Hubman Anže, Volavšek Janez, Urbič Tomaž, Zabukovec Logar Nataša, Merzel Franci
Faculty of Chemistry and Chemical Technology, University of Ljubljana, Večna Pot 113, 1000 Ljubljana, Slovenia.
Theory Department, National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, Slovenia.
Nanomaterials (Basel). 2023 Aug 22;13(17):2387. doi: 10.3390/nano13172387.
Linde type A (LTA) aluminophosphate is a promising candidate for an energy storage material used for low-temperature solar and waste-heat management. The mechanism of reversible water adsorption, which is the basis for potential industrial applications, is still not clear. In this paper, we provide mechanistic insight into various aspects of the hydration process using molecular modeling methods. Building on accurate DFT calculations and available experimental data, we first refine the existing empirical force-field used in subsequent classical molecular dynamics simulations that captures the relevant physics of the water binding process. We succeed in fully reproducing the experimentally determined X-ray structure factors and use them to estimate the number of water molecules present in the fully hydrated state of the material. Furthermore, we show that the translational and orientational mobility of the confined water is significantly reduced and resembles the dynamics of glassy systems.
A型林德磷酸铝（LTA）是一种很有前景的储能材料候选物，可用于低温太阳能和废热管理。可逆水吸附机制是潜在工业应用的基础，但目前仍不清楚。在本文中，我们使用分子建模方法对水化过程的各个方面提供了机理见解。基于精确的密度泛函理论（DFT）计算和现有的实验数据，我们首先完善了随后用于经典分子动力学模拟的现有经验力场，该力场捕捉了水结合过程的相关物理现象。我们成功地完全再现了实验测定的X射线结构因子，并用它们来估计材料完全水合状态下存在的水分子数量。此外，我们表明受限水的平移和取向迁移率显著降低，类似于玻璃态系统的动力学。
