标题： 使用MACE-MP-0机器学习原子间势模拟二氧化硅 显示英文标题

标题： Modelling Silica using MACE-MP-0 Machine Learnt Interatomic Potentials

摘要： 二氧化硅多形体和沸石由于其多样的结构特性、在不同条件下的热力学和机械稳定性以及地质重要性，对于广泛的工业应用至关重要。计算建模在理解二氧化硅和硅酸盐（包括沸石）的结构与功能之间的关系中发挥了关键作用。在本研究中，我们应用了MACE-MP-0机器学习原子间势（ML-IP）来模拟硅沸石的框架能量，并在高压条件下检查二氧化硅和ZSM-5多形体的相变。结果再现了硅沸石相对于{\alpha }-石英的已知亚稳性，MACE-MP-0中等ML-IP和密度泛函理论（DFT）方法计算的微孔相和致密相之间的能量差异与实验量热数据高度一致。高压模拟揭示了二氧化硅的石英、柯石英和斯石英多形体的不同压缩行为，柯石英和斯石英在高压下表现出更高的稳定性，这与实验数据一致。从石英到柯石英（约3.5 GPa）和柯石英到斯石英（约9 GPa）的计算相变压力接近实验结果，证明了MACE ML-IP在模拟二氧化硅多形体的结构和能量特性方面的可靠性。 显示英文摘要

摘要： Silica polymorphs and zeolites are fundamental to a wide range of industrial applications owing to their diverse structural characteristics, thermodynamic and mechanical stability under varying conditions and due to their geological importance. Computational modelling has played a crucial role in understanding the relationship between the structure and functionality of silicas and silicates including zeolites. In this study, we apply the MACE-MP-0 machine learnt interatomic potentials (ML-IP) to model the framework energies of siliceous zeolites and examine the phase transitions of silica and ZSM-5 polymorphs under high-pressure conditions. The results reproduce the known metastability of siliceous zeolites relative to {\alpha}-quartz, with energy differences between microporous and dense phases calculated by MACE-MP-0 medium ML-IP and density functional theory (DFT) methods closely aligning with experimental calorimetric data. The high-pressure simulations reveal distinct compression behaviour in the quartz, coesite, and stishovite polymorphs of silica, with coesite and stishovite showing increased stability at elevated pressures in line with experimental data. The calculated phase transition pressures from quartz to coesite (~3.5 GPa) and coesite to stishovite (~9 GPa) are close to experimental findings, demonstrating the reliability of MACE ML-IP in modelling the structural and energetic properties of silica polymorphs.