Glasses corroded in static aqueous conditions typically reach a slow, residual rate of dissolution as a result of the complex interplay between multiple processes. While intrinsically suited to address this problem, Monte Carlo (MC) models developed to date have relied on lattices to describe the amorphous structure of glass and are thus unable to reproduce the residual rate of glass corrosion. A recently developed MC approach based on amorphous structures derived from molecular dynamics simulations offers a solution [Kerisit and Du J. Non-Cryst. Solids 522 (2019) 119601], but it requires a simple model that can rapidly relax the glass-water interface upon each dissolution/condensation event to retain the ability of MC simulations to reach large spatial and temporal scales. To this end, a patchy particle model of hydrated amorphous silica was developed and evaluated against atomistic simulations in this work. Models of water and amorphous silica were first developed separately, and cross terms were then defined to enable simulations of hydrated amorphous silica structures with varying water content. While the nature of its interaction potential prevents the patchy particle model from reproducing simultaneously the structure and dynamics of the systems of interest with a single set of parameters, it described well the connectivity of hydrated amorphous silica structures and the local coordination geometry of individual species. Therefore, this model opens the door to MC simulations of the residual rate of glass corrosion and offers an alternative to atomistic models to investigate the evolution of silica gels over large spatial and temporal scales.

由于在多个过程之间复杂的相互作用，在静态水性条件下腐蚀的玻璃通常会达到缓慢的残留溶解速率。尽管本质上适合解决此问题，但迄今为止开发的蒙特卡洛（MC）模型已经依赖于晶格来描述玻璃的非晶结构，因此无法重现玻璃腐蚀的残留率。最近开发的基于分子动力学模拟得出的无定形结构的MC方法提供了一种解决方案[Kerisit和Du J. Non-Cryst。Solids 522（2019）119601]，但是它需要一个简单的模型，该模型可以在每次溶解/冷凝事件发生时迅速放松玻璃水界面，以保持MC模拟达到大时空尺度的能力。为此，开发了水合无定形二氧化硅的小颗粒模型，并在这项工作中针对原子模拟对其进行了评估。首先分别开发水和无定形二氧化硅的模型，然后定义交叉项以模拟水含量不同的水合无定形二氧化硅结构。尽管其相互作用潜能的本质阻止了斑块粒子模型通过一组参数同时复制目标系统的结构和动力学，但它很好地描述了水合无定形二氧化硅结构的连通性和各个物种的局部配位几何形状。因此，