Insights into the mechanism and kinetics of dissolution of aluminoborosilicate glasses in acidic media: Impact of high ionic field strength cations
Insights into the mechanism and kinetics of dissolution of aluminoborosilicate glasses in acidic media: Impact of high ionic field strength cations
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深入了解铝硼硅酸盐玻璃在酸性介质中溶解的机理和动力学：高离子场强度阳离子的影响
DOI：
10.1016/j.actamat.2022.118468
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发表时间：
2023
期刊：
影响因子：
9.4
通讯作者：
Goel, Ashutosh
中科院分区：
文献类型：
--
作者：
Qin, Qianhui;Stone-Weiss, Nicholas;Zhao, Tongyao;Mukherjee, Pinaki;Ren, Jinjun;Mauro, John C.;Goel, Ashutosh
实现更薄和更高性能的显示器/基板玻璃和具有可调性能的透明玻璃陶瓷需要精确控制酸蚀刻过程，因此需要全面了解玻璃在酸性介质中的组成-结构-溶解行为关系。不幸的是，关于这一主题的文献仅集中在一组狭窄的玻璃化学上。因此，在广泛的组成空间的多组分硅酸盐玻璃的酸溶解的机制，管理共识仍然缺乏。本工作采用了一套最先进的光谱技术，包括1D和2D NMR、TEM-EELS、ICP-OES和XPS，以深入了解碱金属/碱土金属铝硼硅酸盐玻璃（包含高场强阳离子-HFSC，即，La 3+、Ti 4+、Zr 4+和Nb 5+）在酸性介质（HCl; pH = 2）中的混合物。将HFSC分散到玻璃中诱导其网络中的显著结构变化，从而影响正向速率溶解动力学。基于这些结果，我们假设玻璃在pH = 2下通过“界面溶解-再沉淀机制（IDPM）”和“原位冷凝”耦合模式溶解，其中IDPM导致富Si蚀变层，随后由于未腐蚀的玻璃表面和外部蚀变层之间的界面溶液附近的有限动力学而发生局部再冷凝。
Achieving thinner and higher performance display/substrate glasses and transparent glass-ceramics with tunable properties requires a precise control of acid-etching process, thus necessitating a comprehensive understanding of glass composition–structure–dissolution behavior relationships in acidic medium. Unfortunately, the literature on this subject has been focused only on a narrow set of glass chemistries. Therefore, consensus on the mechanisms that govern the acidic dissolution of multicomponent silicate glasses over a broad compositional space is still lacking. The present work employs a suite of state-of-the-art spectroscopic techniques, including 1D and 2D NMR, TEM-EELS, ICP-OES, and XPS, to provide an insight into the mechanism and kinetics of corrosion of alkali/alkaline-earth aluminoborosilicate glasses (comprising high field strength cations – HFSCs, i.e., La3+, Ti4+, Zr4+and Nb5+) in acidic media (HCl; pH = 2). Incorporating the HFSCs into the glasses induces significant structural changes in their network, thus, impacting the forward rate dissolution kinetics. Based on the results, we hypothesize that the glasses dissolve at pH = 2 through an ‘interfacial dissolution – re-precipitation mechanism (IDPM)’ and ‘in-siturecondensation’ coupled pattern, wherein the IDPM results in a Si-rich alteration layer, followed by local recondensation occurring due to limited kinetics near the interfacial solution between the uncorroded glass surface and the outer alteration layer.