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Interaction studies between U-Zr alloy system and ceramic plasma-spray coated layer at elevated temperature 高温下U-Zr合金体系与陶瓷等离子喷涂层的相互作用研究
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.192
Ki-hwan Kim, Ki-Won Hong, H. Song, S. Oh, J. Park
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引用次数: 0
Sorption parameter setting approaches for radioactive waste disposal considering perturbation effects: sorption reduction factors for organics 考虑扰动效应的放射性废物处理的吸附参数设置方法:有机物的吸附还原因子
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.229
Y. Tachi, M. Ochs
Various types of post-accident radioactive waste have been generated from cleanup and decommissioning activities at the Fukushima Daiichi nuclear power plant. Perturbation effects resulting from co-existing substances may influence radionuclide sorption. For the disposal of these wastes, perturbation effects on sorption parameters must be critically evaluated for the safety assessment of the disposal systems. The present study focuses on developing a methodology to quantify sorption parameters in the presence of such perturbation effects and on illustrating example calculations regarding sorption reduction factors (SRFs) due to the presence of organic ligands (ISA; isosaccharinic acid) for cement systems. Three approaches for the derivation of SRFs; 1) semi-quantitative estimation based on analogy with solubility enhancement factors (SEFs) derived from measured solubility, 2) prediction based on radionuclide speciation calculation, and 3) quantification from experimental sorption data in ternary systems were coupled and tested for the Am-ISA-cement system. Our approach allows to critically evaluate the dependence of sorption reduction factors for various perturbed systems on the chosen method of quantification, in accordance with the data availability for a given perturbation.
福岛第一核电站的清理和退役活动产生了各种类型的事故后放射性废物。共存物质引起的扰动效应可能影响放射性核素的吸收。对于这些废物的处置,必须严格评估摄动对吸附参数的影响,以便对处置系统进行安全评估。本研究的重点是开发一种方法来量化存在这种扰动效应的吸附参数,并举例说明由于有机配体的存在而导致的吸附减少因子(srf)的计算。异糖酸)用于水泥体系。srf的三种推导方法1)基于溶解度增强因子(SEFs)类比的半定量估计,2)基于放射性核素形态计算的预测,以及3)基于三元体系中实验吸附数据的定量预测,对am - isa -水泥体系进行了耦合和测试。我们的方法允许根据给定扰动的数据可用性,批判性地评估各种摄动系统的吸收减少因子对所选择的量化方法的依赖性。
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引用次数: 3
Characteristics of TPDN/SiO2-P adsorbent for MA(III) recovery TPDN/SiO2-P吸附剂回收MA(III)的特性
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.61
H. Kofuji, Sou Watanabe, M. Takeuchi, Hideya Suzuki, T. Matsumura, H. Shiwaku, T. Yaita
Characteristics of TPDN/SiO2-P adsorbent for MA(III) recovery Hirohide Kofuji, Sou Watanabe, Masayuki Takeuchi, Hideya Suzuki, Tatsuro Matsumura, Hideaki Shiwaku and Tsuyoshi Yaita Japan Atomic Energy Agency, 4-33 Muramatsu, Tokai-mura, Naka-gun, Ibaraki-pref., 319-1194, Japan; Japan Atomic Energy Agency,. Shirakata, Tokai-mura, Naka-gun, Ibaraki-pref., 319-1195, Japan; Japan Atomic Energy Agency, 1-1-1, Kouto, Sayo-cho, Sayo-gun, Hyogo-pref., 679-5148, Japan
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引用次数: 3
A first-principles study on point defects in plutonium dioxide 二氧化钚点缺陷的第一性原理研究
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.132
Hiroki Nakamura, M. Machida
Plutonium dioxide is one of the main components of nuclear fuels. In this paper, we evaluated formation energies of charged vacancies and site-interstitial atoms in plutonium dioxide based on density functional theory with spin-orbit coupling and strongly-correlated electron effect using LDA+U method. We also estimated migration energies of oxygen defects. We found that oxygen vacancies with double positive charge and interstitials with double negative charge are the most stable and that the calculated migration energy of an oxygen vacancy is comparable with that of an oxygen interstitial.
二氧化钚是核燃料的主要成分之一。基于自旋轨道耦合和强相关电子效应的密度泛函理论,利用LDA+U方法对二氧化钚中带电空位原子和位隙原子的形成能进行了评价。我们还估计了氧缺陷的迁移能。我们发现带双正电荷的氧空位和带双负电荷的氧空位是最稳定的,并且计算的氧空位的迁移能与氧空位的迁移能相当。
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引用次数: 2
A study of cerium extraction kinetics by TODGA in acidified and non-acidified organic solvent phases in the context of fission product management 裂变产物管理下酸化和非酸化有机溶剂相萃取铈动力学的TODGA研究
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.70
Michael A. Bromley, C. Boxall
In the context of management of the waste streams arising from the reprocessing of spent nuclear fuel, studies have been conducted into the solvent extraction kinetics of lanthanide fission products by the oxygen-donor ligand N,N,N’,N’-tetraoctyl diglycolamide (TODGA) and the effects of solvent phase acidity on the effectiveness of this organic extractant molecule. In this study, we observe a reduction in the rate of cerium extraction as solvent phase acidity increases, attributed to aggregation of the extractant. The effect is shown to be reversible through neutralization while a permanent prevention method is the subject of further work.
在乏燃料后处理产生的废物流管理的背景下,研究了氧供体配体N,N,N ',N ' -四烷基二醇酰胺(TODGA)对镧系裂变产物的溶剂萃取动力学以及溶剂相酸度对该有机萃取剂分子有效性的影响。在本研究中,我们观察到随着溶剂相酸度的增加,由于萃取剂的聚集,铈萃取率降低。这种影响通过中和是可逆的,而永久性的预防方法是进一步工作的主题。
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引用次数: 2
Chemical state analysis of simulated corium debris by EXAFS 用EXAFS分析模拟堆芯碎片的化学状态
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.200
Y. Okamoto, M. Takano
The chemical state of uranium, zirconium, iron and lanthanide elements in simulated corium debris samples prepared in lab-scale were investigated by synchrotron radiation based extended X-ray absorption fine structure (EXFAS) technique. According to the EXAFS analysis of uranium, their most likely local structure was cubic like fluorite UO2. Exceptionally, pentavalent uranium was observed in the UO2-ZrO2-Fe2O3-CaO sample, in which the nearest U-O distance was clearly shorter than those of other samples containing tetravalent uranium. The local structure around zirconium could be classified into cubic, tetragonal and calcia stabilized zirconia with CaO. The oxidation state of iron was divalent for the most samples and a metallic phase was also detected in some of them. The small amount lanthanide elements (Nd and Gd) in the simulated debris seem to exist as a solid solution with UO2.
采用同步辐射扩展x射线吸收精细结构(EXFAS)技术研究了模拟堆芯碎片样品中铀、锆、铁和镧系元素的化学状态。根据铀的EXAFS分析,它们最可能的局部结构是立方状的萤石UO2。特别的是,在UO2-ZrO2-Fe2O3-CaO样品中发现了五价铀,其中U-O距离的最近距离明显短于其他含四价铀样品。氧化锆周围的局部结构可分为立方体、四边形和钙稳定氧化锆。大多数样品的铁的氧化态为二价,在一些样品中还检测到金属相。模拟碎屑中微量的镧系元素(Nd和Gd)似乎与UO2以固溶体形式存在。
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引用次数: 4
Retention of uranium in cement systems: effects of cement degradation and complexing ligands 铀在水泥体系中的保留:水泥降解和络合配体的影响
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.208
M. Ochs, B. Vriens, Y. Tachi
The clean-up activities related to the accident at the Fukushima nuclear power plant give rise to several types of wastes containing cementitious materials as well as substances that can influence radionuclide migration, especially organic complexing substances, boron, and chloride salts. The present study focuses on a methodology, based on available literature information, for quantifying the retention behavior of uranium (VI) in cement materials of different degradation states and in the presence of organics, boron, and salts. To account for the many variables defining uranium uptake in cement systems a stepwise approach is proposed and illustrated: 1) definition of conditions and U speciation in each relevant degradation state, 2) assessment of U(VI) uptake processes based on a critical review of literature information, 3) Kd setting on the basis of original experimental data that are consistent with the identified processes and speciation, 4) assessment of ligand effects based on data preferably from ternary systems, or from speciation and analogue information.
与福岛核电站事故有关的清理活动产生了几种含有胶凝物质以及可能影响放射性核素迁移的物质的废物,特别是有机络合物质、硼和氯盐。本研究的重点是一种方法,基于现有的文献信息,用于量化铀(VI)在不同降解状态的水泥材料中以及在有机物、硼和盐的存在下的保留行为。为了解释水泥系统中确定铀吸收率的许多变量,提出并说明了一种逐步方法:1)定义每个相关降解状态下的条件和U形态;2)基于文献信息的批判性回顾评估U(VI)摄取过程;3)基于与所识别的过程和物种形成一致的原始实验数据设置Kd; 4)基于最好来自三元体系的数据或来自物种形成和模拟信息的配体效应评估。
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引用次数: 6
The discovery of element 117 (INVITED) 117号元素的发现(特邀)
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.14
J. Roberto
In November 2016, four new chemical elements, nihonium (Nh, Z=113), moscovium (Mc, Z=115), tennessine (Ts, Z=117), and oganesson (Og, Z=118) joined the periodic table. Elements 117 and 118 are the highest atomic numbers Z reached to date, and the A=294 isotopes of these elements are the heaviest nuclei ever synthesized. The existence of these elements, together with a consistent trend of increasing lifetimes for superheavy isotopes as neutron number N increases, provide strong evidence for the long sought “island of stability” for superheavy nuclei as the nuclear shell closure at N=184 is approached. Mc, Ts, and Og were discovered using the hot fusion process, bombarding actinide targets with intense beams of doubly-magic Ca ions at the Dubna Gas-Filled Recoil Separator at the Joint Institute for Nuclear Research in Russia. For element 117, a berkelium target from Oak Ridge National Laboratory (ORNL) was required. The berkelium was produced by intense neutron irradiation at ORNL’s High Flux Isotope Reactor and chemically separated at the adjoining Radiochemical Engineering Development Center. The Bk + Ca reaction produced two isotopes of element 117 with atomic weights A=293 and 294. These isotopes decayed into ten additional heaviest isotopes of elements 115, 113, 111, 109, 107, and 105, all closer to the predicted island of stability than previously achieved. The discovery of element 117 will be described together with results of other recent experiments in superheavy element research in the context of the critical importance of actinide target materials, implications for the periodic table and the island of stability, and opportunities to synthesize even heavier nuclei, including heavy isotopes of element 118 and new elements 119 and 120.
2016年11月,四种新的化学元素nihonium (Nh, Z=113)、moscovium (Mc, Z=115)、tennessine (Ts, Z=117)和oganesson (Og, Z=118)加入了元素周期表。元素117和118是迄今为止Z达到的最高原子序数,而这些元素的A=294同位素是迄今为止合成的最重的原子核。这些元素的存在,以及随着中子数N的增加,超重同位素寿命持续增加的趋势,为超重核在N=184处接近核壳闭合时寻求已久的“稳定岛”提供了强有力的证据。Mc、Ts和Og是在俄罗斯联合核研究所的杜布纳气体填充反冲分离器上,利用热聚变过程用强束双重神奇的Ca离子轰击锕系元素目标时发现的。对于117号元素,需要一个来自橡树岭国家实验室(ORNL)的锫靶。这些锫是在ORNL的高通量同位素反应堆中通过强中子辐照产生的,并在毗邻的放射化学工程开发中心进行化学分离。Bk + Ca反应产生117号元素的两种同位素,原子量分别为A=293和294。这些同位素衰变为元素115、113、111、109、107和105的另外10个最重的同位素,它们都比以前所预测的稳定岛更接近。117号元素的发现将与最近超重元素研究中其他实验的结果一起在锕系元素靶材料的关键重要性,对元素周期表和稳定岛的影响,以及合成更重原子核的机会的背景下进行描述,包括118号元素的重同位素和新元素119和120。
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引用次数: 0
Nitrous acid-driven reduction of vanadium as a neptunium analogue 硝酸驱动的钒作为镎类似物的还原
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.37
M. Chimes, C. Boxall, S. Edwards, M. Sarsfield, R. Taylor, D. Woodhead
Neptunium has been previously shown to present challenges within a used nuclear fuel reprocessing scheme due to its tendency to exist in the (IV), (V), and (VI) oxidation states simultaneously. In order to control this neptunium speciation, and informed by relevant work in the literature, we are currently engaged in a study of nitric/nitrous acid redox chemistry with Np(V) and Np(VI). To minimize radiological exposure risks, we are also exploring the validity of using vanadium as an analogue for the study of the kinetics of the Np(VI)/Np(V) reduction by nitrous acid. The kinetics of the reduction of vanadium(V) by nitrous acid in solutions of nitric acid was investigated spectrophotometrically by the method of initial rates. Orders of reaction with respect to V(V), and HNO2 were found to be 0.90, and 1.24 respectively, in reasonable agreement with the analogous reaction orders for the reduction of Np(VI) by nitrous acid previously reported by Precek and Paulenova – suggesting that, for this particular reduction, V(V) can serve as a good kinetic analogue for Np(VI). The value of the rate constant k for the rate law -d[V(V)]/dt = k[V(V)][HNO2]/[H] was found to be 7.5 × 10 M s at 20 °C, two orders of magnitude smaller than that for the reduction of Np(VI) by HNO2, a difference that is attributable to the loss of one of the oxygens during the VO2 to VO reduction reaction.
由于镎倾向于同时以(IV)、(V)和(VI)氧化态存在,先前已证明在乏燃料后处理方案中存在挑战。为了控制这种镎的形态,并根据文献相关工作,我们目前正在研究Np(V)和Np(VI)对硝酸/亚硝酸氧化还原化学的影响。为了最大限度地降低辐射暴露风险,我们也在探索使用钒作为亚硝酸还原Np(VI)/Np(V)动力学研究的类似物的有效性。用初始速率法研究了硝酸溶液中硝酸还原钒的动力学。V(V)和HNO2的反应阶数分别为0.90和1.24,与preprek和Paulenova先前报道的硝酸还原Np(VI)的类似反应阶数基本一致,这表明,对于这种特殊的还原,V(V)可以作为Np(VI)的良好动力学类似物。在20℃时,速率定律-d[V(V)]/dt = k[V(V)][HNO2]/[H]的速率常数k值为7.5 × 10 M s,比HNO2还原Np(VI)的速率常数小两个数量级,这是由于在VO2还原成VO的反应中损失了一个氧所致。
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引用次数: 1
Magnetization study on the ising ferromagnet URhGe with high-precision angle-resolved magnetic field near the hard axis 硬轴附近高精度角分辨磁场的超强铁磁体的磁化研究
Pub Date : 2018-11-01 DOI: 10.15669/PNST.5.123
S. Nakamura, T. Sakakibara, Y. Shimizu, S. Kittaka, Y. Kono, Y. Haga, J. Pospíšil, E. Yamamoto
Shota Nakamura, Toshiro Sakakibara, Yusei Shimizu, Shunichiro Kittaka, Yohei Kono, Yoshinori Haga, Jiří Pospíšil and Etsuji Yamamoto Institute for Solid State Physics, The University of Tokyo, Kashiwa 277-8581, Japan; Institute for Materials Research, Tohoku University, Oarai 311-1313, Japan; Japan Atomic Energy Agency, Tokai 319-1106, Japan; Charles University in Prague, Faculty of Mathematics and Physics, DCMP, Ke Karlovu 5, 121 16 Prague 2, Czech Republic
中村正太,坂原敏郎,清水佑成,北孝一弘,河野洋平,长贺义德,Jiří Pospíšil,东京大学固体物理研究所山本越司,日本柏华277-8581;东北大学材料研究所,日本大原311-1313;日本原子能机构,日本东海319-1106;布拉格查尔斯大学,数学与物理学院,DCMP, Ke Karlovu 5, 121 16布拉格2,捷克共和国
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引用次数: 1
期刊
Progress in Nuclear Science and Technology
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