Insights from molecular dynamics into the chemistry-structure relationships of calcium aluminosilicate glasses
Insights from molecular dynamics into the chemistry-structure relationships of calcium aluminosilicate glasses
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从分子动力学洞察铝硅酸钙玻璃的化学结构关系
DOI：
10.1016/j.jnoncrysol.2023.122545
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发表时间：
2023
影响因子：
3.5
通讯作者：
Ruiz Pestana, Luis
中科院分区：
文献类型：
--
作者：
Liu, Meili;Panda, Subhashree;Suraneni, Prannoy;Ruiz Pestana, Luis
钙铝硅酸盐（CAS）玻璃在自然界中普遍存在，并且在从结构玻璃到可持续胶凝材料的各种技术应用中发挥重要作用。了解CAS玻璃的化学组成和结构之间的关系是优化其未来不同用途性能的重要一步。在这里，我们使用广泛的分子动力学（MD）模拟表征CAS玻璃的多尺度结构在整个组成范围内。短，中程秩序的玻璃分析表明，洛温斯坦的规则被广泛违反，二氧化硅比氧化铝更容易受到解聚作用的钙，高硅玻璃有利于钙在较低的氧配位状态，而相反的是真实的高铝。我们还发现存在高度协调的铝和三簇氧的高铝玻璃，形成作为一个电荷补偿机制。我们发现，目前的理论模型用于预测氧物种，氧桥类型，或四面体协调，而整体定性合理，简化了复杂的不同氧化物之间的相互作用，导致不准确的预测，特别是对于玻璃在中间组成区域。我们的簇，链和环的拓扑结构中的铝硅酸盐网络的分析揭示了一个急剧的过渡，从连接到断开的图形，这不仅取决于玻璃的钙含量，但也对二氧化硅氧化铝的比例。在对应于这种过渡的组成区域中的玻璃显示出所研究的任何玻璃中最大的环和最长的链结构。
Calcium aluminosilicate (CAS) glasses are ubiquitous in nature and play an important role in diverse technological applications ranging from structural glasses to sustainable cementitious materials. Understanding the relationship between the chemical composition and the structure of CAS glasses is an essential step towards optimizing their properties for different uses in the future. Here, we use extensive molecular dynamics (MD) simulations to characterize the multiscale structure of CAS glasses over the full compositional range. Analysis of the short and medium range order of the glasses reveals that Lowenstein's rule is widely violated, that silica is more susceptible than alumina to the depolymerizing effects of calcium, and that high-silica glasses favor calcium in lower oxygen coordination states, while the opposite is true for high-alumina ones. We also find the presence of highly coordinated aluminum and tricluster oxygens in high-alumina glasses, which form as a charge compensation mechanism. We find that current theoretical models used to predict oxygen species, oxygen bridge types, or tetrahedral coordination, while overall qualitatively reasonable, simplify the complex interplay between the different oxides which results in inaccurate predictions, particularly for glasses in intermediate compositional regions. Our analysis of the cluster, chain, and ring topological structures in the aluminosilicate network reveals a sharp transition from a connected to a disconnected graph which depends not only on the calcium content of the glass, but also on the ratio of silica to alumina. Glasses in the compositional region corresponding to such transition display the largest ring and longest chain structures of any glass studied.
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改性铝硅酸盐玻璃中的高配位氧化铝和氧三簇
影响因子：
2.1
作者：
Rebecca S. Welch;Sierra R Astle;R. Youngman;J. Mauro
通讯作者：
J. Mauro
DOI：
10.1021/acs.jpcc.3c01123
发表时间：
2023-04
期刊：
The Journal of Physical Chemistry C
影响因子：
--
作者：
Luis Ruiz Pestana;Swathi Shantha Raju;Chaitanya Guntoorkar;P. Suraneni
通讯作者：
Luis Ruiz Pestana;Swathi Shantha Raju;Chaitanya Guntoorkar;P. Suraneni
玻璃的结构和特性——我们还需要走多远？
影响因子：
3.5
作者：
P. Gaskell
通讯作者：
P. Gaskell
影响因子：
4.4
作者：
Ganster, P;Benoit, M;Delaye, JM
通讯作者：
Delaye, JM
影响因子：
3.3
作者：
M. Bauchy
通讯作者：
M. Bauchy