Environmental behaviors of spent nuclear fuel and canister materials

Environmental behaviors of spent nuclear fuel and canister materials
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DOI:
10.1039/c0ee00582g
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发表时间:
2011-07
影响因子:
32.5
通讯作者:
D. Cui;J. Low;K. Spahiu
D. Cui;J. Low;K. Spahiu
中科院分区:
材料科学1区
文献类型:
--
作者:
D. Cui;J. Low;K. Spahiu

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本文介绍了世界上第一个乏燃料贮存库(瑞典KBS-3)的概念,并报道了在处置初期可能发生漏罐的情况下,乏燃料和漏罐材料的环境行为实验结果。在脱氧合成地下水(2 mM NaHCO 3)中,在辐射(γ 0.9戈伊h−1)下,裂变产物(137 Cs,90 Sr和99 Tc)和锕系元素(238 U,237 Np)的库存部分浸出率分别约为每天10−6和10−7。铸铁罐表面被发现能够吸收从乏燃料中溶解的238 U、90 Sr、99 Tc和237 Np,但铜表面不能。在水辐解产生的氧化物种的存在下,废罐材料、铜和铸铁的腐蚀速率分别为1和30 μm/年。用0.1大气压H2平衡的浸出液中的乏燃料的不显著的溶解的观察被解释为在裂变产物合金颗粒(Mo-Tc-Ru-Rh-Pd)作为催化剂和溶解的Fe(II)在地下水中的存在下的H2的还原作用。本文还讨论了铁沉淀物对乏燃料溶解的包覆作用。
The world's first spent nuclear fuel repository concept (Swedish KBS-3) is illustrated and the results of experiments on environmental behaviors of spent fuel and canister materials under a potential canister breaching at early stage of disposal are reported. In a deoxygenated synthetic groundwater (2 mM NaHCO3) under radiation (γ 0.9 Gy h−1), inventory fraction leaching rates of fission-products (137Cs, 90Sr and 99Tc) and actinides (238U, 237Np) from a spent fuel segment were found to be around 10−6 and 10−7 per day, respectively. A cast-iron canister surface was found to be able to immobilize 238U, 90Sr, 99Tc and 237Np dissolved from spent fuel, but a copper surface could not. In the presence of the oxidative species generated from water radiolysis, the corrosion rates of waste canister materials, copper and cast-iron were found to be 1 and 30 μm per year, respectively. The observation of insignificant dissolution of spent fuel in the leaching solution equilibrated with 0.1 atm H2 is explained by the reducing effects of H2 in the presence of fission-product alloy particles (Mo–Tc–Ru–Rh–Pd) as catalysts and dissolved Fe(II) in groundwater. The coating effect of ferric precipitates on spent nuclear fuel dissolution is also discussed.