With the emergence and popularity of high-performance computers, advances in materials informatics, and improvements in computing architectures and algorithms, the application of modeling in the field of materials science has become increasingly common and affordable. The ability to compute has benefited materials discovery in the last decade alone with many breakthroughs: improved photovoltaics, new functional nanomaterials, more efficient rechargeable batteries, and tailorable catalytic surfaces to name a few. Among various computing tools, first-principles calculations based on density functional theory (DFT) have been widely applied to high throughput computational analysis to better understand the formation, properties, and stability of new and existing materials. The advantages of DFT methods are that they are inexpensive, fast, and are capable of capturing nuances at the atomistic scale. Since DFT calculations are performed at 0 K and in vacuum, thermodynamic corrections need to be taken into account to match real world operating conditions in the laboratory and during use. These thermodynamic corrections have been applied for over twenty years and provided valuable guidance to the analysis of surface structure, vacancy formation, and stability across varying gaseous environments. The combination of DFT with experimental corrections significantly expands its flexibility as it can be used to generate stability conditions for specific elements and multi-component solids in water. This literature review will provide a thorough survey of first-principles DFT calculations combined with thermodynamics, as well as their application and research in the design, predicted stability, and characterization of 2D materials, their surfaces, and interfacial surface reactivity. A particular emphasis will be placed on the behavior of 2D materials in aqueous environments, comparing their surface transformation thermodynamics via processes such as ion release and adsorption using the newly created DFT + Solvent Ion Model (DSIM).

随着高性能计算机的出现和普及、材料信息学的进步以及计算架构和算法的改进，建模在材料科学领域的应用变得越来越普遍和负担得起。仅在过去十年中，计算能力就使材料发现受益匪浅，并取得了许多突破：改进的光伏技术、新的功能纳米材料、更高效的可充电电池以及可定制的催化表面等等。在各种计算工具中，基于密度泛函理论（DFT）的第一性原理计算已广泛应用于高通量计算分析，以更好地了解新材料和现有材料的形成、性质和稳定性。DFT 方法的优点是成本低、速度快，并且能够捕捉原子尺度的细微差别。由于 DFT 计算是在 0 K 和真空中进行的，因此需要考虑热力学校正，以匹配实验室和使用过程中的真实操作条件。这些热力学修正已经应用了二十多年，为分析不同气体环境中的表面结构、空位形成和稳定性提供了宝贵的指导。DFT 与实验校正的结合显着扩展了其灵活性，因为它可用于生成水中特定元素和多组分固体的稳定性条件。本文献综述将对第一原理 DFT 计算与热力学相结合进行全面调查，及其在二维材料、其表面和界面表面反应性的设计、预测稳定性和表征中的应用和研究。将特别强调二维材料在水性环境中的行为，使用新创建的 DFT + 溶剂离子模型 (DSIM) 通过离子释放和吸附等过程来比较其表面转变热力学。