Vuković F, Garcia N A, Perera S, Turchi M, Andersson M P, Solvang M, Raiteri P, Walsh T R
Institute for Frontier Materials, Deakin University, Geelong, VIC 3216, Australia.
Department of Chemical and Biochemical Engineering, Technical University of Denmark, Kgs. Lyngby 2800, Denmark.
J Chem Phys. 2023 Sep 14;159(10). doi: 10.1063/5.0164817.
The dissolution behavior of calcium aluminosilicate based glass fibers, such as stone wool fibers, is an important consideration in mineral wool applications for both the longevity of the mineral wool products in humid environments and limiting the health impacts of released and inhaled fibers from the mineral wool product. Balancing these factors requires a molecular-level understanding of calcium aluminosilicate glass dissolution mechanisms, details that are challenging to resolve with experiment alone. Molecular dynamics simulations are a powerful tool capable of providing complementary atomistic insights regarding dissolution; however, they require force fields capable of describing not-only the calcium aluminosilicate surface structure but also the interactions relevant to dissolution phenomena. Here, a new force field capable of describing amorphous calcium aluminosilicate surfaces interfaced with liquid water is developed by fitting parameters to experimental and first principles simulation data of the relevant oxide-water interfaces, including ab initio molecular dynamics simulations performed for this work for the wüstite and periclase interfaces. Simulations of a calcium aluminosilicate surface interfaced with liquid water were used to test this new force field, suggesting moderate ingress of water into the porous glass interface. This design of the force field opens a new avenue for the further study of calcium and network-modifier dissolution phenomena in calcium aluminosilicate glasses and stone wool fibers at liquid water interfaces.
钙铝硅酸盐基玻璃纤维（如石棉纤维）的溶解行为，对于矿棉在潮湿环境中的使用寿命以及限制矿棉产品释放和吸入纤维对健康的影响而言，是矿棉应用中需要重点考虑的因素。要平衡这些因素，需要从分子层面了解钙铝硅酸盐玻璃的溶解机制，而仅靠实验很难确定这些细节。分子动力学模拟是一种强大的工具，能够提供关于溶解的补充性原子层面见解；然而，这需要能够描述钙铝硅酸盐表面结构以及与溶解现象相关相互作用的力场。在此，通过将参数拟合到相关氧化物 - 水界面的实验数据和第一性原理模拟数据，开发了一种能够描述与液态水接触的无定形钙铝硅酸盐表面的新力场，包括为本工作对氧化亚铁和方镁石界面进行的从头算分子动力学模拟。对与液态水接触的钙铝硅酸盐表面进行模拟，以测试这种新力场，结果表明水适度进入多孔玻璃界面。这种力场设计为进一步研究液态水界面处钙铝硅酸盐玻璃和石棉纤维中的钙及网络改性剂的溶解现象开辟了一条新途径。
