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核废料处置中的移动裂变和活化产物。

Mobile fission and activation products in nuclear waste disposal.

作者信息

Grambow Bernd

机构信息

SUBATECH, Ecole des Mines de Nantes, Université de Nantes, IN2P3/CNRS, 4, rue Alfred Kastler, 44307 Nantes, France.

出版信息

J Contam Hydrol. 2008 Dec 12;102(3-4):180-6. doi: 10.1016/j.jconhyd.2008.10.006. Epub 2008 Oct 17.

Abstract

When disposing nuclear waste in clay formations it is expected that the most radiotoxic elements like Pu, Np or Am move only a few centimetres to meters before they decay. Only a few radionuclides are able to reach the biosphere and contribute to their long-term exposure risks, mainly anionic species like I129, Cl36, Se79 and in some cases C14 and Tc99, whatever the scenario considered. The recent OECD/NEA cosponsored international MOFAP workshop focussed on transport and chemical behaviour of these less toxic radionuclides. New research themes have been addressed, such as how to make use of molecular level information for the understanding of the problem of migration at large distances. Diffusion studies need to face mineralogical heterogeneities over tens to hundreds of meters. Diffusion rates are very low since the clay rock pores are so small (few nm) that electrostatic repulsion limits the space available for anion diffusion (anion exclusion). The large volume of traversed rock will provide so many retention sites that despite weak retention, even certain of these "mobile" nuclides may show significant retardation. However, the question how to measure reliably very low retention parameters has been posed. An important issue is whether redox states or organic/inorganic speciation change from their initial state at the moment of release from the waste during long term contact with surfaces, hydrogen saturated environments, etc.

摘要

在黏土地层中处置核废料时,预计钚、镎或镅等毒性最强的放射性元素在衰变前仅移动几厘米到几米。无论考虑何种情况,只有少数放射性核素能够到达生物圈并造成长期暴露风险,主要是阴离子物种,如碘 - 129、氯 - 36、硒 - 79,在某些情况下还有碳 - 14和锝 - 99。经合组织/核能机构最近共同主办的国际MOFAP研讨会聚焦于这些毒性较小的放射性核素的迁移和化学行为。会议探讨了一些新的研究主题,例如如何利用分子层面的信息来理解远距离迁移问题。扩散研究需要面对数十米到数百米范围内的矿物学非均质性。由于黏土岩孔隙非常小(几纳米),静电排斥作用限制了阴离子扩散的可用空间(阴离子排斥),所以扩散速率非常低。大量穿过的岩石会提供众多的滞留位点,即便滞留作用微弱,某些这类“可移动”的核素甚至也可能表现出显著的滞留。然而,人们提出了如何可靠地测量极低滞留参数的问题。一个重要问题是,在与表面、氢饱和环境等长期接触的过程中,氧化还原状态或有机/无机形态是否会从其在从废料中释放时的初始状态发生变化。

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