UO_2-HF-HCl-H_2O体系中介稳溶液的研究

铀是基本的核燃料,是重要的能源资源,UF_4则是生产金属铀工艺中的重要化合物。湿法生产UF_4又是重要手段之一。但在工业上如何用水法生产合格的UF_4,有不少值得研究的问题,其中对湿法生产UF_4中生产工艺条件的控制是关键,因此必须深入了解和掌握UF_4的生成和结晶的平衡条件。本文研究了UO_2-HF-HCl-H_2O四元体系80℃相平衡,平衡75h,盐酸浓度150g/l载面中介稳溶液的性质,测定了它的区域,分解时间和组成的关系,找到了能够生成良好的UF_4晶体的条件和区域。

Lu-Hf同位素的MC-ICP-MS实验方法及其在华北克拉通典型火山岩研究中的应用

Over past ten years, a great development has been made in the Lu-Hf isotopic system with the advent of MC-ICP-MS. Based on a comprehensive review of available references in the related field, a novel analytical protocol of three exchange chromatographies after one mixed acid attacking geological samples was developed in this work, which not only avoids common multiple sample treatments for natural inhomegeneous samples, but also is useful for Rb-Sr, Sm-Nd and Lu-Hf isotopic system simultaneously, especially for the garnet- and apatite-bearing rocks for the Sm-Nd and Lu-Hf geochronology. An analytical procedure for the Lu and Hf concentration in geological samples determined by by ID-MC-ICP-MS was detailedly investigated. The Hf yield is > 90 % and total procedural blank is less than. 50 pg for Hf and 10 pg for Lu, respectively. The developed method was successfully applied to the determination of Lu and Hf concentrations for USGS geological materials. A one-column procedure for Hf purification in geological samples using common anion exchange chromatography and its isotopic analyses by MC-ICP-MS were also established. Multiple analyses of Standard Reference Materials demonstrate that this method was simple, time-saving, cheap and efficient, especially suitable for the Hf isotopic compositions of young samples. Finally, the measurements of Sr and Nd isotopic compositions using Neptune MC-ICP-MS were described briefly, which indicates that Neptune MC-ICP-MS can precisely measure Sr and Nd isotopic compositions as the TIMS does, even more efficient and less time-consuming than the TIMS method. The Hf isotopic characteristics of typical volcanic rocks (Cenozoic Changle-Linqu basalts, Mesozoic Fangcheng basalts, Mesozoic Jianguo basalts, Mesozoic Wulahada high-Mg andesite, Cenozoic Fanshi, Zuoquan and Xiyang-Pingding basalts of the Taihang Mountains, Paleozoic diamondiferous Menyin and Fuxian Kimblites) from the North China Craton were firstly studied in this work. Coupled with Nd isotopic compositions, it shows that the Hf isotopes could be a better tracer for mantle sources than the Nd isotopes. Individual kimberlite fields from both the Mengyin and Fuxian regions have quite uniform Hf isotopic compositions, similar to the situation for the Nd isotopes.

碎屑锆石年龄和Nd-Hf同位素组成对扬子基底演化的制约

The South China craton was formed by the collision of the Yangtze and Cathaysia blocks during the Neoproterozoic Jiangnan orogeny (also termed as the Jingnin or Sibao orogeny in Chinese literature). Basement rocks within the Yangtze block consist mainly of Proterozoic sediments of the Lengjiaxi and Banxi Groups. U-Pb ages of detrital zircons obtained by the LA-ICP-MS dating technique imply that the deposition of the Lengjiaxi Group continued until the Neoproterozoic. The youngest detrital zircons suggest a maximum deposition age of ~830 Ma for the Lengjiaxi Group, consistent with the initiation time of the deposition of the overlying Banxi Group, likely indicating continuous deposition of these two groups and a short temporal hiatus (~10 Ma) between the Neoproterozoic sedimentary rocks distributed in the South China craton. Detrital zircons from both the Lengjiaxi and Banxi Groups have a wide range of εHf(t) values from -12 to 14.2 and a continuous Nd and Hf model age spectrum from ~820 Ma to 2200 Ma. Some grains have model ages ranging up to ca. 2.9-3.5 Ga, indicating that both juvenile mantle material and ancient crust provided sedimentary detritus. This is also consistent with the Nd isotopic signature of sedimentary rocks recorded in the Lengjiaxi Group, suggesting a back-arc tectonic setting. The Banxi Group has slightly enriched Nd isotopic signatures relative to the Lengjiaxi Group, implying a higher percentage of old continental material in the sedimentary source. Combined with previously published data, new results can help us to reconstruct the Neoproterozoic tectonic evolution of the South China craton. The age spectrum of detrital zircons and Nd-Hf isotopic composition suggests a two-stage collision: Between 1000 Ma to 870 Ma, a continental magmatic arc was build up along the eastern margin of the Yangtze block. Convergence led to continent-based back-arc extension, subsidence and formation of a back-arc basin. Detritus originating from arc-related magmatic and old basement rocks was transported into this back-arc basin resulting in formation of the Lengjiaxi Group and its equivalents. At around 870 Ma, a second (oceanic) arc was formed by extension of an inter-arc basin, subduction subsequently led to the first collision and the emplacement of the blueschist mélange. Accretion of the magmatic arc lasted until the closure of an oceanic basin between the Yangtze and Cathaysia blocks at about 830 Ma. Shortly after the collision, subsequent uplift, further extension of the former back-arc basin and post-collisional granitoid magmatism caused a tilting of the Lengjiaxi sediments. Between 830 Ma and 820 Ma, subsequent closure of the oceanic back-arc basin and formation of the Jiangnan orogen took place, leaving a regional unconformity above the Lengjiaxi Group. Above this unconformity the Banxi Group was immediately deposited during the post-tectonic stage.

Zr、Hf在水合氧化铁上的吸附实验研究

制备了两种不同n(Zr)/n(Hf)的Zr、Hf混合溶液,测定了实时生成的水合氧化铁和预先生成的水合氧化铁在不同pH条件下对Zr、Hf的吸附量,并对其吸附等温线进行了研究.研究结果表明:等价元素Zr、Hf在HFO上的吸附是非线性的,在吸附过程中二者发生了分异,Zr的吸附能力要大于Hf;在天然水体pH值范围内(pH≥6),Zr、Hf的吸附量Q及n(Zr)/n(Hf)不随pH发生变化,显示了Zr、Hf相对惰性的行为;Zr、Hf在吸附过程中表现出惊人的一致性行为,Zr、Hf数据间的相关系数R2在0.98以上;Zr、Hf在HFO上的吸附可能是表面羟基与Zr、Hf表面络合反应的结果,并且络合能力Zr＞Hf.

Zr^4＋和Hf^4＋在水合氧化铁上的吸附及其分异的实验研究

本文研究了4价阳离子Zr、Hf在水合氧化铁(HFO)上的吸附及其在胶体／溶液界面的分异行为。研究结果表明：等价元素Zr、Hf在HFO上的吸附是非线性的，在吸附和共沉淀过程中二者发生了分异，Zr的吸附能力要大于Hf；pH<6时，固相中Zr／Hf比值随pH的升高迅速降低，而在天然水体pH范围内(pH≥6)，Zr、Hf的吸附量Q及Zr／Hf比值则不随pH发生变化，显示了Zr、Hf在表生环境中的相对惰性行为。本研究为吸附／解吸或水／粒相互作用导致Zr、Hf在地表环境的分异提供了实验证据。

气流化学激光理论研究的若干进展

以超声速HF/DF化学激光和超声速氧碘化学激光(COIL)为代表的气流化学激光(GCL),因其科学意义、军事和工业应用价值,近30多年来得到了突飞猛进的发展.由于超声速膨胀混合流在控制强放热反应动力学和热力学过程方面的特殊本领,使气体动力学在高功率GCL的发展中起着关键性的作用.高功率GCL性能的分析计算自然也沿用非平衡气体动力学的方法,假定气流(包括激光能级分子和原子)为连续介质,谱线为均匀加宽,并联立求解气体动力学方程组,增益动力学和基于光强迭加原则的辐射传输诸方程,称为速率方程(RE)模型.20世纪70年代后期又提出和发展了GCL性能计算的半气体动理学(SGK)模型,在SGK模型中仍假定气流为连续介质,但同时考虑了激光能级分子微观热运动的贡献,谱线加宽的非均匀加宽效应,并用双参数摄动法求解激光能级分子速度分布函数方程组(即广义Boltzmann方程组),因此SGK模型是一个同时考虑宏观和微观尺度运动的跨尺度模型.本文综述RE模型和SGK模型以及用它们预测GCL性能的若干研究进展,同时简评等增益模型和腔模(模图样)理论研究的一些进展.最后从气体动力学的角度提出一些值得进一步研究的课题.

Inverse Analysis Determining Interfacial Properties Between Metal Film And Ceramic Substrate With An Adhesive Layer

In the present study, peel tests and inverse analysis were performed to determine the interfacial mechanical parameters for the metal film/ceramic system with an epoxy interface layer between film and ceramic. Al films with a series of thicknesses between 20 and 250 mu m and three peel angles of 90 degrees, 135 degrees and 180 degrees were considered. A finite element model with the cohesive zone elements was used to simulate the peeling process. The finite element results were taken as the training data of a neural network in the inverse analysis. The interfacial cohesive energy and the separation strength can be determined based on the inverse analysis and peel experimental result.

Quantum Monte Carlo study of the CO interaction with a dimer model surface for Cr(110)

The chemisorption of CO on a Cr( 110) surface is investigated using the quantum Monte Carlo method in the diffusion Monte Carlo (DMC) variant and a model Cr2CO cluster. The present results are consistent with the earlier ab initio HF study with this model that showed the tilted/ near-parallel orientation as energetically favoured over the perpendicular arrangement. The DMC energy difference between the two orientations is larger (1.9 eV) than that computed in the previous study. The distribution and reorganization of electrons during CO adsorption on the model surface are analysed using the topological electron localization function method that yields electron populations, charge transfer and clear insight on the chemical bonding that occurs with CO adsorption and dissociation on the model surface.

利用有限差分法求解扩散混合化学反应二维平行流动

利用隐式有限差分方法,对两股平行流的扩散混合、化学反应问题进行了计算。计算中,使用了层流压缩边界层方程并考虑了HF化学激光器的化学反应。计算结果表明:HF(2)振动激发态的浓度要比HF(1),HF(3)、HF(0)的浓度都高,从而获得了粒子数反转条件。另外,在计算中不需要混合长度的假设,就可以求得主流(无化学反应区)与化学反应区的两条界面曲线。当然,本文的计算方法要比直接求解二维Navier-stokes方程要简单得多。

气流与化学激光的增益饱和

本文提出气流与化学激光的增益饱和理论,理论对特征时间比τ/τ_c的所有可能的数值范围均适用,这里τ指流动特征时间(即气流通过激光作用区所需要之时间),τ_c指碰撞弛豫特征时间。阐明并分析了对流和反转数密度“源流”的饱和效应,得到了增益系数之普遍关系式以及一些新的增益饱和规律。本理论在τ/τ_c《1条件下的结果与近来超声速扩散HF化学激光增益饱和的试验结果相符合。气体介质无宏观运动时的熟知增益饱和理论是本理论在τ/τ_c→∞条件下的特例;气流激光的已有增益饱和理论则是本理论在τ/τ_c》1条件下的特例。

连续波化学激光的非均匀加宽效应

本文用运动论模型处理二能级连续波HF化学激光问题.对层流和湍流混合情况,给出了振荡器特性的具体计算公式,并在一定的(?)值和有限的化学泵浦速率K的情况下,精确求解了激光强度、功率和化学效率.计算结果表明,当加宽参数η<0.20时,非均匀加宽影响严重,必需采用运动论模型处理;η>0.20时,本文结果与速率模型结果比较接近,可用速率模型处理.