激光烧蚀铀材料生成铀微粒的形态学研究

本文以激光器作光源,利用激光的高温烧蚀特性,以激光束烧蚀金属铀和二氧化铀材料,模拟高温条件下形成铀微粒的过程,用扫描电子显微镜和透射电子显微镜对铀材料及产生的含铀微粒的形态学特点进行了表征。实验表明,在激光束的轰击下,两种靶材料均出现熔化现象,铀金属表面呈现明显波纹状结构,二氧化铀的表面轰击边缘处呈现趋球状物堆积。生成的铀氧化物微粒为μm级形态不规则微粒及1 μm左右的球形微粒,说明铀在高温过程中产生球形微粒。对比研究了来自高温爆炸过程的金属银微粒,进一步验证了高温高压过程会产生球形微粒。结果表明,密实的铀氧化物微球是铀材料参与高温化学过程的结果,与低温过程中的剥蚀作用有明显的差别,是高温化学过程的特征,这为高温高压环境中的微粒分析提供了参考依据。     

Behavior of Sodium Oxide Aerosol in a Closed Chamber

The behavior of sodium oxide aerosol in a closed chamber was studied for the safety analysis of a Na-cooled fast reactor. The experimental apparatus and techniques are first described. The aerosol was released during a short time by blowing air onto heated Na in a 1 m³ chamber. The maximum mass concentration of the aerosol in the form of Na₂O ranged of 0.05 ～ 10g/m³. The particle size distribution, the aerosol mass concentration and the mass deposition rates were measured as a function of time.

It was found that the mass median diameter of the aerosol was related to the maximum mass concentration. To determine the character of the behavior of sodium oxide aerosol in the chamber, the density of the aerosol material and the thickness of the boundary layer through which the particles deposit on the chamber wall were observed. The initial half-time of the aerosol mass concentration was compared with the values numerically calculated under certain assumptions.     

Aerosol composition and source apportionment in Santiago de Chile

Santiago de Chile, São Paulo and Mexico City are Latin American urban areas that suffer from heavy air pollution. In order to study air pollution in Santiago area, an aerosol source apportionment study was designed to measure ambient aerosol composition and size distribution for two downtown sampling sites in Santiago. The aerosol monitoring stations were operated in Gotuzo and Las Condes during July and August 1996. The study employed stacked filter units (SFU) for aerosol sampling, collecting fine mode aerosol (dp<2 μm) and coarse mode aerosol (210 mass of particles smaller than 10 μm) and black carbon concentration were also measured. Particle-Induced X-ray Emission (PIXE) was used to measure the concentration of 22 trace elements at levels below 0.5 ng m⁻³. Quantitative aerosol source apportionment was performed using Absolute Principal Factor Analysis (APFA). Very high aerosol concentrations were observed (up to 400 μg/m³ PM₁₀). The main aerosol particle sources in Santiago are resuspended soil dust and traffic emissions. Coarse particles account for 63% of PM₁₀ aerosol in Gotuzo and 53% in Las Condes. A major part of this component is resuspended soil dust. In the fine fraction, resuspended soil dust accounts for 15% of fine mass, and the aerosols associated with transportation activities account for a high 64% of the fine particle mass. Sulfate particle is an important component of the aerosol in Santiago, mainly originating from gas-to-particle conversion from SO₂. In the Gotuzo site, sulfates are the highest aerosol component, accounting for 64.5% of fine mass. Direct traffic emissions are generally mixed with resuspended soil dust. It is difficult to separate the two components, because the soil dust in downtown Santiago is contaminated with Pb, Br, Cl, and other heavy metals that are also tracers for traffic emissions. Residual oil combustion is observed, with the presence of V, S and Ni. An aerosol components from industrial emissions is also present, with the presence of several heavy metals such as Zn, Cu and others. A factor with molybdenum, arsenic, copper and sulfur was observed frequently, and it results from emissions of copper smelters.     

Isotopic composition of boron secondary ions as a function of ion-beam fluence

We have examined the effects of target mass on sputtered material using 100 keV argon and neon to sputter an elemental target comprising the two naturally occurring isotopes of boron. At low beam fluences (≈ 1 × 10¹⁵ions/cm²) a light-isotope secondary enhancement is observed relative to steady-state secondary ion yields collected at higher beam fluences. The enhancement (46.1%o for Ne⁺ irradiation and 51.8%o for Ar⁺ irradiation) is large compared to the predictions of analytical theories and is independent of variations in surface potential, chemical effects, and surface impurities. This effect is consistent with an explanation based on an energy and momentum asymmetry in the collision cascade.     

铀自燃对放射性气溶胶的影响研究

以国内某金属铀真空蒸镀实验室的金属铀物料加工工艺为对象,采用放射性气溶胶连续监测,向心式气溶胶粒度分级采样,垂直高度分级采样等方法,研究了金属铀自燃对实验室空气中放射性气溶胶浓度、粒径分布、空间竖直分布的影响。结果表明,金属铀自燃明显提高了实验室空气中放射性气溶胶的浓度;所产生的气溶胶活度中位直径为9.89μm,粒径分布中大粒径气溶胶粒子占优;燃烧产生的放射性气溶胶在物料高度处浓度的增大水平高于工作人员呼吸带的增大水平。     

Pulsed laser treatments of polyethylene films

A Nd:Yag pulsed laser, 3 ns pulse width, 150 mJ pulse energy, operating at the second harmonics (532 nm) has been used to irradiate in air polyethylene thin films.The thermal and chemical effects induced by the laser irradiation in the polymer are responsible of the hydrogen and C_xH_y groups emission at long irradiation times. A special study, concerning the welding effect between two different types of polyethylene films, one transparent and the other strong absorbent the laser light, was performed. The welding, at the interface of the two pressed polymers, depends on the optical and micro-structural material properties besides the irradiation time. In particular, polymers with different viscosity, melting temperature and crystalline degree exhibit different mechanical behaviour.Different techniques were employed to investigate on the polymeric welding effects, such as the mass quadrupole spectrometry, the scanning electron microscope, the surface profiler and the mechanical strength measurement.     

核材料炸药化学爆炸条件下烟云源项的实验与仿真

为获取核材料化学爆炸事故烟云参数和气溶胶扩散规律,本文理论分析了核材料化学爆炸事故烟云扩散过程与机理,建立了基于CFD技术的烟云扩散数值仿真方法,并通过爆炸烟云外场扩散实验对该方法进行了验证。研究结果表明：CFD方法能实现烟云扩散的数值仿真;实验和仿真均显示小当量TNT爆炸高度远小于Church经验公式,宽度比例却增加;气溶胶颗粒在蘑菇云形态的双涡环烟云流场中分布不均匀,粒径大于50 μm的颗粒物大多位于烟柱中,而大部分可吸入颗粒物在烟云顶部聚集;气溶胶在烟云稳定前的驱散与沉降会改变其源项参数,以Operation Roller Coaster实验气溶胶积累质量分布为例的计算显示,空载释放率约为地面气化率的58%,可吸入比率由20%升高至31%,可吸入释放率约为18%。     

A reinvestigation of low molecular weight components in SOA produced by cyclohexene ozonolysis

The ozonolysis of cyclohexene is an important model system for understanding the more complex reaction of O_3 with monoterpenes; however, many previous studies have come to qualitatively different conclusions about the composition of the secondary organic aerosol(SOA)formed in this system. In the present study, the composition of the SOA produced by cyclohexene ozonolysis in the absence of seed aerosols has been investigated online and off-line using synchrotron-based thermal desorption/tunable vacuum ultraviolet photoionization time-of-flight aerosol mass spectrometry(TD-VUV-TOF-PIAMS) in conjunction with a custom-built smog chamber. On the basis of the molecular ions observed by mass spectrometry at 11.5 e V, it was found that dicarboxylic acids, dialdehydes, and cyclic anhydrides are the predominant low molecular weight components in the particle phase. The results also indicated that TD-VUV-TOF-PIAMS coupled with filter sampling is a potentially useful tool for the investigation of SOA composition both in the field and in the laboratory.     

Analysis of atmospheric aerosols by PIXE: the importance of real time and complementary measurements

Particle-Induced X-ray Emission (PIXE) has been used for more than 30 yr in many urban and background air pollution studies. The technique has certainly contributed to the understanding of source-receptor relationship for aerosol particles as well as to aerosol physics and chemistry. In the last few years, where aerosol issues were strongly linked to global climate change through the relationship between aerosol and atmospheric radiation points to new challenges in atmospheric sciences, where PIXE could play an important role. Also the recognition for the inter-relationship between aerosol and liquid and gas phases in the atmosphere makes important to integrate PIXE aerosol analysis with other complementary measurements. The use of Nephelometers and Aethalometers to measure scattering and absorption of radiation by aerosol particles can be done in parallel with particle filter collection for PIXE analysis. Parallel measurements of trace gases using traditional monitors as well as with new techniques such as Differential Optical Absorption Spectroscopy (DOAS) that can provide concentration of O₃, SO₂, NO₃, NO₂, HCHO, HNO₃, Benzene, Toluene, and Xylene, is also important for both urban and remote aerosol studies. They provide information that allows a much richer interpretation of PIXE data. Recently developed instruments that provide real time aerosol data such as the Tapered Element Oscillating Microbalance (TEOM) PM₁₀ monitor and automatic real time organic and elemental carbon analyzers provide extremely useful data to complement PIXE aerosol analysis. The concentrations of trace elements measured by PIXE comprise only 10–30% of the aerosol mass, leaving the organic aerosol characterization and measurement with an important role. The aerosol source apportionment provided by PIXE analysis can be extended with other aerosol measurements such as scattering and absorption, estimating for example, the radiative impact of each discriminated aerosol source. The aerosol bulk PIXE measurements can be complemented with soluble concentrations provided by Ion Chromatography (IC) and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS). Recent developments in remote sensing techniques and products also enhance significantly regional aerosol studies. Three-dimensional air mass trajectories should be integrated in aerosol studies for urban and remote areas. The applications of these techniques to study urban aerosols from São Paulo and Santiago de Chile have broadened extensively the scientific scope of these studies.     

Matrix-assisted pulsed laser evaporation of polymeric materials: a molecular dynamics study

Matrix-assisted pulsed laser evaporation (MAPLE) has been recently developed to deposit high-quality thin films for a wide range of polymeric materials. To analyze the evaporation of polymer molecules in MAPLE, we present a molecular dynamics (MD) simulation of laser ablation where the target material is modeled as a solution of polymer molecules in a molecular matrix. The breathing sphere model is used for MD simulations of laser ablation of the molecular matrix. Polymer molecules are described using a bead-spring model, where each bead represents one or several polymer groups. The initial stage of polymer ejection is investigated at different laser fluences and pulse durations. The influence of polymer molecules on the stability of clusters formed in the plume and the processes that can lead to polymer decomposition are discussed.     

负载型多分散气溶胶在管道内的传输规律

放射性气溶胶的传输一直是倍受关注的环境问题。为研究放射性气溶胶在管道内的传输规律,首先自制了能够产生稳定的、多分散气溶胶的发生器。主要考察了稀释气流速（5~25 L/min）、气溶胶颗粒粒径（多分散体系）及固体颗粒密度（土壤、石英砂）对气溶胶在管道内传输的影响。即考察了粒径多分散的石英砂、土壤颗粒形成的气溶胶及表面负载Ag的石英砂颗粒模拟负载型放射性气溶胶,在不同稀释气流速作用下进入管道内的传输,针对每一节管道内的沉积物进行收集分析,从而得到气溶胶在管道内的传输及沉降规律。研究结果表明：密闭管道内,在一定流速范围内,沉积物最高频度粒径随着管道距离的增长而先增大后减小;小粒径的颗粒在传输过程中自重沉降,且由于布朗运动吸附在大粒径颗粒物表面加速其沉降速率,即减小了其在管道内的传输距离;表面负载Ag的石英砂颗粒形成的气溶胶随着稀释气吹扫导致Ag和石英砂颗粒之间有不同程度的分凝,气流速率越大,分凝现象越明显。     

Effects of Simulated Nuclear Thermal Pulses on Fiber Optic Cables

The effects of pulsed thermal radiation on fiber optic cables with a variety of jackets (polyurethane, PVC, fluorocarbon) are presented. Exposure between 27 and 85 cal/cm2 did not sever the optical fibers, but the radiation did cause disintegration of the jackets and the Kevlar strength members, which resulted in a significant reduction of the cable's ability to survive mechanical stress. Hardening techniques are discussed. The addition of low absorptance materials (white Teflon tape and aluminum foil) under clear or white Teflon jackets prevented some types of cables from being affected at fluences up to 110 cal/cm2.     

A simple mechanistic model for particle penetration and plugging in tubes and cracks

In the course of a severe accident, some nuclear aerosols may be released to the environment through penetrating the containment concrete cracks, even if a catastrophic failure of the containment does not occur. There is experimental and theoretical evidence of strong retention of aerosol particles in the cracks that act as a filter. In this work a Eulerian model is developed based on the numerical solution of the one-dimensional aerosol transport equation. Plug formation is accommodated by allowing the crack diameter to change with time, based on the volume of the deposited mass. Brownian diffusion, gravitational settling and turbulence-driven deposition are considered as the removal mechanisms of the particles along the leak path. The model is verified against analytical solutions and validated by comparing with early as well as recent experimental data. It is concluded that a one-dimensional model of aerosol flow through a hydraulically equivalent leaking duct can simulate with enough accuracy aerosol transport in cracks, so that it may be an appropriate option for a large system code like ASTEC.     

Synchrotron micro-XRF study of metal inclusions distribution and variation in fused silica induced by ultraviolet laser pulses

Metal inclusions play critical roles in laser-induced damage for large fused silica optics. Here, the spatial distribution of sodium, aluminum, iron and copper in as-prepared samples is analyzed by synchrotron based X-ray fluorescence spectrometry microprobe system at the BL15U1 beam line at the Shanghai Synchrotron Radiation Facility. The as-prepared fused silica samples are induced by 355 nm laser pulses with no, or low, or high fluences. The spatial resolution of the obtained elemental maps is up to 50 μm. Analysis of the elemental maps indicates that the distribution of metals has a close association with the laser fluence and pulses. The normalized fluorescence signal attenuation for metal inclusions corresponds to the laser fluence. The decrement of metals depends chiefly upon the fluence other than pulses of the incidence laser, which is most pronounced for iron and least for copper. The decrement is evident for high fluence laser irradiation, while the amount is negligible for low fluence laser irradiation. Among the four metals, iron concentration is suggested as the most destructive factor for optics lifetime, especially under high fluence irradiation. The quasi-periodic feature of elemental distribution is partly ascribed to laser intensity modulation induced by Fresnel diffraction.     

The effect of coatings on deuterium retention and permeation in aluminum 6061-T6 APT tritium production tubes

The accelerator production of tritium project will utilize spallation neutrons incident on thousands of ³He gas filled metal tubes to produce tritium by way of the exothermic ³He(n,p)³H reaction. Tritons with energies up to 192 keV and protons with energies up to 576 keV are directly implanted into the tube walls. To minimize tritium retention in the tubes and permeation into the coolant surrounding the tubes, it is desirable to have the implanted tritium migrate back to the inner surface of the tubes and rapidly recombine to be released as T₂ and HT. Aluminum alloy (Al 6061-T6) is the primary candidate material for fabrication of the tubes. Aluminum alloy samples implanted with deuterons and protons to fluences as high as 3×10²² D (and p)/m² were studied. Deuterium retention was measured by mass spectrometry during thermal desorption. Approximately 10% of the implanted deuterium was retained. Copper, nickel and anodized coatings on aluminum alloy were studied as possible methods of reducing retention and permeation of the tritium. In these experiments, the Cu and Ni coatings reduced the retention significantly, whereas retention increased in the anodized coated sample.     

Disintegration of copper by 680-Mev protons

The results of a radlochemical study of the disintegration products in copper disintegration induced by 680-Mev protons is presented; the yields of nuclei which were not directly observed are obtained by extrapolation. This procedure makes it possible to obtain a complete picture of the residual products and to draw certain conclusions with respect to the basic characteristics of the process; 1) the total cross section for the disintegration of copper is 0,6 · 10^–24 cm² corresponding to 65% of the geometric cross section; 2) the main contribution in the total cross section for the production of disintegration products in copper is due to cobalt, nickel and copper (60%); 3) the isotope yield is increased as the region of stability is approached; 4) in the disintegration process, protons and neutrons are emitted in almost equal numbers _n/_p= 1.3; 5) the emission of an -particle is more probable than the subsequent emission of four nucleons; 6) nuclear structure has no effect on the disintegration of nuclei by high energy particles. By appraising the characteristic features of the disintegration of copper by 680-Mev protons in conjunction with the data obtained in studies of the products of copper disintegration induced by particles with energies from 130 Mev to 2.2 Bev, it is possible to evaluate the effect of the energy of the bombarding particles on the nature of the disintegration process in this element.     

Containment analysis on the PHEBUS FPT-0, FPT-1 and FPT-2 experiments

In a severe accident, most of the fission-product species are already condensed in aerosols when they are released to the containment. The behaviour of these aerosol particles controls the fission-product transport into the containment and affects the global Source Term. The calculations presented here were performed using the CPA module (Containment Package implemented in the European integral code ASTEC) for the in-pile PHEBUS FPT-0, FPT-1 and FPT-2 experiments and are focused on the aerosol transport. A detailed thermal-hydraulic model was used in the CPA/ASTEC code to evaluate the gas circulation pattern in the closed containment volume. The comparison of ASTEC results showed that the patterns are similar to the ones predicted by the CFD-based codes. Good agreement was reached with the measured average thermo-hydraulic parameters such as containment gas pressure, temperature and the condensation rate on the condensers. The calculations with the detailed simulation of the flow in the PHEBUS containment qualitatively predicted the particle settling on the elliptic bottom and deposition on the painted wet condenser surfaces. It was shown that the influence of the gas circulation leads to a relatively quick mixing of aerosols in the containment atmosphere. In the tests investigated, the effect of the gas circulation on the airborne aerosol mass during the aerosol injection period is small because the injected mass flux is significantly higher compared to the deposition fluxes on the vessel surfaces. During the long-term aerosol deposition phase, the flow fields predicted by CPA/ASTEC have a medium impact on the evolution of the airborne mass in the PHEBUS containment.     

一种用于SPM分析的大气气溶胶单颗粒样品的制备方法

介绍了一种用于扫描质子微探针分析的大气气溶胶单颗粒样品的制备方法。通过实验摸索出一种适合于支撑颗粒物的材料聚乙烯醇缩丁醛(PVB)。大气颗粒物被直接采集在PVB薄膜上从而制成样品,保持了颗粒物的原始信息。用显微镜观察了采集的颗粒物,颗粒物之间完全分开,颗粒物间距合适。样品的扫描质子微探针试验结果表明,所制成的单颗粒样品能经受住质子束的长久轰击。对PVB薄膜的本底测试表明,这种膜的本底很小,不会对被测颗粒物的元素产生干扰。     

两步激光－飞行时间质谱法测定铁和镍同位素

采用两步激光－飞行时间质谱法测定了铁和镍同位素。用５３２ｎｍ脉冲激光蒸发铁－镍合金及硫酸亚铁样品，蒸发产生的原子采用染料激光共振电离并由飞行时间质谱探测。结果表明，激光蒸发产生的原子束和共振电离激光之间具有很好的时间匹配效率，与连续加热原子化源相比，样品利用率提高了约三个量级。     

含钆中子屏蔽材料的设计及其力学性能分析

设计了一种具有良好中子屏蔽能力、高强度及高韧性的新型中子屏蔽材料,用于吸收核电站乏燃料储存格架和乏燃料运输过程中的热中子辐射。材料通过蒙特卡罗粒子传输(输运）软件MCNP进行设计,并通过放电等离子烧结设备及热轧的方式制成了板材。MCNP模拟结果及材料热中子屏蔽测试结果表明：铝基Gd₂O₃复合材料的热中子屏蔽性能与铝基碳化硼相当。Gd₂O₃颗粒球磨后呈现μm、亚μm级甚至有些颗粒达到了nm级。随球磨时间的增加,材料的力学性能逐渐增强。X射线衍射检测发现了钆-铝合金相的生成。经TEM分析表明：材料的强化机制主要是位错强化和nm级Gd₂O₃颗粒的弥散强化,拉伸强度和伸长率分别达到了240 MPa和16%,其断口主要为韧性断裂。