热中子诱发239Pu裂变产物累积产额测量

Measurement of Cumulative Fission Product Yields from Thermal Neutron-induced Fission of 239Pu

  • 摘要: 中子诱发239Pu裂变产额是重要核数据,目前实验数据较少且部分不确定度较大。基于西安脉冲反应堆跑兔系统辐照Pu靶,开展了热中子诱发239Pu裂变的累积产额测量。针对不同半衰期的目标产物设计了3次辐照实验,采用标准面源等效刻度了石英封装样品的探测效率曲线,利用自研的γ全能峰干扰检索程序分析各目标产物特征γ能峰的干扰及大小,通过γ无损能谱法获取了辐照后靶中41条质量链上裂变产物的相对含量,以ENDF/B-Ⅷ.0评价数据库推荐的99Mo产额值为基准,经其他裂变核和非热中子成分等修正后得到了其他40种不同质量链上裂变产物的产额及不确定度,大多与数据库评价值及文献测量值在不确定度范围内一致。107Rh和127Sb的产额测量值较评价值偏小,但从测量方法和干扰扣除方面分析认为,与以往文献测量值相比,本文测量结果更可靠。实验测定的质量产额之和为149.3%,后续有必要借助放化方法开展更多质量链上裂变产物产额测量,以实现质量产额的200%归一。

     

    Abstract: As crucial nuclear data, the neutron-induced fission yield of 239Pu plays a vital role in nuclear engineering applications, technological developments, and theoretical studies of fission mechanisms. However, existing experimental data for 239Pu fission yields across varying neutron energies remain scarce and exhibit significant uncertainties, resulting in insufficient reliable data to support critical studies such as yield-energy relationships, yield-mass distributions, and yield-charge distributions. Therefore, it is necessary to conduct further experimental measurements to obtain higher-precision data. Based on the Xi’an Pulsed Reactor (XAPR) rabbit irradiation facility and quartz-encapsulated plutonium targets, a series of cumulative yield measurements for thermal neutron-induced 239Pu fission were carried out. A computational formula was derived to calculate the relative yields among various fission products based on their experimentally measured γ-ray peak areas. To account for the differences in half-lives and activities of the target fission products, three experiments with different irradiation durations and powers were designed by optimizing the experimental scheme using a self-developed fission product gamma-ray spectrum simulation program. After irradiation and appropriate cooling, the contents of fission products in the irradiated target were obtained using gamma-ray non-destructive spectrometry, with the measurement duration for a single spectrum ranging from 120 s to 10 d. The gamma-ray detection efficiency curves of non-destructive were calibrated by an equivalent method with several standard planar sources (57Co, 152Eu, 133Ba, 182Ta, and 24Na). To identify the sources and quantify the proportions of interference affecting the target energy peaks during data processing, a self-developed program for fission product gamma full-energy peak interference retrieval was employed. This method was compared with the traditional interference proportion subtraction approach, demonstrating good agreement between the two. However, the former method exhibits a broader scope of applicability. The relative quantitative relationships of the fission products on 41 mass chains such as 88Kr, 99Mo, 138Xe and 141Ce were obtained by processing the measured gamma-ray spectra. Using the 99Mo yield value recommended by the ENDF/B-Ⅷ.0 evaluated database as the benchmark, the yields of fission products on other 40 mass chains were determined after some corrections such as influence of non-primary neutron field and non-primary isotope. The uncertainty of the yield measurement results was evaluated, with the uncertainty of the characteristic gamma-ray emission probability being the dominant contributor. Most of the measured values in this work agree with the recommended values in evaluated databases and literature values within the uncertainties. Although the measured values of 107Rh and 127Sb obtained in this work are lower than the literature and evaluated values, the analysis suggests that the present measurement results are more reliable, due to the higher precision of the measurement instrument and the more accurate subtraction method for interference contributions. The sum of the experimentally determined mass chain yields is 149%, and reaches 198% after minor extrapolation and interpolation. To achieve the normalization of mass yields to 200%, it is necessary to conduct further measurements, particularly focusing on short-lived nuclides through the application of rapid chemical separation devices.

     

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