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Influence of non-equilibrium sorption on the vertical migration of 137Cs in forest mineral soils of Fukushima Prefecture
Journal of Environmental Radioactivity ( IF 1.9 ) Pub Date : 2021-03-06 , DOI: 10.1016/j.jenvrad.2021.106567
Hamza Chaif , Frédéric Coppin , Aya Bahi , Laurent Garcia-Sanchez

Sorption hypotheses and models are required for the prediction of 137Cs migration in soils contaminated after nuclear reactor accidents and nuclear weapons tests. In assessment models, the Kd (distribution coefficient) hypothesis for sorption, which assumes that sorption is instantaneous, linear and reversible, has often been coupled with the convection-diffusion equation (CDE) to model 137Cs migration. However, it fails to describe 137Cs migration velocities which often decrease with time. Alternative equilibrium-kinetic (EK) hypotheses of 137Cs sorption/desorption have been suggested by laboratory experiments but have not been fully validated in field conditions. This work addressed the influence and magnitude of non-equilibrium 137Cs sorption in field conditions by reinterpreting, with an inverse approach, series of 137Cs profiles measured in mineral soils of forest plots located in Fukushima Prefecture (2013–2018). Our results show that the inclusion of non-equilibrium sorption significantly improves, compared to the equilibrium hypothesis, the realism of simulated 137Cs profiles. Fitted sorption parameters suggest a fast sorption kinetic (half-time of 1–7 h) and a pseudo-irreversible desorption rate (half-time of 3.2 × 100–3.4 × 106 years), whereas equilibrium sorption (4.0 × 10−3 L kg−1 on average) only affects a negligible portion of 137Cs inventory. By June 2011, such EK parameters fitted on our plots realistically reproduced profiles measured in the same forest study site (Takahashi et al., 2015). Predictive modeling of 137Cs profiles in soil suggests a strong persistence of the surface 137Cs contamination by 2030, with exponential profiles consistent with those reported after the Chernobyl accident. This study demonstrates that hypotheses and parameters of 137Cs sorption can be partially inferred from in situ measurements. However, further experiments in controlled conditions are required to better estimate the sorption parameters and to identify the processes behind non-equilibrium sorption.



中文翻译:

非平衡吸附对福岛县森林矿物土壤中137 Cs垂直迁移的影响

吸附假设和模型是预测在核反应堆事故和核武器试验后受污染的土壤中137 Cs迁移所必需的。在评估模型中,假设吸附是瞬时的,线性的和可逆的,吸附的K d(分布系数)假设通常与对流扩散方程(CDE)耦合在一起以模拟137 Cs迁移。但是,它无法描述137 Cs迁移速度,该速度通常会随着时间而降低。137的其他平衡动力学(EK)假设实验室实验已经表明Cs的吸附/解吸,但在野外条件下尚未得到充分验证。这项工作通过反演方法,重新解释了在福岛县(2013–2018)森林地带的矿物土壤中测得的一系列137 Cs剖面,从而解决了田间条件下非平衡137 Cs吸附的影响和强度。我们的结果表明,与平衡假设相比,模拟的137 Cs分布图的真实性与非平衡吸附的包含相比得到了显着改善。拟合的吸附参数表明吸附动力学快(半峰时间为1–7 h)和拟不可逆的解吸速率(半峰时间为3.2×10 0 –3.4×10 6年),而平衡吸附(平均4.0×10 -3  L kg -1)仅影响137 Cs存量的可忽略部分。到2011年6月,在我们的样地上拟合的这些EK参数真实再现了在同一森林研究地点测得的剖面(Takahashi等人,2015)。对土壤中137 Cs剖面的预测模型表明,到2030年,表面137 Cs污染物的持久存在,其指数剖面与切尔诺贝利事故后报道的一致。这项研究表明,137 Cs吸附的假设和参数可以从原位部分推断出来测量。但是,需要在可控条件下进行进一步的实验,以更好地估计吸附参数并确定非平衡吸附背后的过程。

更新日期:2021-03-07
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