The Structural Role of Zn in Nuclear Waste Glasses

The Structural Role of Zn in Nuclear Waste Glasses
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DOI:
10.1111/j.2041-1294.2011.00067.x
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发表时间:
2011-12-01
影响因子:
2.1
通讯作者:
Aquilanti, Giuliana
Aquilanti, Giuliana
中科院分区:
材料科学3区
文献类型:
--
作者:
Cassingham, Nathan J.;Stennett, Martin C.;Aquilanti, Giuliana

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目前正在考虑将ZnO和CaO添加到目前的英国高放废物(HLW)玻璃料中,目的是改善加工行为和水耐久性。进行本研究是为了更好地理解Zn在模型U中的结构作用。K. HLW玻璃,特别是Zn作为这种材料中的网络改性剂、中间体或成形剂的作用。锌K边X射线吸收光谱应用于简单的钠钙硅酸盐玻璃掺杂ZnO和模型非活性U。K. HLW玻璃由模拟的镁诺克斯和混合物(25重量%镁诺克斯+ 75重量% ThORP再处理废物)废物组成。X-射线吸收近边缘和扩展的X-射线吸收精细结构光谱提供了确凿的证据,锌发生在四重协调与Zn-O接触距离为1.95 +/- 0.01埃在所有研究的玻璃。扩展的X射线吸收精细结构数据的分析还表明,在Zn-Si接触距离为3.58 +/-0.03埃处存在与Si次近邻原子的短程有序。
Addition of ZnO and CaO to current United Kingdom high level nuclear waste (HLW) glass frits is currently under consideration with the aim of improving processing behavior and aqueous durability. This study was performed in order to better understand the structural role of Zn in model U. K. HLW glasses and, in particular, the role of Zn as a network modifier, intermediate, or former in such materials. Zinc K-edge X-ray absorption spectroscopy was applied to simple soda-lime-silicate glasses doped with ZnO and on model inactive U. K. HLW glasses consisting of simulated Magnox and Blend (25 wt% Magnox + 75 wt% ThORP reprocessing waste) wastes. X-ray absorption near edge and extended X-ray absorption fine structure spectroscopy provided conclusive evidence that Zn occurs in four-fold coordination with Zn-O contact distances of 1.95 +/- 0.01 angstrom in all glasses studied. Analysis of the extended X-ray absorption fine structure data also indicates the presence of short range order with Si next nearest neighbor atoms present at a Zn-Si contact distance of 3.58 +/- 0.03 angstrom.