Pacific Northwest National Laboratory , 902 Battelle Boulevard, Richland, Washington 99354, United States.
Environ Sci Technol. 2015 Mar 3;49(5):3158-66. doi: 10.1021/es5053733. Epub 2015 Feb 12.
This paper extends the preliminary linear free energy correlations for radionuclide release performed by Schwantes et al., following the Fukushima-Daiichi Nuclear Power Plant accident. Through evaluations of the molar fractionations of radionuclides deposited in the soil relative to modeled radionuclide inventories, we confirm the initial source of the radionuclides to the environment to be from active reactors rather than the spent fuel pool. Linear correlations of the form In χ = −α ((ΔGrxn°(TC))/(RTC)) + β were obtained between the deposited concentrations, and the reduction potentials of the fission product oxide species using multiple reduction schemes to calculate ΔG°rxn (TC). These models allowed an estimate of the upper bound for the reactor temperatures of TC between 2015 and 2060 K, providing insight into the limiting factors to vaporization and release of fission products during the reactor accident. Estimates of the release of medium-lived fission products 90Sr, 121mSn, 147Pm, 144Ce, 152Eu, 154Eu, 155Eu, and 151Sm through atmospheric venting during the first month following the accident were obtained, indicating that large quantities of 90Sr and radioactive lanthanides were likely to remain in the damaged reactor cores.
本文扩展了 Schwantes 等人在福岛第一核电站事故后对放射性核素释放的初步线性自由能相关性的研究。通过评估沉积在土壤中的放射性核素相对于模型放射性核素库存的摩尔分馏，我们确认放射性核素最初进入环境的来源是来自于活性反应堆，而不是乏燃料池。我们采用多种还原方案计算了反应吉布斯自由能（ΔGrxn°(TC)），得到了沉积浓度与裂变产物氧化物还原势之间呈线性关系的形式，In χ = −α ((ΔGrxn°(TC))/(RTC)) + β。这些模型可以估计 2015 年至 2060 年之间 TC 的反应堆温度上限，为了解反应堆事故中裂变产物的蒸发和释放的限制因素提供了依据。通过计算，我们还得出了事故发生后第一个月通过大气排放释放的中等寿命裂变产物 90Sr、121mSn、147Pm、144Ce、152Eu、154Eu、155Eu 和 151Sm 的估计值，表明大量的 90Sr 和放射性镧系元素可能仍留在受损的反应堆堆芯中。
