乏燃料处置的必要性及其处置库环境化学行为

    Spent Fuel Disposal and Chemical Behaviors at Repository Environment

    • 摘要: 为了确保核燃料循环的安全性,不宜处理的乏燃料也应该同玻璃固化体一样作为高放废物进行深地质处置。本文综述了一些前期工作,归纳了空气侵入和水的辐解产生氧化性产物是导致乏燃料UO2基体氧化溶解的主要因素; 核燃料浸出实验结果显示铀和锕系镧系元素每天的浸出量是相应核素总量的1/107,比裂变产物的浸出速率小一个数量级。铁金属被各国选为高放废物处置容器材料的原因是其低价格、高强度和优秀的还原能力。在最不利的地下水侵入深地质处置库、近场处置容器防腐层破损的情景下,铁容器材料表面与地下水反应产生氢气,氢气通过还原反应消耗辐解产生的氧化性自由基和分子, 并能还原乏燃料表面的U(Ⅳ),大幅度减缓乏燃料的腐蚀和溶解;乏燃料中裂变产物贵金属合金颗粒对氢气有催化作用;处置容器表面铁金属能还原沉积溶解的多价态核素U(Ⅵ)、Np(Ⅴ)、Tc(Ⅶ)、Se(Ⅳ)和Se(Ⅵ)。希望本文对我国确立以铁基金属为处置容器材料的包括乏燃料在内的高放废物深地质处置概念有参考作用。

       

      Abstract: If not being reprocessed after safe storage period, spent fuel should be disposed as a high-level radioactive waste like vitrified waste. This article reviews some previously work and concludes that air intrusion and water radiolysis produced oxidative products should be the main substances causing oxidative dissolution of spent fuel UO2 matrix; nuclear fuel leaching experiment results indicate that uranium and other actinides and lanthanides display leaching rate around 1/107 of inventory of corresponding element per day which is an order of magnitude lower than the leaching rates of fission products. Iron metal is selected as the main material of high-level waste disposal containers by various countries due to its low price, high strength and high reducing capacity. In the most unfavorable scenario, where groundwater intrudes into deep geological repository near-field and disposal container is damaged, iron metal reacts with groundwater with generating hydrogen. Hydrogen consumes oxidizing free radicals and molecules produced by radiolysis through redox reaction and reduces the surface of spent fuel to greatly slow down the corrosion and dissolution of spent fuel; the fission product noble metal alloy particles in spent fuel display good catalytic effect on hydrogen; the surface of iron disposal container can reduce and precipitate multivalent nuclides. The authors hope this work is helpful as references in establishing the spent fuel deep geological disposal concept using iron-based metals as disposal container materials.

       

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