首页 > 最新文献

Journal of nuclear and radiochemical sciences最新文献

英文 中文
Uptake of 131I, 134Cs and 137Cs in tulip (Tulipa gesneriana L.) after the Fukushima Daiichi nuclear accident and their translocation from its above ground parts to the bulb 福岛核事故后郁金香(Tulipa generiana L.)对131I、134Cs和137Cs的吸收及其从地上部分向鳞茎的转运
Pub Date : 2022-01-01 DOI: 10.14494/jnrs.22.1
K. Tagami, S. Uchida, Y. Uchihori, H. Kitamura
{"title":"Uptake of 131I, 134Cs and 137Cs in tulip (Tulipa gesneriana L.) after the Fukushima Daiichi nuclear accident and their translocation from its above ground parts to the bulb","authors":"K. Tagami, S. Uchida, Y. Uchihori, H. Kitamura","doi":"10.14494/jnrs.22.1","DOIUrl":"https://doi.org/10.14494/jnrs.22.1","url":null,"abstract":"","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"81197212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Physical and adsorption characteristics of geopolymers prepared using 1–5 M NaOH solution for immobilization of radioactive wastes 用1-5 M NaOH溶液制备的地聚合物固定放射性废物的物理和吸附特性
Pub Date : 2022-01-01 DOI: 10.14494/jnrs.22.7
N. Kinoshita, Yuya Yoda, H. Nakashima, M. Asada, Shunsuke Kiyomura, Yuki Sasaki, K. Torii, K. Sueki
{"title":"Physical and adsorption characteristics of geopolymers prepared using 1–5 M NaOH solution for immobilization of radioactive wastes","authors":"N. Kinoshita, Yuya Yoda, H. Nakashima, M. Asada, Shunsuke Kiyomura, Yuki Sasaki, K. Torii, K. Sueki","doi":"10.14494/jnrs.22.7","DOIUrl":"https://doi.org/10.14494/jnrs.22.7","url":null,"abstract":"","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"7 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"82206988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Isothermal gas chromatography study of Zr and Hf tetrachlorides using radiotracers of 88Zr and 175Hf 用放射性示踪剂88Zr和175Hf等温气相色谱法研究四氯化锆和四氯化铪
Pub Date : 2021-01-01 DOI: 10.14494/jnrs.21.7
K. Shirai, S. Goto, K. Ooe, H. Kudo
{"title":"Isothermal gas chromatography study of Zr and Hf tetrachlorides using radiotracers of 88Zr and 175Hf","authors":"K. Shirai, S. Goto, K. Ooe, H. Kudo","doi":"10.14494/jnrs.21.7","DOIUrl":"https://doi.org/10.14494/jnrs.21.7","url":null,"abstract":"","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"467 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"77033706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Phase transformation of mixed lanthanide oxides in an aqueous solution 混合镧系氧化物在水溶液中的相变
Pub Date : 2021-01-01 DOI: 10.14494/jnrs.21.15
M. Moniruzzaman, Taishi Kobayashi, T. Sasaki
{"title":"Phase transformation of mixed lanthanide oxides in an aqueous solution","authors":"M. Moniruzzaman, Taishi Kobayashi, T. Sasaki","doi":"10.14494/jnrs.21.15","DOIUrl":"https://doi.org/10.14494/jnrs.21.15","url":null,"abstract":"","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"62 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89181822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sorption and desorption of radioactive organic iodine by silver doped zeolite and zeolite X 掺银沸石和X沸石对放射性有机碘的吸附与解吸
Pub Date : 2021-01-01 DOI: 10.14494/jnrs.21.1
Daisuke Akiyama, Tasuku Ishii, Yutaka Masaki, T. Narabayashi, A. Kirishima, N. Sato
{"title":"Sorption and desorption of radioactive organic iodine by silver doped zeolite and zeolite X","authors":"Daisuke Akiyama, Tasuku Ishii, Yutaka Masaki, T. Narabayashi, A. Kirishima, N. Sato","doi":"10.14494/jnrs.21.1","DOIUrl":"https://doi.org/10.14494/jnrs.21.1","url":null,"abstract":"","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2021-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"90748817","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Plutonium Isotopes Research in the Marine Environment: A synthesis 海洋环境中钚同位素研究综述
Pub Date : 2020-01-01 DOI: 10.14494/JNRS.20.1
Jinlong Wang, Jinzhou Du, Z. Jian
Plutonium (Pu), mainly derived from thermonuclear bomb testing, nuclear accidents, nuclear reprocessing facilities and nuclear power plants since the 1950s, entered the ocean by global fallout and by direct release and was then transported by ocean current, exchanged, transformed and eventually buried in the ocean. Pu in the marine environment consists mainly of four isotopes, namely,Pu (T1/2 = 87.7 a), Pu (T1/2 = 24100 a), Pu (T1/2 = 6561 a) and Pu (T1/2 = 14.3 a), in which a very small fraction of Pu originates from uranium mineral and most Pu comes f rom anth ropogenic act iv it y. Additionally, Pu has two isotopes with extremely low concentrations namely, Pu (T1/2 = 376000 a) and Pu (T1/2 = 8.7 ×10 a). The distribution of Pu concentration in the marine environment is influenced by ocean current distribution and biogeochemical cycles, and therefore, Pu isotopes are typically utilized to trace water mass exchange, particle scavenging and biogeochemical cycles. Compared to Sr (Kd: 10-10 L kg) and Cs (Kd: 10-10 L kg), Pu has a much stronger particle affinity in marine environments (Kd: 10-10 L kg) and thus can serve as a better tracer for indicating transport, scavenging and particle deposition. To use Pu as a tracer for environmental process, the geochemical behavior of Pu should be understood and the analytical method for Pu need to be improved. With the development of analytical methods for Pu, the detection limit of Pu in seawater and sediments has continuously decreased, which allows increasing numbers of researchers (Figure 1) to focus on the sources, geochemical behaviors, distribution and environmental implications. Pu fr om different sources or incidents has unique atom (or activity) ratios, e.g., Pu/Pu, Pu/Pu and Pu/Pu, and these ratios can be used to quantitatively evaluate the source of Pu and to study different marine processes along with Pu activity concentration. Therefore, this study aims to synthesize the application of Pu to marine processes based on a summary of its sources, geochemical behaviors, distribution and analytical methods.
钚(Pu)主要来源于20世纪50年代以来的热核炸弹试验、核事故、核后处理设施和核电站,通过全球沉降和直接释放进入海洋,然后被洋流运输、交换、转化,最终埋在海洋中。海洋环境中的Pu主要由4种同位素组成,分别为Pu (T1/2 = 87.7 a)、Pu (T1/2 = 24100 a)、Pu (T1/2 = 6561 a)和Pu (T1/2 = 14.3 a),其中极小部分Pu来源于铀矿物,大部分来自于人工活动。另外,Pu还有2种浓度极低的同位素,分别为:Pu (T1/2 = 376000 a)和Pu (T1/2 = 8.7 ×10 a)。海洋环境中Pu浓度的分布受洋流分布和生物地球化学循环的影响,因此通常利用Pu同位素来追踪水质交换、颗粒清除和生物地球化学循环。与Sr (Kd: 10-10 L kg)和Cs (Kd: 10-10 L kg)相比,Pu在海洋环境中具有更强的颗粒亲和力(Kd: 10-10 L kg),因此可以作为更好的示踪剂来指示运输、清除和颗粒沉积。要将蒲公英作为环境过程的示踪剂,必须了解蒲公英的地球化学行为,改进蒲公英的分析方法。随着分析方法的发展,海水和沉积物中Pu的检出限不断降低,使得越来越多的研究人员(图1)开始关注Pu的来源、地球化学行为、分布和环境影响。不同来源或事件的Pu具有独特的原子(或活度)比,如Pu/Pu、Pu/Pu和Pu/Pu,这些比可用于定量评价Pu的来源,并研究不同海洋过程随Pu活度浓度的变化。因此,本文拟在总结其来源、地球化学行为、分布及分析方法的基础上,综合探讨其在海洋过程中的应用。
{"title":"Plutonium Isotopes Research in the Marine Environment: A synthesis","authors":"Jinlong Wang, Jinzhou Du, Z. Jian","doi":"10.14494/JNRS.20.1","DOIUrl":"https://doi.org/10.14494/JNRS.20.1","url":null,"abstract":"Plutonium (Pu), mainly derived from thermonuclear bomb testing, nuclear accidents, nuclear reprocessing facilities and nuclear power plants since the 1950s, entered the ocean by global fallout and by direct release and was then transported by ocean current, exchanged, transformed and eventually buried in the ocean. Pu in the marine environment consists mainly of four isotopes, namely,Pu (T1/2 = 87.7 a), Pu (T1/2 = 24100 a), Pu (T1/2 = 6561 a) and Pu (T1/2 = 14.3 a), in which a very small fraction of Pu originates from uranium mineral and most Pu comes f rom anth ropogenic act iv it y. Additionally, Pu has two isotopes with extremely low concentrations namely, Pu (T1/2 = 376000 a) and Pu (T1/2 = 8.7 ×10 a). The distribution of Pu concentration in the marine environment is influenced by ocean current distribution and biogeochemical cycles, and therefore, Pu isotopes are typically utilized to trace water mass exchange, particle scavenging and biogeochemical cycles. Compared to Sr (Kd: 10-10 L kg) and Cs (Kd: 10-10 L kg), Pu has a much stronger particle affinity in marine environments (Kd: 10-10 L kg) and thus can serve as a better tracer for indicating transport, scavenging and particle deposition. To use Pu as a tracer for environmental process, the geochemical behavior of Pu should be understood and the analytical method for Pu need to be improved. With the development of analytical methods for Pu, the detection limit of Pu in seawater and sediments has continuously decreased, which allows increasing numbers of researchers (Figure 1) to focus on the sources, geochemical behaviors, distribution and environmental implications. Pu fr om different sources or incidents has unique atom (or activity) ratios, e.g., Pu/Pu, Pu/Pu and Pu/Pu, and these ratios can be used to quantitatively evaluate the source of Pu and to study different marine processes along with Pu activity concentration. Therefore, this study aims to synthesize the application of Pu to marine processes based on a summary of its sources, geochemical behaviors, distribution and analytical methods.","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"31 1","pages":"1-11"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73244721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 7
Liquid interfaces related to lanthanide and actinide chemistry studied using vibrational sum frequency generation spectroscopy 用振动和频率产生光谱法研究了与镧系元素和锕系元素化学相关的液体界面
Pub Date : 2020-01-01 DOI: 10.14494/JNRS.20.28
Ryoji Kusaka
Liquid interfaces, such as gas/liquid, liquid/liquid, and solid/liquid interfaces, are ubiquitous and play important roles in chemistry. For chemical reactions at interfaces, the interfacial region at a ~1-nm depth is important because this thin interfacial region corresponds to the scale of the sizes of molecules. However, it is generally difficult to observe this very thin region of liquid interfaces by conventional methods. For example, photoelectron spectroscopy requires a vacuum to detect electrons ejected from sample surfaces; thus, it is not appropriate for liquid interfaces. X -ray scattering methods are generally used to study liquid interfaces. However, high brightness X-rays are prepared by synchrotrons, and experiments for radioactive species are difficult in such facilities. Vibrational sum frequency generation (VSFG) spectroscopy is one of the vibrational spectroscopic techniques besides FT-IR and Raman spectroscopy. VSFG spectroscopy is interface-specific and offers unique information on the molecular structure in the very thin interfacial region (~1 nm) of liquid interfaces. Although many interfacial studies by VSFG spectroscopy have been published thus far, application to lanthanides and actinides has been very limited because previous studies have paid considerable attention to interface chemistry relating to light elements, such as interface chemistry in the cell membrane. Some metal complexes have been observed at air/aqueous interfaces using VSFG spectroscopy; however, there have been no reports on actinides because special techniques and facilities for the management and treatment of actinides are required. Recently, we constructed an optical experimental setup for VSFG spectroscopy in a radiation management area in the Japan Atomic Energy Agency (JAEA), enabling us to study actinide chemistry by VSFG spectroscopy. In this paper, the focus is on liquid interfaces of solvent extraction of lanthanides and actinides studied using VSFG spectroscopy. In solvent extraction [Figure 1(a)], extractants are dissolved in an organic phase, and some extractant molecules come to the liquid/liquid interface and cover the interface because of the surface activity of the extractants. Metal ions in the aqueous phase come to the interface and form complexes with extractants (ligands) to subsequently transfer to the organic phase. However, it is unknown what occurs at the interface and how water and extractant molecules are bonded to metals at the interface to transfer into the organic phase. This is because of the experimental difficulty related to the organic/aqueous interface, and one reason for the difficulty is that metal complexes at the interface transfer into the organic phase after complex formation at the interface and are difficult to observe at the interface. Therefore, we trapped metal comLiquid interfaces related to lanthanide and actinide chemistry studied using vibrational sum frequency generation spectroscopy
液体界面,如气液界面、液液界面、固液界面等,在化学中无处不在,发挥着重要作用。对于界面上的化学反应,1 ~ nm深度的界面区域是重要的,因为这个薄的界面区域对应于分子大小的尺度。然而,通常很难用常规方法观察到这种非常薄的液体界面区域。例如,光电子能谱需要真空来检测从样品表面射出的电子;因此,它不适用于液体界面。X射线散射法是研究液体界面的常用方法。然而,高亮度的x射线是由同步加速器制备的,在这样的设施中对放射性物质进行实验是困难的。振动和频产生(VSFG)光谱是除FT-IR和拉曼光谱之外的另一种振动光谱技术。VSFG光谱是界面特异性的,可以提供液体界面极薄界面区域(~ 1nm)分子结构的独特信息。虽然目前已经发表了许多利用VSFG光谱进行界面研究的文章,但由于以往的研究主要关注与轻元素有关的界面化学,例如细胞膜中的界面化学,因此在镧系元素和锕系元素界面上的应用非常有限。利用VSFG光谱在空气/水界面上观察到一些金属配合物;但是,由于管理和处理锕系元素需要特殊的技术和设施,所以没有关于锕系元素的报告。最近,我们在日本原子能机构(JAEA)的辐射管理区建立了一个VSFG光谱光学实验装置,使我们能够利用VSFG光谱研究锕系元素的化学性质。本文重点研究了溶剂萃取镧系元素和锕系元素的液相界面。在溶剂萃取中[图1(a)],萃取剂溶解在有机相中,由于萃取剂的表面活性,一些萃取剂分子到达液/液界面并覆盖界面。水相中的金属离子到达界面,与萃取剂(配体)形成配合物,随后转移到有机相。然而,目前尚不清楚界面上发生了什么,以及水和萃取剂分子如何与界面上的金属结合并转移到有机相中。这是因为与有机/水界面相关的实验困难,而困难的一个原因是界面上的金属配合物在界面上形成配合物后转移到有机相中,并且很难在界面上观察到。因此,我们利用振动和频率产生光谱技术研究了与镧系元素和锕系元素化学相关的金属共液界面
{"title":"Liquid interfaces related to lanthanide and actinide chemistry studied using vibrational sum frequency generation spectroscopy","authors":"Ryoji Kusaka","doi":"10.14494/JNRS.20.28","DOIUrl":"https://doi.org/10.14494/JNRS.20.28","url":null,"abstract":"Liquid interfaces, such as gas/liquid, liquid/liquid, and solid/liquid interfaces, are ubiquitous and play important roles in chemistry. For chemical reactions at interfaces, the interfacial region at a ~1-nm depth is important because this thin interfacial region corresponds to the scale of the sizes of molecules. However, it is generally difficult to observe this very thin region of liquid interfaces by conventional methods. For example, photoelectron spectroscopy requires a vacuum to detect electrons ejected from sample surfaces; thus, it is not appropriate for liquid interfaces. X -ray scattering methods are generally used to study liquid interfaces. However, high brightness X-rays are prepared by synchrotrons, and experiments for radioactive species are difficult in such facilities. Vibrational sum frequency generation (VSFG) spectroscopy is one of the vibrational spectroscopic techniques besides FT-IR and Raman spectroscopy. VSFG spectroscopy is interface-specific and offers unique information on the molecular structure in the very thin interfacial region (~1 nm) of liquid interfaces. Although many interfacial studies by VSFG spectroscopy have been published thus far, application to lanthanides and actinides has been very limited because previous studies have paid considerable attention to interface chemistry relating to light elements, such as interface chemistry in the cell membrane. Some metal complexes have been observed at air/aqueous interfaces using VSFG spectroscopy; however, there have been no reports on actinides because special techniques and facilities for the management and treatment of actinides are required. Recently, we constructed an optical experimental setup for VSFG spectroscopy in a radiation management area in the Japan Atomic Energy Agency (JAEA), enabling us to study actinide chemistry by VSFG spectroscopy. In this paper, the focus is on liquid interfaces of solvent extraction of lanthanides and actinides studied using VSFG spectroscopy. In solvent extraction [Figure 1(a)], extractants are dissolved in an organic phase, and some extractant molecules come to the liquid/liquid interface and cover the interface because of the surface activity of the extractants. Metal ions in the aqueous phase come to the interface and form complexes with extractants (ligands) to subsequently transfer to the organic phase. However, it is unknown what occurs at the interface and how water and extractant molecules are bonded to metals at the interface to transfer into the organic phase. This is because of the experimental difficulty related to the organic/aqueous interface, and one reason for the difficulty is that metal complexes at the interface transfer into the organic phase after complex formation at the interface and are difficult to observe at the interface. Therefore, we trapped metal comLiquid interfaces related to lanthanide and actinide chemistry studied using vibrational sum frequency generation spectroscopy","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"22 1","pages":"28-31"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"89062042","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Solubility and solid phase of trivalent lanthanide hydroxides and oxides 三价镧系氢氧化物和氧化物的溶解度和固相
Pub Date : 2020-01-01 DOI: 10.14494/JNRS.20.32
M. Moniruzzaman, Taishi Kobayashi, T. Sasaki
For the safety assessment of radioactive waste disposal, it is necessary to predict the migration behavior of actinide elements under relevant geochemical conditions, as they are included in the waste as alpha-emitting radionuclides wit h long half-lives. Actinide elements of thorium, uranium, neptunium, and plutonium can exist in a tetravalent oxidation state under reducing geochemical conditions, deep underground and easily precipitate as a sparingly soluble amorphous hydroxide solid phase (An(IV)(OH)4(am)) under neutral to alkaline pH conditions of the waste repository systems [1-4]. The solubilities of An(IV)(OH)4(am), hence, play an important role in understanding their migration behavior. It is known that a crystalline oxide solid phase as An(IV)O2(cr) is thermodynamically more stable and it has been reported that the crystallization of An(IV)(OH)4(am) towards An(IV)O2(cr) proceeded under certain solution conditions such as strong alkaline pH or elevated temperatures [5-7]. The solubilities of An(IV)O2(cr) have been reported to several orders of magnitude lower than those of An(IV)(OH)4(am) [1-7]. Trivalent actinide elements of americium and curium also exhibit a strong hydrolysis reactions under neutral to alkaline pH conditions to precipitate the sparingly soluble amorphous hydroxide solid phase (An(III)(OH)3(am)) [8-11]. In contrast to the tetravalent actinide elements, no crystalline oxide solid phase (An(III)2O3(cr)) was observed in the solubility experiments [2,12]. A few literatures have observed crystalline hydroxide solid phase (An(III)(OH)3(cr)) from X-ray diffraction patterns instead of An(III)2O3(cr) and showed an order of magnitude lower solubility values than those of An(III) (OH)3(am) [13,14]. This can be explained by thermodynamic data of An(III)2O3(cr). For example, the standard enthalpy (∆fHm°) and entropy (Sm°) of Am2O3(cr) have been reported to be ∆fHm° = −1690.4±8.0 kJ/mol and Sm° = 133.6±6.0 J/K/mol resulted in the standard formation Gibbs energy of ∆fGm° = −1605.449±8.284 [2]. Combined with the thermodynamic data for Am and H2O [2], the standard reaction Gibbs energy (∆rGm°) for 1/2 Am2O3(cr) + 3H Am + 3/2 H2O was calculated to be ∆rGm° = −151.59 kJ/mol, leading to the solubility product (Ks°) of log Ks° = 26.56. This value is approximately 10 orders of magnitude h igher than those repor ted for Am(OH)3(am) and Am(OH)3(cr) [2,4], hinting the oxide solid phase is less stable in aqueous systems. However, due to experimental limitations for handling macro amounts of trivalent actinide elements, only few studies have investigated the An(III) solubility with a definite solid phase characterization [8,11,13] and the stability of An(III)2O3(cr) in aqueous systems has not been well experimentally clarified. Trivalent lanthanide elements are often used as analogues of trivalent actinide elements. A number of literatures have investigated the hydrolysis behavior, solubilities and solid phases of lighter to heavier lanthanide el
锕系元素作为半衰期较长的α -放射性核素存在于放射性废物中,因此对放射性废物处置安全性评价有必要预测其在相关地球化学条件下的迁移行为。锕系元素钍、铀、镎和钚在还原性地球化学条件下以四价氧化态存在,在地下深处,在中性到碱性的pH条件下容易沉淀为难溶的无定形氢氧化物固相(An(IV)(OH)4(am))[1-4]。因此,An(IV)(OH)4(am)的溶解度对理解它们的迁移行为起着重要的作用。众所周知,像An(IV)O2(cr)这样的结晶氧化物固相在热力学上更稳定,有报道称,在某些溶液条件下,如强碱性pH值或高温下,An(IV)(OH)4(am)向An(IV)O2(cr)结晶[5-7]。据报道,An(IV)O2(cr)的溶解度比An(IV)(OH)4(am)的溶解度低几个数量级[1-7]。三价锕系元素镅和curium在中性到碱性的pH条件下也表现出强烈的水解反应,沉淀出难溶的无定形氢氧化物固相(An(III)(OH)3(am))[8-11]。与四价锕系元素相比,在溶解度实验中没有观察到结晶氧化物固相(An(III)2O3(cr))[2,12]。少数文献从x射线衍射图中观察到结晶氢氧化物固相(An(III)(OH)3(cr))而不是An(III)2O3(cr),其溶解度值比An(III)(OH)3(am)低一个数量级[13,14]。这可以用An(III)2O3(cr)的热力学数据来解释。例如,据报道,Am2O3(cr)的标准焓(∆fHm°)和熵(Sm°)分别为∆fHm°= - 1690.4±8.0 kJ/mol和Sm°= 133.6±6.0 J/K/mol,因此标准生成吉布斯能为∆fGm°= - 1605.449±8.284[2]。结合Am和H2O的热力学数据[2],计算出1/ 2am2o3 (cr) + 3H Am + 3/ 2h2o的标准反应吉布斯能(∆rGm°)为∆rGm°=−151.59 kJ/mol,得到溶解度积(Ks°)为log Ks°= 26.56。该值比报道的Am(OH)3(Am)和Am(OH)3(cr)[2,4]高约10个数量级,这表明氧化物固相在水体系中不太稳定。然而,由于处理大量三价锕系元素的实验限制,只有少数研究以确定的固相表征研究了An(III)的溶解度[8,11,13],并且An(III)2O3(cr)在水体系中的稳定性也没有得到很好的实验澄清。三价镧系元素常被用作三价锕系元素的类似物。许多文献研究了轻到重镧系元素的水解行为、溶解度和固相,并报道了它们的热力学数据[15-24]。一些著作偶尔总结了关于三价镧系元素溶解度的知识状态[25-28]。最近,Brown和Ekberg[4]整理了镧系元素水解的文献数据,并选择了氢氧化物固相溶解度积(Ln(III) (OH)3(s))的推荐值和相关热力学数据。值得注意的是,由于对固相鉴定较差,短时效期后得到的无定形氢氧化物固相(Ln(III) (OH)3(am))的溶解度产物被排除在综述之外[4]。Konings等人[29]对镧系元素和锕系元素氧化物的热力学性质进行了全面的综述,其中选择了镧系元素氧化物固相(Ln(III)2O3(cr))的推荐值∆fHm°和Sm°。例如,根据已报道的溶液量热法和热容测量结果,La2O3(cr)的∆fHm°和Sm°的值分别为∆fHm°=−1791.6±2.0 kJ/mol和Sm°= 127.32±0.84 J/K/mol[29]。1/2 La2O3(cr) + 3H La + 3/ 2h2o的计算∆fGm°和随后的∆rGm°为- 192.33 kJ/mol,导致log Ks°= 33.70,远远大于La(OH)3(s)的选择k°值(log Ks°= 19.72)[4]。在一些文献中观察到Ln(III)2O3(cr)在水溶液中向Ln(III) (OH)3(cr)的转变[30-32]。Ln(III)(OH)3(cr)的形成是通过NaOH沉淀Ln(III)溶液,在热硝酸盐溶液中完全溶解初始Ln(III)2O3(cr)后观察到的[31]。Neck等人[32]在进行三价镧系氢氧化物和氧化物的溶解度和固相溶解度实验之前,观察到初始材料Nd2O3(cr)在25℃的纯净水中经过几个月转化为Nd(OH)3(cr)
{"title":"Solubility and solid phase of trivalent lanthanide hydroxides and oxides","authors":"M. Moniruzzaman, Taishi Kobayashi, T. Sasaki","doi":"10.14494/JNRS.20.32","DOIUrl":"https://doi.org/10.14494/JNRS.20.32","url":null,"abstract":"For the safety assessment of radioactive waste disposal, it is necessary to predict the migration behavior of actinide elements under relevant geochemical conditions, as they are included in the waste as alpha-emitting radionuclides wit h long half-lives. Actinide elements of thorium, uranium, neptunium, and plutonium can exist in a tetravalent oxidation state under reducing geochemical conditions, deep underground and easily precipitate as a sparingly soluble amorphous hydroxide solid phase (An(IV)(OH)4(am)) under neutral to alkaline pH conditions of the waste repository systems [1-4]. The solubilities of An(IV)(OH)4(am), hence, play an important role in understanding their migration behavior. It is known that a crystalline oxide solid phase as An(IV)O2(cr) is thermodynamically more stable and it has been reported that the crystallization of An(IV)(OH)4(am) towards An(IV)O2(cr) proceeded under certain solution conditions such as strong alkaline pH or elevated temperatures [5-7]. The solubilities of An(IV)O2(cr) have been reported to several orders of magnitude lower than those of An(IV)(OH)4(am) [1-7]. Trivalent actinide elements of americium and curium also exhibit a strong hydrolysis reactions under neutral to alkaline pH conditions to precipitate the sparingly soluble amorphous hydroxide solid phase (An(III)(OH)3(am)) [8-11]. In contrast to the tetravalent actinide elements, no crystalline oxide solid phase (An(III)2O3(cr)) was observed in the solubility experiments [2,12]. A few literatures have observed crystalline hydroxide solid phase (An(III)(OH)3(cr)) from X-ray diffraction patterns instead of An(III)2O3(cr) and showed an order of magnitude lower solubility values than those of An(III) (OH)3(am) [13,14]. This can be explained by thermodynamic data of An(III)2O3(cr). For example, the standard enthalpy (∆fHm°) and entropy (Sm°) of Am2O3(cr) have been reported to be ∆fHm° = −1690.4±8.0 kJ/mol and Sm° = 133.6±6.0 J/K/mol resulted in the standard formation Gibbs energy of ∆fGm° = −1605.449±8.284 [2]. Combined with the thermodynamic data for Am and H2O [2], the standard reaction Gibbs energy (∆rGm°) for 1/2 Am2O3(cr) + 3H Am + 3/2 H2O was calculated to be ∆rGm° = −151.59 kJ/mol, leading to the solubility product (Ks°) of log Ks° = 26.56. This value is approximately 10 orders of magnitude h igher than those repor ted for Am(OH)3(am) and Am(OH)3(cr) [2,4], hinting the oxide solid phase is less stable in aqueous systems. However, due to experimental limitations for handling macro amounts of trivalent actinide elements, only few studies have investigated the An(III) solubility with a definite solid phase characterization [8,11,13] and the stability of An(III)2O3(cr) in aqueous systems has not been well experimentally clarified. Trivalent lanthanide elements are often used as analogues of trivalent actinide elements. A number of literatures have investigated the hydrolysis behavior, solubilities and solid phases of lighter to heavier lanthanide el","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"29 1","pages":"32-42"},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88341420","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Accurate determination of three halogen elements (Cl, Br, and I) in U.S. Geological Survey geochemical reference materials by radiochemical neutron activation analysis and an exhaustive comparison with literature data: a review 美国地质调查局地球化学参考物质中三种卤素元素(Cl、Br和I)的放射化学中子活化分析及与文献数据的详尽比较:综述
Pub Date : 2020-01-01 DOI: 10.14494/JNRS.20.12
S. Sekimoto, M. Ebihara
,
{"title":"Accurate determination of three halogen elements (Cl, Br, and I) in U.S. Geological Survey geochemical reference materials by radiochemical neutron activation analysis and an exhaustive comparison with literature data: a review","authors":"S. Sekimoto, M. Ebihara","doi":"10.14494/JNRS.20.12","DOIUrl":"https://doi.org/10.14494/JNRS.20.12","url":null,"abstract":",","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"7 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"74945427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pretreatment conditions for detecting 134Cs -Eight years after the Fukushima Daiichi nuclear accident- 检测134Cs的预处理条件-福岛第一核电站事故发生8年后-
Pub Date : 2020-01-01 DOI: 10.14494/JNRS.20.25
K. Shozugawa, Mayumi Hori
is an activation product with a short half-life (2.06 years) that was released during the disaster. It is an important indicator of contamination from the disaster it has been more years since the last event when 134 Cs was released. The ratio of 137 Cs to 134 Cs was approximately the time of the and thus, it is possible to quantitatively evaluate the of
是灾难期间释放的半衰期短(2.06年)的激活产物。这是灾难污染的一个重要指标,距离上次134 - c泄漏事件已经过去多年了。137cs与134cs的比值近似于时间,因此可以定量评价时间
{"title":"Pretreatment conditions for detecting 134Cs -Eight years after the Fukushima Daiichi nuclear accident-","authors":"K. Shozugawa, Mayumi Hori","doi":"10.14494/JNRS.20.25","DOIUrl":"https://doi.org/10.14494/JNRS.20.25","url":null,"abstract":"is an activation product with a short half-life (2.06 years) that was released during the disaster. It is an important indicator of contamination from the disaster it has been more years since the last event when 134 Cs was released. The ratio of 137 Cs to 134 Cs was approximately the time of the and thus, it is possible to quantitatively evaluate the of","PeriodicalId":16569,"journal":{"name":"Journal of nuclear and radiochemical sciences","volume":"32 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2020-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88436469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
期刊
Journal of nuclear and radiochemical sciences
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1