<br>水负载对原始和缺陷 UiO-66 稳定性的影响,Journal of Materials Chemistry A

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水负载对原始和缺陷 UiO-66 稳定性的影响
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-08-16 , DOI: 10.1039/d4ta04252b
E. Acuna-Yeomans _{1,

2} , P. J. Goosen ₃ , J. J. Gutiérrez-Sevillano ₄ , D. Dubbeldam ₅ , S. Calero _{1,

2}

Affiliation

用于水处理目的的材料需要稳定，以便于处理和成本效益。 UiO-66 已被认为是一个有前途的选择。在这项工作中，我们使用经典分子模拟研究了水负载对原始和有缺陷的 UiO-66 的结构和机械性能的影响。我们采用并比较了两种模拟框架和水分子之间非键相互作用的方法：直接洛伦兹-贝特洛（L-B）混合和混合混合。我们进行了分子动力学模拟，以检查框架内水分子的空间排列、特定框架相互作用位点的水亲和力，以及它们在大气条件、高静水压力和增加的水负载下对框架结构参数的影响。我们的结果表明，两种方法都预测锆簇附近的水亲和力，但在识别主要相互作用位点和相互作用强度方面有所不同。 L-B 混合预测与连接氧原子的强烈结合，限制水的运动，而混合混合表明动态水行为，在中等和高负载下观察到位点到位点的跳跃和孔到孔的运动。水负载增加时的结构分析表明，由于连接基团键拉伸，使用 L-B 混合会导致吸附引起的膨胀，这与混合混合预测的轻微系统收缩形成鲜明对比。高压 NPT 模拟证明水负载降低了非晶化压力，尽管使用两种方法获得的值在中等和高负载下显着不同。

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Effect of water loading on the stability of pristine and defective UiO-66

Materials used for water treatment purposes need to be stable for easy handling and cost-effectiveness. UiO-66 has been identified as a promising option. In this work, we investigate the impact of water loading on the structural and mechanical properties of pristine and defective UiO-66 using classical molecular simulations. We employ and compare two approaches for modeling non-bonded interactions between the framework and water molecules: direct Lorentz–Berthelot (L–B) mixing and hybrid mixing. We conducted molecular dynamics simulations to examine the spatial arrangement of water molecules within the framework, water affinity for specific framework interaction sites, and their impact on the framework's structural parameters under atmospheric conditions, high hydrostatic pressures, and increased water loading. Our results indicate that both methods predict water affinity near zirconium clusters, but differ in identifying principal interaction sites and interaction strength. L–B mixing predicts strong binding to linker oxygen atoms, restricting water movement, while hybrid mixing indicated dynamic water behavior, with site-to-site hopping and pore-to-pore movement observed at moderate and high loadings. Structural analysis at increased water loadings showed adsorption-induced expansion using L–B mixing due to linker–cluster bond stretching, contrasting with slight system contraction predicted by hybrid mixing. High-pressure NPT simulations evidence that water loading reduces amorphization pressure, although values obtained using both approaches differ significantly at moderate and high loadings.

更新日期：2024-08-16

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