Structural evolution of high zirconia aluminosilicate glasses
Structural evolution of high zirconia aluminosilicate glasses
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高氧化锆铝硅酸盐玻璃的结构演变
DOI：
10.1016/j.jnoncrysol.2020.120050
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发表时间：
2020
影响因子：
3.5
通讯作者：
L. Cormier
中科院分区：
文献类型：
--
作者：
M. Ficheux;E. Burov;G. Aquilanti;N. Trcera;V. Montouillout;L. Cormier
我们报告了使用 X 射线吸收光谱、拉曼光谱以及 27Al 和 29Si NMR 对含有 0-20 wt% ZrO2 的 Ca-Na 铝硅酸盐玻璃进行的详细结构研究。 X射线吸收光谱数据表明Zr主要存在于ZrO6八面体中，但随着ZrO2含量的增加，Zr配位发生显着变化。尽管Al和Zr竞争被电荷平衡阳离子包围，但27Al NMR数据并未显示高配位Al物种的存在；因此，电荷平衡阳离子优先位于靠近 AlO4 四面体而不是 Zr 多面体的位置，这解释了 Zr 配位数的增加最终导致限制 Zr 在玻璃中的溶解度。拉曼和29Si NMR数据表明Zr原子与硅酸盐网络相连，并且在高氧化锆含量下具有更高程度的网络连通性的趋势。网络连接和 Zr 环境的变化为了解玻璃的化学耐久性或结晶提供了见解。
We report a detailed structural investigation of Ca-Na aluminosilicate glasses containing 0–20 wt% ZrO2using X-ray absorption spectroscopy, Raman spectroscopy and27Al and29Si NMR. The X-ray absorption spectroscopy data reveal that Zr is predominantly present in ZrO6octahedra but a significant Zr coordination change occurs with increasing ZrO2content. Though Al and Zr are competing to be surrounded by charge balancing cations,27Al NMR data do not show the presence of high-coordinated Al species; thus charge-balancing cations are preferentially localized close to AlO4tetrahedra rather than Zr polyhedra, explaining the increase in Zr coordination number that ultimately leads to limit Zr solubility in glasses. Raman and29Si NMR data indicates that Zr atoms are linked to the silicate network with a trend for higher degree of network connectivity at high zirconia content. Change in network connectivity and in Zr environment provide insights to understand chemical durability or crystallization in glasses.