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镍在凯洛夫-牛津粘土中的滞留:现有稀溶液体系吸附模型在真实致密岩石中应用的适用性。

Nickel Retention on Callovo-Oxfordian Clay: Applicability of Existing Adsorption Models for Dilute Systems to Real Compact Rock.

机构信息

SUBATECH UMR6457, IMT Atlantique/CNRS-IN2P3/Université de Nantes, 4, Rue Alfred Kastler, F-44304 Nantes, France.

BRGM, 3 Avenue Claude Guillemin, F-45060 Orléans, France.

出版信息

Environ Sci Technol. 2020 Oct 6;54(19):12226-12234. doi: 10.1021/acs.est.0c04381. Epub 2020 Sep 25.

DOI:10.1021/acs.est.0c04381
PMID:32924461
Abstract

In a waste management context, predicting the mobility of contaminants is essential. A key issue entails assessing the applicability of current knowledge on adsorption processes to natural systems. Such is the focus herein for nickel in interaction with Callovo-Oxfordian (COx) clay rock, a formation selected in France for possible radioactive waste disposal. The challenge is to link predictive modeling results with the experimental data characterizing the behavior of the labile and naturally occurring Ni fraction by implementing a new simple method. Retention studies on compact systems serve to complete this work. Combined electron microprobe and laser ablation high-resolution inductively coupled plasma mass spectrometry data show that natural Ni (∼39 mg kg) is homogeneously distributed within the clay matrix, which corresponds to the main reservoir (∼70%). Data interpretation of desorption tests yields an value of ∼80 L kg and a labile Ni amount of ∼5 mg kg, that is, ∼13% of the Ni inventory. Predictive modeling explains the sorption data in considering that only weak clay fraction sites take part in the adsorption. The role of the clay matrix in Ni retention is confirmed by analyzing the Ni-spiked compact COx samples, whereby an increase of the Ni content in the clay fraction is observed following the retention experiment.

摘要

在废物管理的背景下,预测污染物的迁移性是至关重要的。其中一个关键问题是评估当前对吸附过程的认识在自然系统中的适用性。本文聚焦于镍与法国选定的可能用于放射性废物处置的库鲁索-奥克西唐(COx)黏土岩之间的相互作用,旨在利用一种新的简单方法,将预测模型结果与表征实验室中不稳定和自然存在的 Ni 部分行为的实验数据联系起来。在紧凑系统上进行的保留研究用于完成这项工作。电子探针和激光烧蚀高分辨率电感耦合等离子体质谱数据的组合表明,天然 Ni(约 39mg/kg)均匀分布在黏土基质中,这对应于主要的储存库(约 70%)。解吸试验的数据解释表明,值约为 80L/kg,可移动 Ni 的量约为 5mg/kg,即 Ni 总量的约 13%。考虑到只有弱的黏土部分位点参与吸附,预测模型解释了吸附数据。通过分析 Ni 掺杂的紧凑 COx 样品,证实了黏土基质在 Ni 保留中的作用,在保留实验后观察到黏土部分的 Ni 含量增加。

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