For chemical warfare agent removal, the humidity emerges as an unavoidable challenge that significantly affects the performance of metal–organic frameworks. In this work, via density functional theory calculations, ab initio molecular dynamics and classical molecular dynamics simulations, we investigate the structural and diffusion properties of water in the pristine defect‐free UiO‐66, one Zr‐based metal–organic framework. Through the detailed analyses of the distribution probability of water in two different cages of UiO‐66, the binding interaction between water and UiO‐66, the hydrogen bonding networks and resulted localized water clusters, we gain a fundamental understanding of structural and dynamics properties as well as the concentration dependence of water in UiO‐66. We anticipate those theoretical results could provide insight to the competitive adsorption of water and chemical warfare agents, which eventually shows the utmost importance for the design and development of the next generation porous materials with appropriate water properties in real‐life applications.

中文翻译：

---

UiO-66 Zr-MOF中水的计算研究：扩散，氢键网络和约束效应

对于化学战剂的去除，湿度是不可避免的挑战，会显着影响金属有机框架的性能。在这项工作中，通过密度泛函理论计算，从头算分子动力学和经典分子动力学模拟，我们研究了纯净无缺陷的UiO-66（一种基于Zr的金属有机框架）中水的结构和扩散特性。通过详细分析两个不同的UiO-66笼中水的分布概率，水与UiO-66之间的结合相互作用，氢键网络和形成的局部水团簇，我们对结构和动力学性质有了基本的了解以及UiO-66中水的浓度依赖性。