SIMS含铀微粒同位素比分析中多原子离子影响及消除方法研究

实际环境样品基体成分十分复杂,多原子离子对二次离子质谱(SIMS)单微粒铀同位素比分析的影响不可忽略。本文实验分析了Pb、Ni、Zn、Si的多原子离子在SIMS单微粒铀同位素比分析中的干扰,并分别采用提高质量分辨率以及根据核素离子强度扣除其多原子离子的方法对结果进行校正。结果表明：Pb和Ni的多原子离子会影响含铀微粒次同位素比的测量,对铀主同位素比的影响可忽略;Zn和Si的多原子离子对铀主、次同位素比测量均基本无影响。将质量分辨率提高至800,能完全消除Ni多原子离子的影响,Ni-CRM U030混合（Ni粉混合CRM U030）微粒²³⁴U/²³⁸U同位素比测量值与参考值之间的相对偏差基本好于5%,²³⁶U/²³⁸U同位素比测量值与参考值之间的相对偏差基本好于15%;Pb多原子离子干扰无法通过提高质量分辨率进行消除,根据Pb离子强度扣除其多原子离子后,Pb-CRM U030混合微粒的²³⁴U/²³⁸U同位素比测量值与参考值之间的相对偏差基本好于10%,²³⁶U/²³⁸U同位素比测量值与参考值之间的相对偏差基本好于50%。将以上消除干扰的方法应用于真实样品分析,结果表明,其有效消除了多原子离子带来的干扰。     

Roadside dust contamination with toxic metals along industrial area in Islamabad,Pakistan

An investigation has been carried out to understand the contamination characteristics of roadside dust in the industrial area of Islamabad, Pakistan. The amounts of Si, S, Cl, K, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Pb, Zn, Ga, As, Se and Cd were determined from 95 roadside dust samples collected along the Islamabad industrial area using Proton Induced X-ray Emission （PIXE）. The results indicated that concentrations of all elements, except Cd, in the roadside dust were significant. The results of the enrichment factor show that the elementary composition of the roadside dust could be categorized as soil elements from the crust of the earth and elements from anthropogenic pollution. The high enrichment factors imply that elements such Cr, Cu, Pb, Zn, As, Se, Cd, Ni, Co and S came from anthropogenic activities. The source of metal contamination was identified using multivariate statistical analysis. It has been concluded that Ca, Sc, Ti, V, Mn and Fe mainly originate from crustal sources; Cr, Cu, Ni, Pb, Zn and Ga are associated with point-sources from industrial pollution/traffic; and S, Cl, K, As and Se are mainly related to oil/coal combustion.     

恒星中子源~(13)C(α,n)~(16)O反应的研究

13 C(α,n)16 O是渐进巨星支(AGB)星中慢速中子俘获(s)过程的主中子源反应,而17 O 6.356 MeV1/2+阈下共振对13 C(α,n)16 O反应影响很大。本文使用HI-13串列加速器和Q3D磁谱仪,首次测量了13C(11B,7Li)17 O转移反应角分布,确定了影响13C(α,n)16 O反应最关键、最不确定的17 O(Ex=6.356MeV)阈下共振态的α宽度,从而得出天体物理能区13 C(α,n)16 O反应的天体物理S因子和反应率,澄清了国际上已有S因子数据间高达25倍的巨大分歧。AGB星s过程核合成网络计算表明:新反应率数据导致恒星中铅的丰度增加了25%。     

AG-MP-1M在氢溴酸体系中分离镉的方法

Cd同位素质谱分析中存在的质谱干扰有¹¹⁰Pd、⁷⁰Zn⁴⁰Ar、⁹⁵Mo¹⁶O、¹¹²Sn、¹¹³In、¹¹⁴Sn和⁹⁸Mo¹⁶O等。因此在分析前应将Cd元素与产生干扰的其他元素分离,以避免测量过程中的质谱干扰。目前分离Cd的常用方法通常采用盐酸体系,分离过程中存在Sn与Cd分离困难的问题,操作步骤繁琐且淋洗体积大。针对上述问题,本工作开发了用阴离子树脂AG-MP-1M在氢溴酸体系中分离Cd的方法,采用混合酸消解的方法将样品消解完全后,用1 mL 0.25 mol/L的氢溴酸溶解样品并上柱,用3 mL 0.25 mol/L氢溴酸淋洗后可将绝大部分Sn、Zn、Mo等元素分离,然后用1 mL 2 mol/L盐酸和3 mL 0.5 mol/L盐酸淋洗Pb等其它元素,最后,用3 mL 0.002 mol/L盐酸解吸Cd。实验表明Cd回收率可达99.1%,且能将Sn、Zn、Mo等产生干扰的元素完全分开。采用此方法分离Cd总的淋洗体积为10 mL,和之前文献报道的方法相比大量减少了淋洗体积。该方法提高了Cd的分离效果,节约了实验流程时间,可用于Cd含量测试和Cd同位素测试的前处理工作中。     

水平衡法与高温转化法在矿泉水氢氧稳定同位素测定中的应用

为了鉴别不同品牌矿泉水标注水源地信息真伪,对11种不同品牌饮用水的氢氧稳定同位素(δD和δ¹⁸O)进行测定。结果表明,水平衡法(GasBench-IRMS)和高温转化法(TC/EA-IRMS)的测定结果一致性较好,两种方法测定6种不同饮用水的δD和δ¹⁸O的平均差异分别为(0.6±1.59)‰和(0.02±0.13)‰。水平衡法需要较长的制备和测定时间,但δD和δ¹⁸O的测定精度明显优于高温转化法。11种饮用水δD和δ¹⁸O变化范围较大,其δD和δ¹⁸O受不同品牌饮用水的水源地降水影响形成明显的地域性。虽然无法区分矿泉水是否由其他类别饮用水伪造,但δD和δ¹⁸O可以为特定区域(如高海拔与沿海地区)以及产地相近的矿泉水水源地鉴别提供依据。     

Determination of O concentrations in musamples of biological fluids

The ¹⁸O(p, )¹⁵N reaction has been developed for the analysis of musamples of biological fluids containing ¹⁸O-enriched water. Samples as small as 50 μl have been used. Well characterized Ta₂O₅ targets were prepared from these fluids and irradiated with several hundred nA of protons from the 3 MV Van de Graaff at Lucas Heights. The broad (47 keV) 846 kV resonance in this reaction was used to measure ¹⁸O concentrations down to natural backgrounds (0.2 at.%) in a few minutes of accelerator running time. Concentrations of ¹⁸O from 0 to 5 at.% were measured in body fluids in small Australian lizards directly after doping with ¹⁸O-enriched water and then again after several days of roaming around in their natural desert environments. The changes in these levels were related to the metabolic rates of these animals.     

Trace elements in lake sediments measured by the PIXE technique

Lakes are ecosystems where there is a great potential of metal accumulation in sediments due to their depositional characteristics. Total concentration of trace elements was measured on a 50 cm long sediment core from the Infernão Lake, that is an oxbow lake of the Moji-Guaçu River basin, in the state of São Paulo, Brazil. Dating of the core shows up to 180 yrs old sediment layers. The use of the PIXE technique for elemental analysis avoids the traditional acid digestion procedure common in other techniques. The multielemental characteristic of PIXE allows a simultaneous determination of about 20 elements in the sediment samples, such as, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Rb, Sr, Zr, Ba, and Pb. Average values for the elemental composition were found to be similar to the bulk crustal composition. The lake flooding pattern strongly influences the time series of the elemental profiles. Factor analysis of the elemental variability shows five factors. Two of the factors represent the mineralogical matrix, and others represent the organic component, a factor with lead, and another loaded with chromium. The mineralogical component consists of elements such as, Fe, Al, V, Ti, Mn, Ni, K, Zr, Sr, Cu and Zn. The variability of Si is explained by two distinct factors, because it is influenced by two different sources, aluminum-silicates and quartz, and the effect of inundation are different for each other. The organic matter is strongly associated with calcium, and also bounded with S, Zn, Cu and P. Lead and chromium appears as separated factors, although it is not clear the evidences for their anthropogenic origin. The techniques developed for sample preparation and PIXE analysis was proven as advantageous and provided very good reproducibility and accuracy.     

福岛核事故向环境释放的Pu研究进展

福岛核事故向环境释放的放射性核素中包含了锕系元素Pu,其中以极毒组的239Pu、240Pu和高毒组的241Pu为主。本文总结并分析了针对福岛核事故向环境释放的Pu的相关研究。据估计,福岛核事故向环境中排放的239+240Pu总量约为109 Bq,是切尔诺贝利核事故排放量的万分之一。此次事故排放的Pu同位素原子比(240Pu/239Pu和241Pu/239Pu)及活度比(A(238Pu)/A(239+240Pu))明显异于全球沉降值,可作为事故中Pu溯源的判定依据。事故所排放的Pu全部来源于核电站1~3号反应堆堆芯而非乏燃料池。现有研究报道的数据表明,在福岛核电站周围30km范围内的陆地环境中存在来自核事故排放的Pu污染,污染相对严重的"热点"区域和该地区与核电站的相对位置没有明显关联,主要是受地形和降水的影响。而对于人们关心的海洋环境,来自福岛核事故的Pu污染非常小。核事故向海洋中排放的Pu相对于核事故前海洋环境中的Pu污染水平可忽略不计。     

三七各部位氢氧同位素特征及其与灌溉水关系

分析不同产地三七各部位(茎叶、芦头、块根、筋条、须根)及灌溉水中稳定氢氧同位素特征、相关性及影响因素,为其能否作为产地溯源指标提供技术支撑.在三七产区——广西靖西片区、云南文山片区、云南新拓展片区采集43个春三七样点植株和相应的灌溉水并测定其稳定氢氧同位素比率,现场测定经纬度、海拔,进行差异分析和相关性分析.结果表明,...     

Charged-particle activation methods for the analysis of carbon and oxygen in high-purity gallium

Methods for the instrumental analysis of C and O at trace level in high-purity gallium were developed. The ¹²C (d, n)¹³N and ¹⁶O(t, n)¹⁸F reactions were used between 2.5 and 3.5 MeV, allowing analyses down to tens of ppb/weight. The ¹⁶O(p, )¹³N reaction at 15 MeV was also used; in this case ¹³N has to be separated radiochemically.     

松嫩平原湖泊沉积物中有机质及碳酸盐中δ（^13C）影响因素分析

以松嫩平原西部湖泊表层沉积为研究对象,通过对沉积物有机质正构烷烃组分的分析,了解了湖泊中有机质的来源和沉积环境。结合湖泊水介质和沉积物特征,综合分析了沉积物有机质对碳酸盐中碳同位素组成的影响。结果显示,湖泊沉积物中不同有机质类型对碳同位素组成有较大影响,生物有机质的大量输入使碳酸盐中碳同位素组成明显偏轻,而石油类污染物的输入对应于碳酸盐中的碳同位素组成稍偏重。     

锦屏深地核天体物理实验(JUNA)进展

锦屏深地核天体物理实验（JUNA）项目将利用中国锦屏深地实验室（CJPL）的良好条件,在天体物理伽莫夫能量窗口开展核天体关键反应²⁵Mg(p,γ)²⁶Al、¹⁹F(p,α)¹⁶O、¹³C(α,n)¹⁶O和¹²C(α,γ)¹⁶O的直接测量。目前已成功完成400 kV强流加速器和ECR离子源的研发,获得了400 keV、10 mA的质子束流和一价氦离子束流及800 keV、2 mA二价氦离子束流。大功率固体靶的研制及实验数据获取系统的建立也已成功完成。超低本底快中子探测器、4π BGO探测器阵列以及大立体角带电粒子探测器阵列已研制组装完成,并测量了地面和锦屏地下实验室的本底水平。总体来说,JUNA项目整体进展顺利,完成了中期设立的目标并通过了基金委评估（A级）和国际评估。     

湖泊沉积物中污染有机质及碳酸盐的δ13C影响因素分析

摘要：本文以松嫩平原湖泊表层沉积为研究对象。通过对沉积物有机质正构烷烃组分的分析,了解湖泊中有机质的来源和沉积环境。结合湖泊水介质和沉积物特征,综合分析了沉积物有机质和碳酸盐碳同位素组成的影响因素。结果显示出湖泊沉积物中不同有机质类型对碳同位素组成有较大的作用,生物有机质的大量输入使碳酸盐的碳同位素组成明显偏轻,而石油类污染的输入对应于碳酸盐中的碳同位素组成稍偏重。     

燃料元件破坏性燃耗测量过程的质量控制

燃耗是核燃料元件最重要的性能指标之一,其准确测量对新型燃料元件研制和换料周期确定等具有重要意义。破坏性燃耗测量属于强放射性下的精细化学分析,需建立系统的方法对测量过程进行质量控制,确保测量数据准确可靠。本文从方法适用性分析、数据预估、质谱干扰分析、样品污染分析、多种方法验证等方面介绍了破坏性燃耗测量过程质量控制的方法。剖析了重同位素法、¹⁴⁸Nd监测体法、¹⁴⁵Nd+¹⁴⁶Nd监测体法、¹³⁷Cs监测体法等的优缺点和适用范围。介绍了由裂变产额比值预估钕同位素丰度比、由铀同位素丰度比预估燃耗值的方法。分析了质谱测量时由Ce和Sm同位素造成的同量异位素干扰及其检测、排除手段。针对天然本底污染和样品间的交叉污染,分别论述了两种污染源的判断和修正技巧。还探讨了对燃耗值、稀释剂浓度、同位素丰度比等关键数据进行对比验证的方法。     

西北太平洋表层海水中239+240Pu浓度及240Pu/239Pu同位素比

钚是与核工业密切相关的敏感元素,是来源于人类核活动、以痕量或超痕量水平存在于环境中的重要锕系元素。与陆地土壤中钚的环境行为不同,输入到海洋环境中的钚会随洋流路径进行远距离迁移扩散。因此,对于包括我国近海在内的西北太平洋区域海水,除受全球沉降影响外,还长期受到美国太平洋核试验场（PPG）所造成区域污染的显著影响。本文利用从相关报道中收集的数据,对西北太平洋表层海水中钚浓度及同位素比的分布特征进行了分析。结果表明,2000年至今,西北太平洋表层海水中^239+240Pu浓度和²⁴⁰Pu/²³⁹Pu同位素比分别在1.15~22.3 mBq/m³和0.184~0.31间变化,其中,^239+240Pu浓度分布与西北太平洋各区域的环境条件等密切相关,而²⁴⁰Pu/²³⁹Pu分布则相对均匀,后者在除中国南海以外的西北太平洋地区均值为0.247±0.025(1σ),据此估算得美国太平洋核试验场区域污染输入的钚对该海域表层海水中钚的贡献约占其总活度的45%。此外,本文还对福岛核电站附近海域中核事故前后钚的相关数据进行了分析对比,未观察到该事故对西北太平洋海域中钚分布的影响。     

Low energy radioactive beams by inversion kinematics

Kinematically focussed radioactive beams of energies lower than 10 MeV/nucleon were produced by means of inversion kinematic in heavy ion induced reactions on ¹H. The characteristics of the produced radioactive beam were examined with the view of performing scattering and reaction experiments. On the basis of these results, a new beamline was constructed to collect and focus the radioactive beams. Using this beamline the elastically scattered spectra of ¹⁵O obtained from the ¹H(¹⁵N, ¹⁵O) reaction were observed with an energy resolution better than 0.6 MeV.     

铬电镀工头发中重金属元素含量的测定和分析

头发是人体内重金属元素的排泄器官之一,头发中的重金属元素含量是体内重金属含量的一种反映。由于头发收集、运输、保存和处理较为方便,被检测对象也乐于接受,因此,国内外有关头发分析的报道很多。 随着工业的发展和文明建设的需要,对环境污染引起的疾病日益重视。职业病是环境医学的一个重要方面,而重金属元素的危害又是职业病的一个主要因素。众所周知,人体对各     

自动电位滴定硼浓度方法在MOFs对硼同位素分离效果测定中的应用

金属 有机骨架（MOFs）材料作为吸附剂具有吸附硼同位素的潜力,为系统研究硼同位素效应,本文建立测定硼酸溶液中硼浓度的自动电位滴定法,以三种MOFs为例测定其对硼同位素的分离效果。采用弱酸强化法,甘露醇用量为理论用量的4倍,硼酸标准物质的测量值与参考值之差最小（-0.000 13 g）,方法的测量不确定度为0.000 2~0.000 8,测量精度为0.10%~0.40%,方法有效、可靠。应用建立的自动电位滴定法测定吸附前、后硼酸溶液的硼浓度,用MC-ICP-MS测定吸附前、后硼酸溶液的硼同位素丰度比¹⁰B/¹¹B,以Cu-MOF-OCH₃、UiO-66-NH₂、MIL-101(Cr)-2,3-OH三种MOFs材料为例,测定其对硼同位素的静态分离效果。结果表明,Cu-MOF-OCH₃、UiO-66-NH₂和MIL-101(Cr)-2,3-OH对硼同位素的分离因子(S)分别为1.066、1.037和1.079,均大于商用树脂Amberlite IR743的S（1.027）,其中,Cu-MOF-OCH₃对¹⁰B的10/11S>1,UiO-66-NH₂、MIL-101(Cr)-2,3-OH对¹¹B的^11/10S>1。本结果可为系统研究MOFs材料对硼同位素的分离效果提供参考。     

Elemental depth profiles in marine sediments of Singapore coastal waters

Thirty-eight core sediment samples were recently collected from different locations of the Singapore coastal region. The aim of the project was to trace the history of marine pollution in various coastal regions and to determine the impact of industrial activities. Two nuclear analytical techniques were employed in this study: particle induced X-ray emission (PIXE), Rutherford backscattering (RBS) as well as X-ray fluorescence (XRF). Combined together these techniques provide an excellent tool to determine elemental concentrations of more than 30 elements with detection limits as low as few ppm. Our results show that elemental concentrations in most of the regions do not show a significant variation with depth. However, in regions where industrial and shipping activities are high, for example the Port of Singapore area and the northern part of Johore Straits, the concentrations of metals like Cr, Ni, Cu, Zn, Sn and Pb were found to have an obvious decreasing trend with the depth. In these cores, concentrations in the top 10–15 cm were sometimes ten times higher than the corresponding base line concentrations. Elemental depth profiles of Ni, Cu, Zn, As, Sn and Pb and their mean concentrations in various regions are reported and discussed.     

Proton-induced γ-ray analysis of lithium in thick samples

A method for proton-induced γ-ray analysis (PIGE) of Li (either elemental or isotopic composition) in thick samples is presented in this work, which is based on a code that integrates the nuclear reaction excitation function, measured at the same experimental conditions, along the depth of the sample. The energy steps needed to define accurately the excitation function are used as energy intervals for the integration procedure. The excitation function and cross-sections of the reaction ⁷Li(p,p^′γ)⁷Li, for protons in the energy range 0.60–2.5 MeV, were obtained and used as input to calculate lithium concentrations in thick and intermediate samples. The calculated thick target yields of samples with several amounts of lithium were compared with the respective measured yields, showing that this is a reliable and accurate method for PIGE analysis of Li in thick samples.