A mechanistic model for long-term nuclear waste glass dissolution integrating chemical affinity and interfacial diffusion barrier
A mechanistic model for long-term nuclear waste glass dissolution integrating chemical affinity and interfacial diffusion barrier
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DOI：
10.1016/j.jnucmat.2017.01.001
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发表时间：
2017-04-01
影响因子：
3.1
通讯作者：
Han, Xiaoyuan
中科院分区：
文献类型：
--
作者：
Ma, Teqi;Jivkov, Andrey P.;Han, Xiaoyuan
了解核废料玻璃在地质处置库条件下的变化是分析处置库滞留功能的关键。玻璃改建的实验观察提供了以下制度的一般协议：相互扩散，水解过程，速率下降，残留率，并在非常特殊的条件下，恢复改建。其中，控制利率下降和剩余利率的机制仍然存在争议。本文提供了一个关键的审查与这些制度相关的两个最具竞争力的模型：亲和力限制溶解和扩散障碍。这些模型的局限性突出了他们的预测与现有的实验证据的比较。在综合分析现有模型的基础上，提出了一个新的机理模型，该模型将化学亲合势和扩散势垒概念相结合。它演示了如何模型可以解释实验现象和数据，现有的模型被证明是不充分的。(C)2017由Elsevier B.V.出版
Understanding the alteration of nuclear waste glass in geological repository conditions is critical element of the analysis of repository retention function. Experimental observations of glass alterations provide a general agreement on the following regimes: inter-diffusion, hydrolysis process, rate drop, residual rate and, under very particular conditions, resumption of alteration. Of these, the mechanisms controlling the rate drop and the residual rate remain a subject of dispute. This paper offers a critical review of the two most competitive models related to these regimes: affinity limited dissolution and diffusion barrier. The limitations of these models are highlighted by comparison of their predictions with available experimental evidence. Based on the comprehensive discussion of the existing models, a new mechanistic model is proposed as a combination of the chemical affinity and diffusion barrier concepts. It is demonstrated how the model can explain experimental phenomena and data, for which the existing models are shown to be not fully adequate. (C) 2017 Published by Elsevier B.V.