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首页> 外文期刊>RSC Advances >Solubility, speciation and local environment of chlorine in zirconolite glass-ceramics for the immobilisation of plutonium residues
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Solubility, speciation and local environment of chlorine in zirconolite glass-ceramics for the immobilisation of plutonium residues

机译：锆石玻璃玻璃中氯气的溶解度，物种和局部环境用于固定钚残留物的玻璃陶瓷

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摘要

The immobilisation and disposal of fissile materials from civil and defence nuclear programmes requires compatible, passively safe and proliferation resistant wasteforms. In this study, we demonstrate the application of an albite glass-zirconolite ceramic material for immobilisation of chloride contaminated plutonium oxide residues in the United Kingdom. The chlorine solubility limit in the albite glass phase was determined to be 1.0 +/- 0.1 wt%, above the maximum envisaged chorine inventory of 0.5 wt%, attainable at a 20 wt% PuO(2)incorporation rate within the ceramic. Cl K-edge of X-ray Absorption Near Edge Spectroscopy (XANES) was exploited to confirm partitioning of Cl to the glass phase, speciated as the chloride anion, with exsolution of crystalline NaCl above the chlorine solubility limit. Combinatorial fitting of Cl XANES data, utilising a library of chemically plausible reference spectra, demonstrated the association of Cl with Na and Ca modifier cations, with environments characteristic of the aluminosilicate chloride minerals eudialyte, sodalite, chlorellestadite and afghanite. Adventitious incorporation of Ca, Zr and Ti within the albite glass phase apparently assists chlorine solubility, by templating a local chemical environment characteristic of the mineral reference compounds. The partitioning of Ce, as a Pu analogue, within the glass-ceramic was not adversely impacted by incorporation of Cl. The significance of this research is in demonstrating the compatibility of the glass-ceramic wasteform toward Cl solubility at the expected incorporation rate, below the determined solubility limit. Thus, an upstream heat treatment facility to remove chloride contamination, as specified in the current conceptual flowsheet, would not be required from the perspective of wasteform compatibility, thus providing scope to de-risk the technology roadmap and reduce the projected capital and operational plant costs.
机译：来自民用和国防核计划的固定和处理裂变材料需要兼容，被动安全和激增的抗性废物。在这项研究中，我们证明了Albate玻璃 - 锆石陶瓷材料的应用，以固定在英国的氯化物污染的钚氧化物残留物。将Albate玻璃相中的氯溶解度极限确定为1.0 +/- 0.1wt％，高于最大设想的浓度库存为0.5wt％，可在陶瓷内的20wt％puo（2）掺入速率下可获得。利用边缘光谱（XANES）附近的X射线吸收的CL k边缘以确认CL对玻璃相的分配，称为氯阴离子，在氯溶解度极限上方的结晶NaCl的eX展示。 Cl XANES数据的组合拟合，利用化学合理的参考光谱库，证明了CL与Na和Ca改性剂阳离子的关联，具有氯化铝硅酸盐矿物质，钠，氯甾醇盐和阿富汗的环境。通过模糊矿物参考化合物的局部化学环境，可在Albite玻璃相中的不定掺入Ca，Zr和Ti显然有助于氯溶解性。 Ce作为PU类似物，在玻璃陶瓷内的划分不会因掺入Cl而产生不利影响。该研究的重要性在于以低于确定的溶解度限制，表明玻璃陶瓷废物朝向CL溶解度的相容性。因此，上游热处理设施，以除去氯化物污染，如在当前的原理流程图说明，将不被从wasteform兼容性的角度看所需要，因此提供范围脱风险的技术路线图和降低投影资本和运营设备成本。

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  • 来源
    《RSC Advances》 |2020年第54期|共14页
  • 作者

    Thornber Stephanie M.; Mottram Lucy M.; Mason Amber R.; Thompson Paul; Stennett Martin C.; Hyatt Neil C.;

  • 作者单位

    Univ Sheffield Immobilisat Sci Lab Dept Mat Sci Sc Engn Sir Robert Hadfield Bldg Mappin St Sheffield S1 3JD S Yorkshire England;

    Univ Sheffield Immobilisat Sci Lab Dept Mat Sci Sc Engn Sir Robert Hadfield Bldg Mappin St Sheffield S1 3JD S Yorkshire England;

    Univ Sheffield Immobilisat Sci Lab Dept Mat Sci Sc Engn Sir Robert Hadfield Bldg Mappin St Sheffield S1 3JD S Yorkshire England;

    ESRF XMaS UK CRG 71 Ave Martyrs F-38043 Grenoble France;

    Univ Sheffield Immobilisat Sci Lab Dept Mat Sci Sc Engn Sir Robert Hadfield Bldg Mappin St Sheffield S1 3JD S Yorkshire England;

    Univ Sheffield Immobilisat Sci Lab Dept Mat Sci Sc Engn Sir Robert Hadfield Bldg Mappin St Sheffield S1 3JD S Yorkshire England;

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