Department of Integrative Structural and Computational Biology, Scripps Research, La Jolla, California 92037, United States.
J Chem Theory Comput. 2023 May 9;19(9):2535-2556. doi: 10.1021/acs.jctc.2c01087. Epub 2023 Apr 24.
Water desolvation is one of the key components of the free energy of binding of small molecules to their receptors. Thus, understanding the energetic balance of solvation and desolvation resulting from individual water molecules can be crucial when estimating ligand binding, especially when evaluating different molecules and poses as done in High-Throughput Virtual Screening (HTVS). Over the most recent decades, several methods were developed to tackle this problem, ranging from fast approximate methods (usually empirical functions using either discrete atom-atom pairwise interactions or continuum solvent models) to more computationally expensive and accurate ones, mostly based on Molecular Dynamics (MD) simulations, such as Grid Inhomogeneous Solvation Theory (GIST) or Double Decoupling. On one hand, MD-based methods are prohibitive to use in HTVS to estimate the role of waters on the fly for each ligand. On the other hand, fast and approximate methods show an unsatisfactory level of accuracy, with low agreement with results obtained with the more expensive methods. Here we introduce WaterKit, a new grid-based sampling method with explicit water molecules to calculate thermodynamic properties using the GIST method. Our results show that the discrete placement of water molecules is successful in reproducing the position of crystallographic waters with very high accuracy, as well as providing thermodynamic estimates with accuracy comparable to more expensive MD simulations. Unlike these methods, WaterKit can be used to analyze specific regions on the protein surface, (such as the binding site of a receptor), without having to hydrate and simulate the whole receptor structure. The results show the feasibility of a general and fast method to compute thermodynamic properties of water molecules, making it well-suited to be integrated in high-throughput pipelines such as molecular docking.
水去溶剂化作用是小分子与其受体结合自由能的关键组成部分之一。因此,在估计配体结合时,了解单个水分子的溶剂化和去溶剂化的能量平衡可能至关重要,特别是在评估不同分子和构象时,如高通量虚拟筛选(HTVS)中所做的那样。在最近几十年中,已经开发了几种方法来解决这个问题,从快速近似方法(通常是使用离散原子-原子相互作用或连续溶剂模型的经验函数)到更昂贵和准确的方法,主要基于分子动力学(MD)模拟,例如网格不均匀溶剂化理论(GIST)或双解耦。一方面,基于 MD 的方法在 HTVS 中不适合用于实时估计每个配体上水的作用。另一方面,快速和近似方法的准确性令人不满意,与更昂贵方法的结果吻合度较低。在这里,我们引入了 WaterKit,这是一种新的基于网格的采样方法,使用显式水分子来使用 GIST 方法计算热力学性质。我们的结果表明,水分子的离散放置成功地以非常高的精度再现了结晶水的位置,并提供了与更昂贵的 MD 模拟相当的准确性的热力学估计。与这些方法不同,WaterKit 可用于分析蛋白质表面上的特定区域(例如受体的结合位点),而无需水合和模拟整个受体结构。结果表明,计算水分子热力学性质的通用快速方法是可行的,使其非常适合集成到分子对接等高通量管道中。