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首页> 外文期刊>Journal of Non-Crystalline Solids: A Journal Devoted to Oxide, Halide, Chalcogenide and Metallic Glasses, Amorphous Semiconductors, Non-Crystalline Films, Glass-Ceramics and Glassy Composites >Crystallisation of a simulated borosilicate high-level waste glass produced on a full-scale vitrification line
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Crystallisation of a simulated borosilicate high-level waste glass produced on a full-scale vitrification line

机译：在全尺寸玻璃化生产线上生产的模拟硼硅酸盐高级废玻璃的结晶

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摘要

A simulated (inactive) borosilicate high-level waste (HLW) glass was produced on a full-scale vitrification line with composition simulating vitrified oxide fuel (UO2) reprocessing waste. As-cast samples were compositionally homogeneous (Type I microstructure) and/or compositionally inhomogeneous displaying compositional 'banding' and frequently containing 'reprecipitated calcine' (Type II microstructure). Crystal phases identified in as-cast samples were: tetragonal RuO_2, cubic Pd-Te alloy, cubic (Cr,Fe,Ni,Ru)_3O_4, trigonal Na_3Li(MoO _4)_2?6H_2O, ostensibly cubic Zr 1 - x - yCexGdyO2 - 0.5y and a lanthanoid (Nd,Gd,La,Ce) silicate. Zr1 - x - yCexGd yO2 - 0.5y and lanthanoid (Nd,Gd,La,Ce) silicate were found exclusively in the Type II microstructure as component crystal phases of 'reprecipitated calcine'. Heat treated samples (simulating the retarded cooling experienced by actual (active) borosilicate HLW glasses after pouring) displayed extensive crystallisation and cracking (Type A microstructure) and/or 'banded' crystallisation (Type B microstructure) depending on their parent (as-cast) microstructure (Type I and/or Type II respectively). Crystal phases identified in heat treated samples were: tetragonal SiO_2 (α-cristobalite), tetragonal (Na,Sr,Nd,La)MoO4, cubic Ce1 - x - yZr xGdyO2 - 0.5y, a Ni-rich phase, a lanthanoid (Nd,Gd,La,Ce) silicate and orthorhombic LiNaZrSi6O15 (zektzerite). α-cristobalite was found exclusively in the Type A microstructure, while lanthanoid (Nd,Gd,La,Ce) silicate and zektzerite were only found in the Type B microstructure. Potential host phases for HLW radionuclides are: Pd-Te alloy (107Pd and 79Se), (Cr,Fe,Ni,Ru) 3O4 (63Ni), Zr1 - x - yCe xGdyO2 - 0.5y (93Zr, Pu and U), both lanthanoid (Nd,Gd,La,Ce) silicates (Am and Cm), (Na,Sr,Nd,La)MoO4 (90Sr, Am and Cm), Ce1 - x - yZrxGd yO_2 - 0.5y (93Zr, Pu and U), the Ni-rich phase (63Ni) and zektzerite (93Zr, 126Sn and U). Cracking in samples was attributed to thermal expansion mismatch between the borosilicate HLW glass matrix and RuO2, cristobalite (both α and β), (Na,Sr,Nd,La)MoO4 and zektzerite on cooling. There was also a contribution from the cristobalite α-β phase transition.
机译：在全尺寸玻璃化生产线上生产了模拟的（非活性）硼硅酸盐高放废物（HLW）玻璃，其组成模拟了玻璃化氧化物燃料（UO2）的后处理废物。铸态样品在成分上是均质的（I型微观结构）和/或在成分上是不均匀的，显示出成分“条带”，并经常包含“再沉淀的煅烧粉”（II型微观结构）。铸态样品中鉴定出的晶相为：四方RuO_2，立方Pd-Te合金，立方（Cr，Fe，Ni，Ru）_3O_4，三角Na_3Li（MoO_4）_2？6H_2O，表面立方Zr 1-x-yCexGdyO2- 0.5y和镧系元素（Nd，Gd，La，Ce）硅酸盐。 Zr1-x-yCexGd yO2-0.5y和镧系元素（Nd，Gd，La，Ce）硅酸盐仅在II型微结构中被发现为“再沉淀煅烧”的组分晶体相。热处理后的样品（模拟实际的（活性）硼硅酸盐HLW玻璃在浇注后经历的延迟冷却）根据其母体（铸态）显示出广泛的结晶和裂纹（A型微结构）和/或“带状”结晶（B型微结构）。 ）微结构（分别为I型和/或II型）。在热处理样品中鉴定出的晶相为：四方SiO_2（α-方石英），四方（Na，Sr，Nd，La）MoO4，立方Ce1-x-yZr xGdyO2-0.5y，富镍相，镧系元素（Nd ，Gd，La，Ce）硅酸盐和正交晶LiNaZrSi6O15（沸石）。仅在A型微结构中发现了α-方石英，而在B型微结构中仅发现了镧系元素（Nd，Gd，La，Ce）硅酸盐和沸石。 HLW放射性核素的潜在主体相为：Pd-Te合金（107Pd和79Se），（Cr，Fe，Ni，Ru）3O4（63Ni），Zr1-x-yCe xGdyO2- 0.5y（93Zr，Pu和U）镧系元素（Nd，Gd，La，Ce）硅酸盐（Am和Cm），（Na，Sr，Nd，La）MoO4（90Sr，Am和Cm），Ce1-x-yZrxGd yO_2-0.5y（93Zr，Pu和U ），富镍相（63Ni）和沸石（93Zr，126Sn和U）。样品开裂是由于硼硅酸盐HLW玻璃基质与RuO2，方石英（α和β），（Na，Sr，Nd，La）MoO4和zektzerite在冷却时的热膨胀不匹配所致。方石英α-β相变也有贡献。

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