岩石矿物中铀钍的分析方法进展——非破坏分析法

非破坏分析法部分着重介绍了岩石矿物中铀钍的非破坏性分析方法原理、特点和应用范围。非破坏分析手段主要包括:中子活化分析法(NAA)、裂变径迹法(FTA)、X射线荧光光谱法(XRF)、激光烧蚀光谱法(LIBS)和γ能谱直接测量法。非破坏分析鉴于其独特优势仍有发展空间,LIBS技术是新近发展的具有较大潜力的技术手段,而γ能谱直接测量法针对铀钍等放射性核素的测量具有无可比拟的发展优势。     

Improving Our Knowledge on the 229mThorium Isomer: Toward a Test Bench for Time Variations of Fundamental Constants

For more than four decades, the lowest excitation in the whole landscape of atomic nuclei, the low‐lying, isomeric state of ²²⁹Th, the so‐called thorium isomer, has challenged physicists of various disciplines. Being a solitaire with its uniquely low excitation energy of <10 eV, its predicted lifetime of a few hours results in an extremely sharp relative linewidth ΔE/E as low as 10^–20. While until recently the indication of its existence was based only on indirect evidence, its unique properties inspired a multitude of potential applications, like the use of the thorium isomer as a nuclear frequency standard, potentially able to outperform even the best atomic clocks and a sensitivity‐enhanced access to potential temporal variations of fundamental constants. The various proposals to exploit the unique properties of ^229mTh are presented herein, in particular focusing on its ability to serve as a test bench for time variations of fundamental constants like the fine structure constant.     

Adsorption of the lanthanum and thorium cryptates at mercury electrode

The adsorption behavior of cryptates of La³⁺ and Th⁴⁺ cations at the Hg/aqueous solution interface is studied by using the electrochemical impedance spectroscopy method. It was shown that the studied complexes have high surface activity at the interface. The lanthanum cryptate adsorption parameters are found using the regression analysis based on the two parallel capacitor model supplemented by the Frumkin adsorption isotherm. The differential capacitance curves calculated by using these parameters agree satisfactorily with the experimental ones. The more complicated adsorption behavior of lanthanum cryptate, as compared with the complexes of lower valence cations, is interpreted with taking into consideration the strong interaction of the La³⁺ cation contained in the [2.2.2.] cryptand intramolecular cavity with the supporting electrolyte anions.     

First-principles study of the elastic and thermodynamic properties of thorium hydrides at high pressure

The high pressure behaviors of Th_4H_(15) and ThH_2 are investigated by using the first-principles calculations based on the density functional theory(DFT). From the energy–volume relations, the bct phase of ThH_2 is more stable than the fcc phase at ambient conditions. At high pressure, the bct ThH_2 and bcc Th_4H(15) phases are more brittle than they are at ambient pressure from the calculated elastic constants and the Poisson ratio. The thermodynamic stability of the bct phase ThH_2 is determined from the calculated phonon dispersion. In the pressure domain of interest, the phonon dispersions of bcc Th_4H(15) and bct ThH_2 are positive, indicating the dynamical stability of these two phases, while the fcc ThH_2 is unstable. The thermodynamic properties including the lattice vibration energy, entropy, and specific heat are predicted for these stable phases. The vibrational free energy decreases with the increase of the temperature, and the entropy and the heat capacity are proportional to the temperature and inversely proportional to the pressure. As the pressure increases, the resistance to the external pressure is strengthened for Th_4H_(15) and ThH_2.     

离线测量钍快中子裂变反应率方法

钍快中子裂变反应率是钍铀燃料循环中的重要数据.为了测量基于聚变-裂变混合能源堆包层概念设计的钍样品在宏观中子学装置中的钍快中子裂变数据,发展了钍快中子裂变率的离线活化γ测量方法.通过测量232Th裂变碎片85mKr的β衰变产物85Rb发射的151.16 keV特征γ射线,并结合钍裂变产额数据,获得了钍样品装置中232Th裂变反应率的分布.详细介绍了此方法的原理和影响因素,并利用14 MeV的D-T中子源在贫铀球壳中开展了校验实验,实验不确定度为5.3%—5.5%.采用MCNP5程序和ENDF/B-VI及ENDF/B-VII数据库模拟计算的结果与实验结果在实验不确定度内基本符合,这证明该方法能够有效地模拟装置中232Th裂变反应率.     

ChemInform Abstract: Infrared Spectroscopic and Theoretical Investigations of the OUF2 and OThF2 Molecules with Triple Oxo Bond Character.

The title molecules are prepared by reaction of OF₂ molecules with laser ablated uranium and thorium atoms in solid argon and neon.     

Infrared Spectra of the HAnX and H2AnX2 Molecules (An=Th and U,X=Cl and Br) in Argon Matrices Supported by Electronic Structure Calculations

Uranium and thorium hydrides are known as functional groups for ligand stabilized complexes and as isolated molecules under matrix isolation conditions. Here, the new molecular products of the reactions of laser-ablated U and Th atoms with HCl and with HBr, namely HUCl, HUBr and HThCl, HThBr, based on their mid and far infrared spectra in solid argon, are reported. The assignment of these species is based on the close agreement between observed and calculated vibrational frequencies. The H−U and U−³⁵Cl stretching modes of HUCl were observed at 1404.6 and 323.8 cm⁻¹, respectively. Using DCl instead to form DUCl gives absorption bands at 1003.1 and 314.7 cm⁻¹. The corresponding bands of HThCl are 1483.8 (H−Th) and 1058.0 (D −Th), as well as 340.3 and 335.8 cm⁻¹ (Th−³⁵Cl), respectively. HUBr is observed at 1410.6 cm⁻¹ and the BP86 computed shift from HUCl is 6.2 cm⁻¹ in excellent agreement. The U−H stretching frequency increases from 1383.1 (HUF), 1404.6 (HUCl), 1410.6 (HUBr) to 1423.6 cm⁻¹ (UH) as less electronic charge is removed from the U−H bond by the less electronegative substituent. These U−H stretching frequencies follow the Mayer bond orders calculated for the three HUX molecules. A similar trend is found for the Th counterparts. Additional absorptions are assigned to the H₂AnX₂ molecules (An=U, Th, X=Cl, Br) formed by the exothermic reaction of a second HX molecule with the above primary products.     

Measurement of fast neutron induced fission cross section of thorium using Lexan plastic track detector

Fission-track registration characteristics of Lexan solid state nuclear track detectors have been used to measure the fast neutron induced fission cross section of²³²Th. The fast neutrons (?14.2MeV) were produced with the help of an AN-400 model Van-de-Graaff accelerator at Banaras Hindu University laboratory using³H(²H,n)⁴He reaction and were used to irradiate the fissile target deposited on the plastic detector. The track densityT, registered on the plastic detector is related to the fission cross sectionσ _f, through the relationT=knσ _føt wheren is the number of fissile atoms per cm² in the deposit, ø is the neutron flux,k is fission track registration efficiency andt is the time of irradiation. The fission cross sectionσ _f of²³²Th, relative to the well measured fission cross section of²³⁸U, was found to be 0.36±0.04 barn.     

3,6-二-〔二甲氨基〕二苯并碘六环六硝酸钍配合物的研究

本文报道了在甲醇介质中以硝酸钍和碘杂环硝酸盐为原料合成了3,6—二—〔二甲氨基〕二苯并碘六环六硝酸钍配合物,组成为:     

Component activities in the system thorium nitrate-nitric acid-water at 25°C

The equilibrium composition of the vapor above thorium nitrate-nitric acid-water mixtures has been studied as a function of the concentrations of thorium nitrate and nitric acid using a transpiration technique. At 25°C, the thorium nitrate concentrations m _T ranged from 0.1 to 2.5 molal and the nitric acid concentrations m _N from 0.3 to 25 modal. The vapor pressure of the nitric acid was found to increase with increasing thorium nitrate concentration for a constant molality of nitric acid in aqueous solution. At constant m _T , the nitric acid vapor pressure was particularly enhanced at low nitric acid concentrations. The water vapor pressures decreased regularly with increasing concentrations of both nitric acid and thorium nitrate. The experimental data were fitted to Scatchard's ion-component model, and to empirical multiparameter functions. From the fitting parameters, and available literature data for the nitric acid-water and thorium nitrate-water systems at 25°C, expressions were calculated for the variation of water and thorium nitrate activities, as functions of the nitric acid and thorium nitrate concentrations, using the Gibbs-Duhem equation. Calculated values for the thorium nitrate activities were strongly dependent on the form of the function originally used to fit the vapor pressure data.Issued as AECL-7461.