质谱、α谱联合测定钚年龄

介绍了用质谱和α谱相结合测定钚材料年龄的方法.该方法利用质谱计测得试样中239Pu相对于241Pu比、用α能谱仪测得试样中239Pu相对于241Am比,利用241Pu和241Am核素级联衰变关系及其参数进行数学运算,求得钚材料的年龄.     

不同级钚材料的衰变放热功率计算分析

钚材料中放射性核素会不断衰变并释放能量,改变钚材料及周围部件的温度。为研究不同级钚材料在其整装存储及运输过程中衰变放热功率随时间的变化规律,依据不同级钚材料的放射性核素组分,在分析核素级联衰变规律的基础上,并在物理模型中考虑衰变时的能量分支比,计算得到了武器级钚、反应堆级和混合级钚材料中各核素的衰变放热功率和总热功率随时间的演变规律。计算结果表明,1 kg不同级的钚材料,其衰变放热功率最大的是混合级钚,放热最少的是武器级钚;武器级钚材料衰变放热功率主要来自于~(239)Pu,而反应堆级与混合级钚材料的衰变放热功率主要来自于~(241)Pu和~(238)Pu。三种不同级钚材料中,~(242)Pu的衰变放热功率均很小。考虑能量分支比后,可更准确地计算给出钚材料的衰变热功率。     

同位素稀释一多接收电感耦合等离子体质谱测量痕量钚年龄的方法研究

对钚材料的来源及历史的鉴定在许多领域是非常重要的。年龄是在追溯核材料的历史时第一个需要被测定的参数。钚样品的年龄测定基于钚的同位素及其子体，即238Pu／234U、239Pu/235U、240Pu/236U和241Pu／241Am的原子比的测定。     

钚丰度、年龄测定技术研究

扼要地总结了利用自主开发的实用γ谱分析软件和~(239)Pu的γ能峰的相对效率,采用高纯锗探测器对耦合的γ能峰使用非耦合峰推算它的计数分配,从而得到各核素的原子比。根据钚的衰变规律,获得了分析钚材料的年龄、丰度的方法。推算出原子比与丰度、年龄的计算公式,获得了钚材料的年龄和丰度。对已知样品进行了重复测量,将研究分析的结果与PC-FRAM以及保管单位给出的参考值进行了比较。     

同位素稀释．萃取液闪法测量高放废液中的241Pu

在钚的238Pu、239Pu、240Pu、241Pu和242Pu5个同位素中，只有241Pu是β放射性核素，其余4个均为α衰变核素。241Pu的半衰期为14．29a，是钚同位素中放射性活度的主要贡献者，但能量很低（20．81keV），直接测量它的β放射性是较为困难的，对复杂体系来说尤其如此。     

钚中~(241)Am的测定方法

本文报道了用NaI(T1)γ谱仪和α谱仪测定钚中~(241)Am的两种方法。 (1)方法一 用~(241)Am和纯钚标准溶液标定γ谱仪60keV峰区的探测效率ε_(Am)和ε_(Pu),再用γ和α谱仪分别测量单位重量钚样品溶液的γ计数率γ(Am+Pu)和α衰变率α(Pu),则钚样品溶液中~(241)Am和钚的α放射性比为     

用HPGe和Ge(Li)探测器测定~(238)Pu,~(239)Pu,~(240)Pu,~(241)Pu丰度和~(241)Am含量

本文介绍了用γ能谱法精确测定浅燃耗钚样品的同位素丰度和~(241)Am相对含量的方法和实验结果。在38—60 keV钚的低能γ射线和203—208 keV两个能区中获取数据。选择不同同位素能量相近的γ射线对计算同位素丰度比,并对这些γ射线对的小的能量差别进行了仔细的效率修正,~(238)Pu,~(239)Pu,~(240)Pu,~(241)Pu丰度和~(241)Am相对含量的精度分别为±4.1%,±0.04%,±0.37%。±0.45%和±0.40%。与质谱仪测得结果相比,在误差范围内相互符合。     

液闪和α谱结合测量痕量钚样品中钚年龄

建立了液闪-α谱法测量241Pu/241Am原子数比得到痕量钚年龄的方法。基于钚、镅的分离,研究纳克量级钚样品的年龄测量技术。用该法分别对已知和未知年龄的钚样品进行了测量,结果表明,已知年龄的钚样品的测量结果与参考值基本一致。本工作建立的痕量钚年龄的测定技术有可能作为核保障和军备控制中钚材料的核查技术。     

动态法-多接收电感耦合等离子体质谱测量痕量钚同位素丰度

^239Pu和^240Pu的相对含量与钚的级别及其来源密切相关。由于环境样品中钚的含量一般低至皮克甚至亚皮克量级，MC—ICP—MS测量^240Pu和^239Pu时需选用离子计数器来接收钚的束流。离子计数器之间的效率差异和质谱仪器固有的质量偏倚是影响准确分析钚同位素丰度比的两个主要因素。由于缺乏^240Pu／^239Pu的同位素标准物质，只能采用现有的^242Pu/^239Pu同位素标准来保持数据的溯源性。     

Reillex-Reillex阴离子交换分离克量级铀中微量钚北大核心CSCD

采用Reillex-Reillex串联阴离子交换色层柱,建立了高铀钚比样品中微量钚的高效分离方法。考察了树脂类型、淋洗条件、价态调节等对钚分离效果的影响,确定了分离流程的条件。当铀钚质量比为106时,经两级Reillex柱分离后,钚的平均回收率为99.35%,铀的去污因子大于107。最后使用该方法从克量级辐照铀靶中分离出了微克量级超纯239 Pu,(^(238)U+^(238)Pu)/^(239)Pu原子比为(3.60±1.15)×10^(-5)(n=6)。     

α能谱法测定Pu材料中^241Am／Puα活度比

文章介绍用α能谱法测定Ｐｕ材料中＾２４１Ａｍ／Ｐｕα活度比的原理、方法及结果，该测定结果与用ＮａＩ（ＴＩ）γ能谱法测定的结果相一致。     

Determination of americium in plutonium based nuclear fuel materials: An assessment of different methodologies

Determination of americium (Am) is one of the requirements of chemical quality assurance of plutonium (Pu) bearing fuel materials. Though many methods are published for determining Am at picogram to femtogram levels in environmental and biological matrices, yet a few of them are used routinely for Pu based nuclear fuel samples. This paper gives a brief summary of the different analytical methods available and presents results of our experiments on the determination of Am in Pu bearing fuels using gamma spectroscopy. The methods utilizing gamma emissions from ²⁴¹Am and Pu isotopes are fast as they do not involve chemical separation of Pu and Am, do not require an accurate knowledge of the efficiency values of the detector systems and are not dependent on the availability of a radiometric standard for ²⁴¹Am. In addition, for aged Pu samples containing large amounts of ²⁴¹Am, there is no need for dilution and this reduces the volume of analytical radioactive waste solution. Future requirements of reference materials to validate different methodologies for determining Am isotopes are also highlighted.     

Radiochemical Determination of Plutonium Isotopes and Americium-241 in a Plutonium Sample

Isotopic ratios of ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu and ²⁴¹Am in a plutonium sample were approximately determined by means of combined α- and γ-ray spectrometry without chemical separation of americium from plutonium. The intensity of α-ray followed by internal conversion was determined by measuring the intensity of LX-rays. The ratio of ²⁴⁰Pu to ²³⁹Pu was obtained from the ratio between the α-ray intensity thus determined and the total α-ray intensity from the two nuclides.     

Peak identification of L X-ray spectra of elemental Np and U

The L X-ray photons emitted by transuranic (TRU) elements are expected to be useful for developing nondestructive TRU monitors. Energy spectra of L X-rays emitted by ²⁴¹Am, ²³⁸Pu and ²³⁹Pu sources were measured by a transition edge sensor (TES) microcalorimeter, which allowed precise peak identification with high energy resolution. In the measurements using the TES microcalorimeter, the full width at half-maximum energy resolution was 62.6 eV at 17.222 keV for ²³⁹Pu source, 62.5 eV at 17.222 keV for ²³⁸Pu source and 60.9 eV at 17.751 keV for ²⁴¹Am source. This study demonstrates the separation of ²⁴¹Am and plutonium isotopes by L X-ray spectroscopy using a TES microcalorimeter.     

基于NPL-NMC系统的γ测量子系统的建模与优化

在军控核查中,核部件的质量、丰度、年龄属性需采用无损方法进行核查,NPL-NMC系统是一套利用中子多重性测量核部件质量属性的装置,为建立完善的属性测量系统,还需在NPL-NMC系统的基础上建立γ测量子系统。本文通过设计γ测量子系统在NPL-NMC系统上的布局及对中子屏蔽的优化,使系统能对铀部件的丰度、年龄属性进行测量。模拟计算结果表明,该γ测量子系统能很好地满足军控核查对铀部件丰度、年龄属性测量的要求。     

高纯锗γ谱仪计数比法测量滤材样品中241Am/239Pu原子比

使用阱型高纯锗γ谱仪测量了待测滤材样品和参比溶液中²⁴¹Am 59.5 keV和²³⁹Pu 129.3 keV的能峰计数比,结合参比溶液中已知的²⁴¹Am/²³⁹Pu原子比数据给出了滤材样品的²⁴¹Am/²³⁹Pu原子比,结果与滤材样品经化学处理后采用同位素稀释质谱法测量的²⁴¹Am/²³⁹Pu原子比在不确定度范围内一致。     

Gamma-Ray Spectrometric Determination of Isotopic Ratios of Plutonium

Abstract

Plutonium samples (3–30 μg) of various isotopic compositions were measured with a high-resolution Ge(Li) detector. The γ-rays counted are the 43.5 keV of ²³⁸Pu, the 38.7, 51.6 and 129.3 keV of ²³⁹Pu, the 45.2 keV of ²⁴⁰Pu, and the 148.6 keV of ²⁴¹Pu. To estimate the relative photopeak efficiencies of the γ-rays, an empirical curve was derived from measurements of the three γ-rays of ²³⁹Pu adopted as internal standard. Data treatment is described in detail as well as the method of correction to account for the activities of ²³⁷U and ²⁴¹Am inherently accumulating in the plutonium sample. The branching ratios of the γ-rays of plutonium were also evaluated by comparing the γ-ray spectrometric results with mass-spectrometric data.     

Irradiation analysis of U, Am samples irradiated in experimental fast reactor “Joyo” for protected plutonium production in fast breeder reactor blanket

Americium is a key element to design the FBR based nuclear fuel cycle, because of its long-term high radiological toxicity as well as a resource of even-mass-number plutonium by its transmutation in reactors, which contributes the enhancement of proliferation resistance. The present paper summarizes analysis of the individual Am and U samples irradiation in Joyo to re-evaluate the results of Pu isotopes in the measure of proliferation resistance, and to combine the results for the prediction of DU-Am irradiation especially in the production of Pu isotopes. By the prediction of DU-Am oxide fuel in fast reactor environment with detail fuel irradiation analysis, it was confirmed that neutron moderation and fuel size affects the produced Pu isotope and its vector due to the very high sensitivity of ²³⁸U resonance capture reaction, the larger diameter fuel is more preferable in the case of moderated neutron spectrum environment for denaturing Pu in fast reactor blanket. Finally proliferation resistance of all the Pu produced in U, Am sample irradiation and DU-Am fuel irradiation prediction were evaluated based on decay heat and spontaneous fission neutron rate, and it was confirmed ²⁴¹Am produces un-attractive Pu to abuse from the beginning to the end of irradiation, and more than 2% of ²⁴¹Am doping is required to enhance the proliferation resistance of Pu to MOX grade and Kessler’s proposal in moderated neutron spectrum environment in fast reactor.     

乏燃料溶液嬗变堆焚烧锕系核素能力分析

针对焚烧锕系核素的目标,选择不同的乏燃料成分和堆芯功率,构造了7种乏燃料溶液嬗变堆( HSTR)堆芯模型,采用溶液堆堆芯燃料管理程序FMCHR计算了堆芯内Pu、Np及其他长寿命锕系核素的燃耗变化,分析了HSTR焚烧锕系核素的能力.结果表明:HSTR可以有效实现焚烧239pu的目标,同时嬗变可观数量的237Np;若要实现...     

某地区土壤中241Am和239Pu的化学形态

用连续提取法研究了某地区放射性污染土壤中241Am和239Pu的化学形态.结果表明,供试土壤样品中各级态241Am和239Pu都以一种优势形态即残渣态存在,其中241Am的残渣态含量达到总量的84%～91%,239Pu达到98%左右,其它各级态含量较少,这说明实验土壤中的241Am和239Pu主要赋存于土壤的原生和次生稳定矿物中,属于稳定的化学形态,在环境中的迁移活性较小.