Chaplin Joshua D, Christl Marcus, Straub Marietta, Bochud François, Froidevaux Pascal
Institute of Radiation Physics, Lausanne University Hospital and University of Lausanne, 1 Rue du Grand-Pré, Lausanne CH-1007, Switzerland.
Laboratory of Ion Beam Physics, ETH Zürich, Otto-Stern-Weg 5, Hönggerberg, Zürich 8093, Switzerland.
ACS Omega. 2022 Jun 2;7(23):20053-20058. doi: 10.1021/acsomega.2c01884. eCollection 2022 Jun 14.
Spent nuclear fuel must be carefully managed to prevent pollution of the environment with radionuclides. Within the framework of correct radioactive waste management, spent fuel rods are stored in cooling pools to allow short-lived fission products to decay. If fuel rods leak, they liberate radionuclides into the cooling water; therefore, it is essential to determine radionuclide concentrations in the pool water for monitoring purposes and to plan the decommissioning process. In this work, we present, to our knowledge, the first passive sampling technique for measures of actinides in spent nuclear fuel pools, based on recently developed diffusive gradients in thin-film (DGT) configurations. These samplers eliminate the need to retrieve and handle large samples of fuel pool water for radiochemical processing by immobilizing their targeted radionuclides in situ on the solid phase within the sampler. This is additionally the first application of the DGT technique for Cm measure. Herein, we make the calibrated effective diffusion coefficients of U, Pu, Am, and Cm in borated spent fuel pool water available. We tested these samplers in the fuel pool of a nuclear facility and measured samples using accelerator mass spectrometry to provide high-precision isotopic reports, allowing for the first independent implementation of a recently developed technique for dating nuclear fuel based on its Cm isotope signature.
必须对乏核燃料进行妥善管理，以防止放射性核素污染环境。在正确的放射性废物管理框架内，乏燃料棒存放在冷却池中，以使短寿命裂变产物衰变。如果燃料棒发生泄漏，它们会将放射性核素释放到冷却水中；因此，为了监测和规划退役过程，确定池水中放射性核素的浓度至关重要。在这项工作中，据我们所知，我们基于最近开发的薄膜扩散梯度（DGT）配置，提出了第一种用于测量乏核燃料池中锕系元素的被动采样技术。这些采样器通过将目标放射性核素原位固定在采样器内的固相上，消除了为进行放射化学处理而采集和处理大量燃料池水样的需求。这也是DGT技术首次用于测量锔。在此，我们给出了硼化乏燃料池水中铀、钚、镅和锔的校准有效扩散系数。我们在一个核设施的燃料池中对这些采样器进行了测试，并使用加速器质谱法对样品进行测量，以提供高精度的同位素报告，从而首次独立应用了一种基于锔同位素特征对核燃料进行年代测定的最新技术。
