Efficient Isotope Ratio Analysis of Uranium Particles in Swipe Samples by Total-Reflection X-ray Fluorescence Spectrometry and Secondary Ion Mass Spectrometry

A new particle recovery method and a sensitive screening method were developed for subsequent isotope ratio analysis of uranium particles in safeguards swipe samples. The particles in the swipe sample were recovered onto a carrier by means of vacuum suction-impact collection method. When grease coating was applied to the carrier, the recovery efficiency was improved to 48±9%, which is superior to that of conventionally-used ultrasoneration method. Prior to isotope ratio analysis with secondary ion mass spectrometry (SIMS), total reflection X-ray fluorescence spectrometry (TXRF) was applied to screen the sample for the presence of uranium particles. By the use of Si carriers in TXRF analysis, the detection limit of 22 pg was achieved for uranium. By combining these methods with SIMS, the isotope ratios of ²³⁵U/²³⁸U for individual uranium particles were efficiently determined.     

A method for thickness determination of thin films of amalgamable metals by total-reflection X-ray fluorescence

A method for thickness determination of thin amalgamable metallic films by total-reflection X-ray fluorescence (TXRF) is presented. The peak’s intensity in TXRF spectra are directly related to the surface density of the sample, i.e. to its thickness in a homogeneous film. Performing a traditional TXRF analysis on a thin film of an amalgamated metal, and determining the relative peak intensity of a specific metal line, the layer thickness can be precisely obtained. In the case of gold thickness determination, mercury and gold peaks overlap, hence we have developed a general data processing scheme to achieve the most precise results.     

TEVA树脂分离-ICP-MS测量钍基体中微量铀

针对233 U提取工艺1AW钍基体中微量铀(m(Th)/m(U)=105)的分析,以TEVA树脂萃取色谱为主要分离纯化手段,以ICP-MS为测量手段,建立了一个简便快速的分析方法。上柱时模拟料液的体积为1mL、酸度为2.5mol/L,铀的洗脱液为12mL硝酸(2mol/L),方法对1AW模拟样品中铀的回收率为97.1%~100.0%,sr=1.1%(n=5)。该方法能够有效地将钍基体去除,从而实现微量铀的准确测量。     

Total reflection X-ray fluorescence analysis using polycapillaries. A comparison with conventional setups

The possibility of producing parallel X-ray beams with low divergence by means of half monolithic polycapillaries gives the impression to be useful in total reflection X-ray fluorescence (TXRF) experiments. On one hand, the use of polycapillaries facilitates the alignment and the setup of the experiment. As expected, the spectra registered in the experiment shown low background and good signal-noise ratio. On the other hand, the intensity of photons on the samples when polycapillaries are employed is lower than in other configurations, which produces a loss of efficiency for the excitation of the sample mainly for light elements. In this work, different TXRF experiments were carried out and the minimum detection limits attained were compared with the ones obtained from TXRF using polycapillaries. The results indicate that the decrease of intensity produced by polycapillaries is imposing when detection limits are analyzed. Nevertheless, detection limits are better than conventional XRF. The possibility of employing non-symmetrical polycapillaries could eventually improve the detection limits so as to be equivalent to the conventional TXRF setups.     

全反射X射线荧光光谱法测定核废水中的铀和钍

建立了直接制样-全反射X射线荧光光谱法（TXRF）测定核废水中U、Th元素。以Ga做内标,方法的检出限分别为0.010、0.008 mg/L,标准溶液测量结果相对标准偏差小于7%（n=6）,加标回收率在95%~115%之间。通过TXRF法与电感耦合等离子体质谱法（ICP-MS）对未知样品的测量结果比较,两种方法测量结果一致,U和Th的线性回归方程的斜率分别约为0.93、1.0,线性相关系数分别为0.997、0.999。     

Quantitative Analysis of Heavy Metals in Water Based on LIBS with an Automatic Device for Sample Preparation

Heavy metals in water can be deposited on graphite flakes,which can be used as an enrichment method for laser-induced breakdown spectroscopy(LIBS) and is studied in this paper.The graphite samples were prepared with an automatic device,which was composed of a loading and unloading module,a quantitatively adding solution module,a rapid heating and drying module and a precise rotating module.The experimental results showed that the sample preparation methods had no significant effect on sample distribution and the LIBS signal accumulated in 20 pulses was stable and repeatable.With an increasing amount of the sample solution on the graphite flake,the peak intensity at Cu Ⅰ 324.75 nm accorded with the exponential function with a correlation coefficient of 0.9963 and the background intensity remained unchanged.The limit of detection(LOD) was calculated through linear fitting of the peak intensity versus the concentration.The LOD decreased rapidly with an increasing amount of sample solution until the amount exceeded 20 mL and the correlation coefficient of exponential function fitting was 0.991.The LOD of Pb,Ni,Cd,Cr and Zn after evaporating different amounts of sample solution on the graphite flakes was measured and the variation tendency of their LOD with sample solution amounts was similar to the tendency for Cu.The experimental data and conclusions could provide a reference for automatic sample preparation and heavy metal in situ detection.     

有源中子计数法测量铀总量方法研究

含铀物料中铀总量是核材料衡算与控制中最关注的信息之一,因非破坏性测量分析方法(NDA)不破坏样品,不产生二次废物,可对样品整体测量,因此常用作含铀物料中铀总量的测量分析.本研究基于有源中子计数法建立测量含铀物料中铀总量的新方法.对10组铀的标准样品进行测量分析,结果表明,测量误差为1.7％,小于5％,达到非破坏性分析技...     

CZT探测器测量核燃料组件铀丰度实验研究

采用CZT探测器、数字谱仪、准直器等组成了1套便携式CZT探测器铀丰度测量装置。该装置可对燃料组件铀丰度进行测定,以便确定相应铀产品丰度符合规定要求。实验研究中,对几类燃料组件丰度进了测量,建立了CZT探测器测量燃料组件铀丰度的方法。现场测量结果表明,铀丰度测量结果相对偏差小于3%,方法简单可靠,装置简便,能满足核材料保障监督和核设施现场测量中的需求。     

离子色谱分离-峰面积比值法测定核燃料元件中的钚

建立了用离子色谱法和峰面积比值法分离U并测量核燃料元件中钚的方法。该方法可以消除铀等基体的干扰，色谱条件在一定范围内变化时对测量结果无影响。在一定色谱条件下，通过实验获得相同含量的钚铀峰面积之比后，实际测量时可不采用钚标准溶液对仪器进行校准。方法的检出限为0.05 mg/L。该方法适用于各种乏燃料元件中钚含量的测定。     

Rapid Detection of Oil Pollution in Soil by Using Laser-Induced Breakdown Spectroscopy

Detection of oil pollution in soil has been carried out using laser-induced breakdown spectroscopy(LIBS). A pulsed neodymium-doped yttrium aluminum garnet(Nd:YAG) laser(1,064 nm, 8 ns, 200 mJ) was focused onto pelletized soil samples. Emission spectra were obtained from oil-contaminated soil and clean soil. The contaminated soil had almost the same spectrum profile as the clean soil and contained the same major and minor elements. However, a C–H molecular band was clearly detected in the oil-contaminated soil, while no C–H band was detected in the clean soil. Linear calibration curve of the C–H molecular band was successfully made by using a soil sample containing various concentrations of oil. The limit of detection of the C–H band in the soil sample was 0.001 mL/g. Furthermore, the emission spectrum of the contaminated soil clearly displayed titanium(Ti) lines, which were not detected in the clean soil. The existence of the C–H band and Ti lines in oil-contaminated soil can be used to clearly distinguish contaminated soil from clean soil. For comparison, the emission spectra of contaminated and clean soil were also obtained using scanning electron microscope-energy dispersive X-ray(SEM/EDX) spectroscopy,showing that the spectra obtained using LIBS are much better than using SEM/EDX, as indicated by the signal to noise ratio(S/N ratio).     

堆浸铀矿堆氡析出规律的实验研究

堆浸铀矿堆是铀矿山大气氡的主要来源之一。为了揭示堆浸过程中矿堆表面的氡析出规律,以我国南方某铀矿山新上堆的矿石为实验对象,利用自主设计并制造的改进型一维堆浸实验装置,采用局部静态法测定了不同喷淋状态下和排水过程中矿堆表面的氡析出率。结果表明:在布液和改变喷淋强度的瞬间,矿堆表面的氡析出率突然增大,之后随着喷淋的进行而逐渐减小并趋于稳定,且喷淋强度越大,稳定期间的氡析出率反而越小;在排水过程中,氡析出率先迅速减小,而后逐渐增大趋于稳定。     

Influence of void fraction change on plutonium and minor actinides recycling in BWR with equilibrium burnup

A study on the influence of void fraction change on plutonium and minor actinides recycling in standard boiling water reactor (BWR) with equilibrium burnup model has been conducted. We considered the equilibrium burnup model since it is a simple time independent burnup method that can handle all possible produced nuclides in any nuclear system.

The uranium enrichment for the criticality of the reactor diminishes significantly for the plutonium and minor actinides recycling case compared to that of the once-through cycle of BWR case. This parameter decreases much lower with the increasing of the void fraction. A similar propensity was also shown in the required natural uranium per annum. The annual required natural uranium was calculated by assuming that the uranium concentration in the tail of the enrichment plant is 0.25 w%. The amount of loaded fuel reduces slightly with the increment of the void fraction for plutonium and minor recycling in BWR.     

X-ray diffraction analysis of uranium tritide after aging for 420 days

Uranium tritide aging leads to continuous creation of decayed product ³He, vacancies, vacancy clusters, self interstitials, dislocations and helium bubbles. These defects result in the changes of material properties such as degradation of tritium storage, swelling, hardening and intergranular embrittlement. In our previous study, a simple hermetic sample holder that fits the Philip X’Pert Pro X-ray diffractometer has been developed for X-ray diffraction (XRD) analysis of uranium hydride. In order to help resolve unknowns regarding aging effects of uranium during long-term storage of tritium, XRD techniques with the hermetic method are applied to obtain the structural changes of aged uranium tritide. XRD analysis of uranium tritide aged for 420 days have shown that noticeable peak shifts appear in the diffraction patterns of uranium tritide, which indicate lattice distortion occurrence during the formation and growth of helium bubbles and other associated defects.     

Spectrometric method of evaluating spent nuclear fuel characteristics

A spectrometric method of identifying spent fuel assemblies according to the type of fuel elements present in them is described. The method is based on the results of spectrometric measurements and subsequent analysis of the radiation from fission products and the characteristic radiation from uranium in the irradiated fuel. The fuel assemblies used in the VVR-2 and OR research reactors contained fuel elements of a different type, differing by the initial quantity of uranium contained in them. To prepare the spent fuel assemblies for shipment to a reprocessing facility after long-time storage in cool-down pools, the assemblies must be sorted according to the type of fuel elements present in them. The method developed for identifying the types of fuel elements in the irradiated fuel is based on the dependence of the intensity of the characteristic radiation from uranium on the uranium content in a fuel element. The degree of excitation of the characteristic radiation of uranium also depends on the intensity of the radiation from fission products, which is monitored during the spectrometric measurements performed on the irradiated fuel; ultimately, this makes it possible to sort the spent fuel assemblies.     

水生植物大薸和凤眼莲对水中铀的去除

通过室内水培和静态吸附实验,研究了铀矿区土著水生植物大薸(Pistia stratiotes L.)和凤眼莲(Eichhornia crassipes)对真实铀矿坑水和不同铀浓度水中铀的去除能力。结果表明:干体大薸和凤眼莲根系以1g/L(干重)的比例投加至铀矿坑水(ρ0(U)=1.93mg/L,pH0=7.83)中,1h后,矿坑水中铀去除率分别达58%和48%,5d后铀质量浓度降至0.3mg/L以下;活体大薸和凤眼莲对水体中铀的去除作用主要集中在第1d内,单株鲜重约为400g左右的活体大薸在10min内可以将1Lρ0(U)=0.045~4.5mg/L的水体中铀质量浓度降至30μg/L以下,符合世界卫生组织建议的饮用水标准;单株鲜重约为400g左右的活体凤眼莲在1d内可以将1Lρ0(U)=0.5~4.5mg/L的水体中铀质量浓度降至国家标准(GB 23727—2009)规定值(0.05mg/L)以下。     

铀材料的识别

对铀材料的探测和识别进行了研究，给出了不同浓缩度铀的γ特征谱，并对其中＾２３５Ｕ与＾２３８Ｕ的丰度比和其γ射线强度比进行了分析。根据实验结果，可以直接由铀材料的γ特征谱得到其浓缩度，并计算出该铀材料的质量。     

Measurements of natural concentrations of I in uranium ores by accelerator mass spectrometry

An accelerator mass spectrometry system is described and utilized for measurements of ¹²⁹I concentrations in natural and environmental samples. We report here on measurements of ¹²⁹I isotopic abundances in iodine reagents and in iodine of mineral origin and of ¹²⁹I concentrations in uranium ores of different origins. The ¹²⁹I isotopic abundances for two measured contemporary iodine reagents and for iodine from a deep underground brine are 1.3 × 10⁻¹³ and about 4 × 10⁻¹⁴, respectively. ¹²⁹I/U ratios in the range 10⁻¹³–10⁻¹² are measured and compared to a simple model of ¹²⁹I production by spontaneous and induced fission of uranium. No clear correlation with the uranium concentrations or residence times is observed.     

球形浓缩铀装置的中子价值和裂变率分布测量

为得到Rossi-α测量临界装置的瞬发中子衰减常数的空间修正因子，利用²⁵²Cf中子源测量带贫化铀反射层的球形浓缩铀临界装置(CFBR-Ⅱ)的中子价值空间分布，同时用浓缩铀裂变电离室测量该装置的裂变率空间分布，得到该装置的空间修正因子为1.096。     

微波消解-激光荧光法测定土壤样品中微量铀

建立了一种快速、准确的分析测量土壤样品中微量铀的方法:微波消解样品-激光荧光法。该法利用微波消解技术极大地缩短了样品前处理时间,将前处理速度提高了十几倍,回收率可达到95%以上,同时避免了多个样品同时处理过程中交叉污染的问题。当样品溶液的pH值在6.5~7.5时,荧光强度最高,UO2+2与荧光增强剂形成的络合物最稳定,测量灵敏度最高,在实际样品测量时,应及时调节样品溶液的酸度,以及加入硝酸体系铀标准溶液后溶液的酸度;荧光增强剂、样品溶液、标准溶液等应提前放入仪器间,待温度稳定后再上机测定。仪器放置在温度相对稳定的房间,测定最佳室温为20~25℃。本方法的检出限为0.009μg/g,对于1.4~6.5μg/g的样品,方法精密度优于10%(n=9)。     

Impact of different moderator ratios with light and heavy water cooled reactors in equilibrium states

As an issue of sustainable development in the world, energy sustainability using nuclear energy may be possible using several different ways such as increasing breeding capability of the reactors and optimizing the fuel utilization using spent fuel after reprocessing as well as exploring additional nuclear resources from sea water. In this present study the characteristics of light and heavy water cooled reactors for different moderator ratios in equilibrium states have been investigated. The moderator to fuel ratio (MFR) is varied from 0.1 to 4.0. Four fuel cycle schemes are evaluated in order to investigate the effect of heavy metal (HM) recycling. A calculation method for determining the required uranium enrichment for criticality of the systems has been developed by coupling the equilibrium fuel cycle burn-up calculation and cell calculation of SRAC 2000 code using nuclear data library from the JENDL 3.2. The results show a thermal spectrum peak appears for light water coolant and no thermal peak for heavy water coolant along the MFR (0.1 ? MFR ? 4.0). The plutonium quality can be reduced effectively by increasing the MFR and number of recycled HM. Considering the effect of increasing number of recycled HM; it is also effective to reduce the uranium utilization and to increase the conversion ratio. trans-Plutonium production such as americium (Am) and curium (Cm) productions are smaller for heavy water coolant than light water coolant. The light water coolant shows the feasibility of breeding when HM is recycled with reducing the MFR. Wider feasible area of breeding has been obtained when light water coolant is replaced by heavy water coolant.