Elucidating the Atomic Structures of the Gel Layer Formed during Aluminoborosilicate Glass Dissolution: An Integrated Experimental and Simulation Study
Elucidating the Atomic Structures of the Gel Layer Formed during Aluminoborosilicate Glass Dissolution: An Integrated Experimental and Simulation Study
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阐明铝硼硅酸盐玻璃溶解过程中形成的凝胶层的原子结构：综合实验和模拟研究
DOI：
10.1021/acs.jpcc.1c10463
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Ishida Keisuke
中科院分区：
文献类型：
--
作者：
Furutani Kenta;Ohkubo Takahiro;Du Jincheng;Ohara Koji;Deguchi Kenzo;Ohki Shinobu;Shimizu Tadashi;Inagaki Yaohiro;Matsubara Ryuta;Ishida Keisuke
在硅酸盐和硼硅酸盐玻璃的水溶解过程中产生的蚀变玻璃是在原子水平上理解的最复杂的结构之一，这是由于它们的无定形性质、随机孔隙率和各种水平的水合作用。在这项研究中，我们通过结合一系列实验和计算方法，深入了解了改变的铝硼硅酸盐玻璃的复杂原子结构。通过将具有不同水平氧化铝的三种玻璃在酸中溶解7天来制备改变的玻璃。一套全面的实验[元素分析，高能X射线衍射，29 Si和27 Al固态核磁共振（NMR），和O 1s X射线光电子能谱（XPS）]和建模（分子动力学（MD）模拟使用非反应和反应力场）的方法被用来研究这些改变玻璃的原子结构。元素分析表明，原始玻璃中的大部分B浸出到溶液中，并且不包含在改变的玻璃中。29Si和27Al的固体核磁共振谱表明，与原始玻璃相比，改变后的玻璃具有更多的聚合硅酸盐网络，这是由于改变后的玻璃中Si和Al氧多面体之间的键的重新形成。桥和nonbridging（或羟基O）原子在改变玻璃也量化从他们的O 1s XPS光谱。原子结构模型的改变玻璃构建使用MD模拟使用反应力场的基础上从实验中获得的组成信息。使用不同的初始密度和CS温度的电荷缩放（CS）方法产生各种孔结构，然后通过与从高能X射线衍射获得的实验结构因子进行比较来确定每个改变的玻璃的最佳CS参数。分析了这些孔表面的孔和原子结构以及振动特性。因此，从这个全面的研究结果提供了一个现实的洞察改变玻璃的孔隙形态，原子结构和振动特性。
Altered glasses produced during the aqueous dissolution of silicate and borosilicate glasses are among the most complex structures to understand at the atomic level due to their amorphous nature, random porosity, and various levels of hydration. In this study, we gained insights into the complex atomic structures of altered aluminoborosilicate glasses by combining a range of experimental and computational approaches. The altered glasses were prepared by the dissolution of three glasses with varying levels of alumina in an acid for 7 days. A comprehensive set of experimental [elemental analysis, high-energy X-ray diffraction,29Si and27Al solid-state nuclear magnetic resonance (NMR), and O 1s X-ray photoelectron spectroscopy (XPS)] and modeling (molecular dynamics (MD) simulations using nonreactive and reactive force fields) approaches were used to study the atomic structures of these altered glasses. Elemental analysis showed that most of the B in the pristine glasses was leached into the solution and was not contained in the altered glass. The29Si and27Al solid-state NMR spectra revealed that the altered glasses have more polymerized silicate networks as compared to those in the pristine glasses due to the reformation of linkages among Si and Al oxygen polyhedral in the altered glasses. The bridging and nonbridging (or hydroxyl O) atoms in the altered glasses were also quantified from their O 1s XPS spectra. Atomic structure models of the altered glasses were constructed using MD simulations using the reactive force field based on the compositional information obtained from experiments. Various pore structures were generated using the charge-scaling (CS) method using different initial densities and CS temperatures; the best CS parameters of each altered glass were then determined by comparing with the experimental structure factors obtained from high-energy X-ray diffraction. Pore and atomic structures and vibrational properties around these pore surfaces were analyzed. These results from this comprehensive study thus provide a realistic insight into the pore morphology, atomic structure, and vibrational properties of altered glasses.
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