,新墨西哥州,使用γ(γ)光谱和电感耦合等离子体质谱分析226Ra和U,分别。固体样品的226Ra/238U的活度比范围为0.34±0.13至16±2.9,反映了铀的运输和积累(<1),处于长期平衡状态的相对原始的材料(1),和通过风化作用去除铀(>1)。在Jackpile矿附近未过滤的水样中检测到80至225μgL-1U的浓度。矿山上游和下游的水样浓度范围为12至15μgL-1U。从夹头矿山的北坑站立池塘收集的水样中含有多达1560pCiL-1的226Ra,并且使水通过0.2μM过滤器基本上没有降低水中226Ra的活性。234Th和226Ra在该水中处于长期平衡状态,而氡气从水中流失。当前研究的结果提供了对拉古纳地区普韦布洛地区U系列放射性核素分布的见解,包括在Jackpile矿井内的某些位置检测到水中的高放射性水平。
    Surface water and sediments from the Jackpile mine, St. Anthony mine, Rio Paguate, Rio Moquino, and Mesita Dam areas near Pueblo of Laguna, New Mexico, were analyzed for 226Ra and U using gamma (γ) spectroscopy and inductively coupled plasma mass spectroscopy, respectively. Activity ratios for 226Ra/238U for solid samples range from 0.34 ± 0.13 to 16 ± 2.9, which reflect uranium transport and accumulation (<1), relatively pristine material in secular equilibrium (1), and removal of uranium by weathering (>1). Concentrations ranging from 80 to 225 μg L-1 U were detected in unfiltered water samples near the Jackpile mine. Water samples upstream and downstream from the mine contained concentrations ranging from 12 to 15 μg L-1 U. Water samples collected from the North Pit standing pond in the Jackpile mine contained as much as 1560 pCi L-1 of 226Ra, and passing the water through a 0.2 μM filter did not substantially reduce the activity of 226Ra in the water. 234Th and 226Ra are in secular equilibrium in this water, while radon gas was lost from the water. The results of the current study provide insight into the distribution of U-series radionuclides in the Pueblo of Laguna area, including detection of high levels of radioactivity in water at some locations within the Jackpile mine.
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  • 文章类型: Journal Article
    这项研究提供了刚果共和国沿海生态系统沉积物中天然放射性元素水平的第一批数据。收集了来自五个沿海地点的沉积物样品,并通过高分辨率伽马光谱法进行了分析,以确定长寿命的发射伽马的放射性核素的活性(234Th,238U,226Ra,210Pb,228Th,228Ra,和40K)。具体活动与刚果共和国附近大多数国家的沉积物中测量的活动具有相同的数量级。然而,从一个地点到另一个地点以及从同一地点的一个采样点到另一个采样点观察到活动的变化,而没有超过全球平均参考值。可以假设,因此,在研究区域中没有明显的人为影响。最常用的放射性危害参数,主要基于238U,232Th,和40K活动,进行了评估,并应用了ERICA工具来量化沉积物中放射性核素对人类和生物群的辐射暴露负担。除了对未来的监测工作有用之外,这项工作中产生的数据对于全球海洋放射性数据库(MARIS)可能很重要,因为在刚果海洋环境中没有可用的数据。
    This study presents the first data on levels of natural radioactive elements in sediments from coastal ecosystems of the Republic of Congo. Sediment samples from five coastal sites were collected and analyzed by high-resolution gamma spectrometry for determination of activities of long-lived gamma-emitting radionuclides (234Th, 238U, 226Ra, 210Pb, 228Th, 228Ra, and 40 K). The specific activities were of the same order of magnitude as those measured in sediments of most countries neighboring the Republic of Congo. However, variations in activities were observed from one site to another and also from one sampling point to another within the same site without exceeding the global average reference values. It can be assumed, therefore, that no significant anthropogenic impact is perceptible in the study area. The most commonly used radiological hazard parameters, based mainly on 238U, 232Th, and 40 K activities, were assessed and the ERICA tool was applied to quantify the radiation exposure burden to human and biota resulting from radionuclides in sediments. Besides being useful for future monitoring efforts, the data produced in this work could be important for the worldwide database on radioactivity in the oceans and seas (MARIS) since no data are available in the Congolese marine environment.
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  • 文章类型: Journal Article
    铀是核电运行最重要的燃料,其资源的安全供应是我国核电发展的关键。由于海水环境复杂,铀浓度极低,从天然海水中提取铀构成了重大挑战。在这项研究中,制备了聚酰胺肟-磷酸化纤维素纳米原纤维复合气凝胶,作为从海水中提取铀的吸附剂。吸附动力学试验,平衡吸附等温线模型拟合,吸附-解吸循环试验,并进行了选择性测试,以评估复合气凝胶对铀萃取的吸附性能。在掺铀的纯水中初始浓度为4和8ppm的吸附能力分别为96.9和204.3mg-U/g-Ads,分别。铀掺杂模拟海水的平衡铀吸附能力分别为38.9和51.7mg-U/g-Ads,分别。铀的分配系数KD计算为2.5×107mL/g。结果表明,本研究制备的聚胺肟-磷酸化纤维素纳米纤维复合气凝胶具有低成本和高铀选择性的优点,用于从海水中提取铀。
    Uranium is the most important fuel for nuclear power operations, and the safe supply of its resources is the key to the development of nuclear power in China. Because of the complex seawater environment and extremely low uranium concentration, extracting uranium from natural seawater poses a significant challenge. In this study, a polyamidoxime-phosphorylated cellulose nanofibril composite aerogel was prepared as an adsorbent for uranium extraction from seawater. An adsorption kinetics test, equilibrium adsorption isotherm model fitting, an adsorption-desorption cycle test, and a selectivity test were carried out to evaluate the adsorption performance of the composite aerogel for uranium extraction. The adsorption capacities for the initial concentrations of 4 and 8 ppm in uranium-spiked pure water were 96.9 and 204.3 mg-U/g-Ads, respectively. The equilibrium uranium adsorption capacities of uranium-spiked simulated seawater were 38.9 and 51.7 mg-U/g-Ads, respectively. The distribution coefficient KD of uranium was calculated to be 2.5 × 107 mL/g. The results show that the polyamidoxime-phosphorylated cellulose nanofiber composite aerogels prepared in this study have the advantages of low cost and high uranium selectivity for uranium extraction from seawater.
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  • 文章类型: Journal Article
    石墨氮化碳(CN)作为吸附剂显示出去除水中铀的潜力。然而,活性位点的缺乏严重制约了其实际应用。与传统的引入新配体的方法相反,我们提出了一种通过注入π电子来激活CN上的原始配体的策略,这可以通过在CN(PCN)上接枝4-苯氧基苯酚(PP)来实现。与CN相比,PCN对铀的最大吸附量从150.9mg/g增加到380.6mg/g。此外,PCN在较宽的铀浓度(1~60mg/L)和pH值(4~8)范围内保持良好的吸附性能。连续5个周期后,PCN表现出持续的除铀性能,但损失很小。实验和理论结果表明,吸附性能的增强主要是由于配体通过π电子与PP的离域激活了CN。此外,这种激活可以通过辐照来增强,因为CN可以被光激发以为PP提供额外的光电子。因此,休眠配体如N-CN,C-O-C,C-N-H和N-(C)3可活化参与与铀的配位。该工作为高效铀吸附剂的设计和制备提供了理论指导。
    Graphitic carbon nitride (CN) as an adsorbent exhibit promising potential for the removal of uranium in water. However, the lack of active sites seriously restricts its practical application. In contrast to the traditional method of introducing new ligands, we propose a strategy to activate original ligands on CN by injecting π electrons, which can be realized by grafting 4-phenoxyphenol (PP) on CN (PCN). Compared with CN, the maximum adsorption capacity of PCN for uranium increased from 150.9 mg/g to 380.6 mg/g. Furthermore, PCN maintains good adsorption properties over a wide range of uranium concentrations (1 ∼ 60 mg/L) and pH (4 ∼ 8). After 5 consecutive cycles, PCN exhibited sustained uranium removal performance with a little of losses. The experimental and theoretical results show that the enhancement of adsorption performance is mainly due to the ligands activation of CN by delocalization of π electrons from PP. Furthermore, this activation can be enhanced by irradiation, as the CN can be photoexcited to provide additional photoelectrons for PP. As a result, dormant ligands such as N-CN, C-O-C, C-N-H and N-(C)3 can be activated to participate in coordination with uranium. This work provides theoretical guidance for the design and preparation of high efficiency uranium adsorbent.
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  • 文章类型: Journal Article
    在本文中,我们报道了来自蛋壳生物的羟基磷灰石,嵌入在二乙醇酸官能化石墨碳氮化物纳米复合材料(缩写为HAp@D-gCN)上。HAp@D-gCN的组成和形态特征用扫描电子显微镜进行了评价,X射线衍射,BET,FTIR技巧和表面电荷运用zeta电位丈量。通过分批研究研究了U(VI)物种在HAp@D-gCN上的吸附作为pH的函数,接触时间,初始U(VI)浓度,吸附剂用量和离子强度。通过FTIR证实了U(VI)在HAp@D-gCN上的吸附,XRD和EDS元素作图。吸附动力学遵循伪二阶模型,并在20分钟内达到平衡。吸附等温线数据与Langmuir等温线模型密切相关,在298K时的最大吸附容量为993.06mgg-1。可以使用0.01MNa2CO3作为解吸剂从负载的吸附剂中浸出U(VI),即使经过4次吸附-解吸循环,其吸附能力也不受影响。因此,本研究表明,HAp@D-gCN纳米复合材料可以作为一种环境友好材料,在环境修复中具有潜在的应用前景。
    In this paper, we report hydroxyapatite derived from egg-shell biowaste embedded on diglycolamic acid functionalized graphitic carbon nitride nanocomposite (abbreviated as HAp@D-gCN). The compositional and morphological characteristics of HAp@D-gCN were evaluated using scanning electron microscope, X-ray diffraction, BET, FTIR techniques and surface charge using zeta potential measurement. The sorption of U(VI) species on HAp@D-gCN was investigated through batch studies as a function of pH, contact time, initial U(VI) concentration, adsorbent dosage and ionic strength. The adsorption of U(VI) onto HAp@D-gCN was confirmed by FTIR, XRD and EDS elemental mapping. Adsorption kinetics follow pseudo second order model and it attains equilibrium within 20 min. Adsorption isotherm data correlates well with Langmuir isotherm model with a maximum sorption capacity of 993.6 mg of U(VI) per gram of HAp@D-gCN at 298K. U(VI) can be leached from the loaded adsorbent using 0.01 M Na2CO3 as desorbing agent and its sorption capacity remains unaffected even after 4 adsorption-desorption cycles. Hence, the present study reveals that HAp@D-gCN nanocomposite could serve as an environmental friendly material with potential application in environmental remediation.
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  • 文章类型: Journal Article
    提出了一种快速原位合成电致变色共价有机骨架(EC-COFs)的绿色电化学界面聚合方法,N,N\',N-四(对氨基苯基)对苯二胺(TPDA)和2,5-二羟基对亚苯基二甲醛(DHBD)。合成的TPDA-DHBD薄膜在不同的施加电势下表现出稳定的多晶型颜色变化,这可以归因于COFs骨架内双(三苯胺)和亚胺电活性官能团的氧化还原态变化。由于UO22+的存在引起的空间位阻效应,TPDA-DHBD代表从红色到青色明显不同的电致变色,展示了COFs材料的独特可调性。这项工作为EC-COFs的快速合成和可调谐EC-COFs的实现提供了新的可行思路。
    A rapid in situ synthesis of electrochromic covalent organic frameworks (EC-COFs) was proposed by using green electrochemical interface polymerization of N,N,N\',N\'-tetrakis(p-aminophenyl)p-phenylenediamine (TPDA) and 2,5-dihydroxy-p-phenylenedicarboxaldehyde (DHBD). The synthetized TPDA-DHBD films exhibit stable polymorphic colour variations under different applied potentials, which can be attributed to the redox state changes of bis(triphenylamine) and imine electroactive functional groups within the COFs skeleton. TPDA-DHBD represents markedly different electrochromisms from red to cyan due to the steric hindrance effect caused by the presence of UO22+, demonstrating the unique tunability of COFs materials. This work offers a new feasible idea for rapid EC-COFs synthesis and tunable EC-COFs realization.
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  • 文章类型: Journal Article
    光催化已成为处理含铀废水的极有前途的绿色技术。本研究的重点是通过在Ti3C2Tx纳米片上原位生长Cd0.8Zn0.2S,制备具有肖特基结的Ti3C2Tx/Cd0.8Zn0.2S复合材料,无需牺牲剂即可实现U(VI)的有效光还原。结果表明,在100ppm铀溶液中,Ti3C2Tx/Cd0.8Zn0.2S复合材料在60分钟内可实现显着的99.48%U(VI)还原效率。此外,5次循环后去除率保持在90%以上。Ti3C2Tx和Cd0.8Zn0.2S形成肖特基异质结导致内部电场的产生,显著促进光生载流子的快速分离和转移,从而提高Ti3C2Tx/Cd0.8Zn0.2S-3:100(TC/CZS-3:100)的光催化还原效率。相当数量的电子通过肖特基势垒积聚在Ti3C2Tx上,有效促进U(VI)降低到U(IV)。作为助催化剂,Ti3C2Tx增强Cd0.8Zn0.2S的光催化性能和稳定性。此外,在稀土尾矿废液中的实际应用表明,去除率可高达91.24%。这项研究对于开发有效的光催化剂以消除废水中的铀具有重要价值。
    Photocatalysis has emerged as a extremely promising green technology for the treatment of uranium-containing wastewater. This study focuses on the fabrication of Ti3C2Tx/Cd0.8Zn0.2S composites with Schottky junctions through the in-situ growth of Cd0.8Zn0.2S on Ti3C2Tx nanosheets, enabling efficient photoreduction of U(VI) without the requirement of sacrificial agents. The results demonstrate that the Ti3C2Tx/Cd0.8Zn0.2S composites achieve remarkable 99.48 % U(VI) reduction efficiency within 60 min in a 100 ppm uranium solution. Furthermore, the removal rate remains above 90 % after five cycles. The formation of Schottky heterojunctions by Ti3C2Tx and Cd0.8Zn0.2S leads to the generation of an internal electric field that significantly promotes the rapid separation and transfer of photogenerated carriers, thereby enhancing the photocatalytic reduction efficiency of Ti3C2Tx/Cd0.8Zn0.2S-3:100 (TC/CZS-3:100). A considerable amount of electrons accumulate on Ti3C2Tx via the Schottky barrier, effectively facilitating the reduction of U(VI) to U(IV). As a co-catalyst, Ti3C2Tx enhances the photocatalytic performance and stability of Cd0.8Zn0.2S. Moreover, the practical application in the waste liquid of rare earth tailings reveals that the removal rate can be as high as 91.24 %. This research is of significant value in the development of effective photocatalysts for the elimination of uranium from wastewater.
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