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Glass-bonded iodosodalite waste form for immobilization of 129I
Journal of Nuclear Materials ( IF 2.8 ) Pub Date : 2018-03-20
Saehwa Chong, Jacob A. Peterson, Brian J. Riley, Diana Tabada, Donald Wall, Claire L. Corkhill, John S. McCloy

Immobilization of radioiodine is an important requirement for current and future nuclear fuel cycles. Iodosodalite [Na8(AlSiO4)6I2] was synthesized hydrothermally from metakaolin, NaI, and NaOH. Dried unwashed sodalite powders were used to synthesize glass-bonded iodosodalite waste forms (glass composite materials) by heating pressed pellets at 650, 750, or 850 °C with two types of sodium borosilicate glass binders. These heat-treated specimens were characterized with X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, energy dispersive spectroscopy, thermal analysis, porosity and density measurements, neutron activation analysis, and inductively-coupled plasma mass spectrometry. For the best waste form produced (pellets mixed with 10 mass% of glass binder and heat-treated at 750 °C), the maximum possible elemental iodine loading was 19.8 mass%, but only ∼8–9 mass% waste loading of iodine was retained in the waste form after thermal processing. Other pellets with higher iodine retention either contained higher porosity or were incompletely sintered. ASTM C1308 and C1285 (product consistency test, PCT) experiments were performed to understand chemical durability under diffusive and static conditions. The C1308 test resulted in significantly higher normalized loss compared to the C1285 test, most likely because of the strong effect of neutral pH solution renewal and prevention of ion saturation in solution. Both experiments indicated that release rates of Na and Si were higher than for Al and I, probably due to a poorly durable Na-Si-O phase from the glass bonding matrix or from initial sodalite synthesis; however the C1308 test result indicated that congruent dissolution of iodosodalite occurred. The average release rates of iodine obtained from C1308 were 0.17 and 1.29 g m-2 d-1 for 80 or 8 m−1, respectively, and the C1285 analysis gave a value of 2 × 10−5 g m-2 d-1, which is comparable to or better than the durability of other iodine waste forms.



中文翻译:

玻璃键合碘伏钠废料,用于固定129 I

固定放射性碘是当前和未来核燃料循环的重要要求。碘代钠盐[Na 8(AlSiO 46 I 2由偏高岭土,NaI和NaOH水热合成。干燥的未洗涤的方钠石粉末通过与两种类型的硼硅酸钠玻璃粘合剂在650、750或850°C下加热压制的颗粒,从而用于合成玻璃粘合的碘代钠废料形式(玻璃复合材料)。这些热处理过的样品的特征在于X射线衍射,傅立叶变换红外光谱,扫描电子显微镜,能量色散光谱,热分析,孔隙率和密度测量,中子活化分析以及电感耦合等离子体质谱。对于产生的最佳废料形式(将小丸与10质量%的玻璃粘合剂混合并在750°C进行热处理),元素碘的最大可能负载量为19.8质量%,但是热处理后,仅约8–9质量%的碘废物负载保留在废物形式中。其他具有较高碘保留率的颗粒或具有较高的孔隙率或未完全烧结。进行ASTM C1308和C1285(产品一致性测试,PCT)实验以了解在扩散和静态条件下的化学耐久性。与C1285测试相比,C1308测试导致归一化损失明显更高,这很可能是由于中性pH溶液更新的强大作用以及防止溶液中离子饱和的结果。两项实验均表明,Na和Si的释放速率高于Al和I的释放速率,这可能是由于玻璃键合基体或初始方钠石合成过程中Na-Si-O相的耐久性差。但是,C1308测试结果表明,碘伏钠完全溶解。从C1308获得的碘的平均释放速率分别为0.17和1.29 g·m对于80或8 m -1分别为-2  d -1,C1285分析得出的值为2×10 -5  g m -2  d -1,与其他碘废物形式的耐久性相当或更好。

更新日期:2018-03-20
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