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Micron-sized spinel crystals in high level waste glass compositions: Determination of crystal size and crystal fraction
Journal of Nuclear Materials ( IF 3.1 ) Pub Date : 2018-11-30 , DOI: 10.1016/j.jnucmat.2018.11.039
C.E. Lonergan , K. Akinloye-Brown , J. Rice , V. Gervasio , N. Canfield , M.J. Schweiger , J.D. Vienna

The compositions utilized for immobilization of high-level nuclear wastes (HLW) are controlled using glass property models to avoid the deleterious effects of crystallization in the high-level waste (HLW) vitrification melters. The type and size of the crystals that precipitate during melter operations (typically at 1150 °C) and idling (∼1000 °C) are significantly impacted by glass composition and thermal history. This study was conducted to measure the impact of melt composition and heat treatment temperature on crystal size and fraction. A matrix of 31 multi-component glasses canvasing the expected Hanford HLW compositional space was developed and the glasses fabricated and heat treated at 850, 900, and 950 °C. The crystal amounts, as determined by X-ray diffraction, varied from 0.2 to 41.0 wt%. Spinel concentrations ranged from 0.0 to 13.8 wt%. One glass of the matrix did not precipitate spinel and contained 0.2 wt% RuO2, which was assumed to be undissolved from the melting process. All compositions contained crystals in the as-quenched glass. All of the spinel based crystals present in the glasses were less than 10 μm in diameter, as determined by scanning electron microscopy with image analysis. Composition and temperature dependent models were generated using the resulting data and the best model fit was obtained by only considering spinel concentrations (R2 = 0.87). Two glasses were unable to be characterized because of an inability to process the glass under the conditions of this study. Those glasses were utilized to give insight into a potential multi-component constraint to aid in future statistical composition designs.



中文翻译:

高含量废玻璃组合物中的微米级尖晶石晶体:晶体尺寸和晶体分数的测定

使用玻璃特性模型控制用于固定高级核废料(HLW)的组成,以避免在高级废料(HLW)玻璃化熔化器中结晶的有害影响。玻璃成分和热历程对熔炉运行期间(通常在1150°C下)和空转(约1000°C)期间析出的晶体的类型和大小产生显着影响。进行该研究以测量熔体组成和热处理温度对晶体尺寸和分数的影响。开发了31个多组分玻璃的矩阵,该玻璃覆盖了预期的Hanford HLW组成空间,并在850、900和950°C的温度下进行了制备和热处理。通过X射线衍射测定的晶体量为0.2至41.0重量%。尖晶石浓度范围为0.0至13.8重量%。图2中,假定其未从熔融过程中溶解。所有组合物在急冷玻璃中均包含晶体。如通过扫描电子显微镜和图像分析所确定的,存在于玻璃中的所有基于尖晶石的晶体的直径均小于10μm。使用所得数据生成成分和温度相关的模型,仅考虑尖晶石浓度即可获得最佳模型拟合(R 2  = 0.87)。由于无法在此研究条件下加工玻璃,因此无法鉴定出两种玻璃。那些眼镜被用来洞察潜在的多组分约束,以帮助将来的统计组成设计。

更新日期:2018-11-30
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