The heulandite-type zeolite (HEU) is an important class of naturally occurring zeolite materials. The recent development of a synthetic HEU zeolite with a high Si/Al ratio opens new possibilities for various applications. Herein, a periodic density functional theory with dispersion correction scheme (DFT-D3) was performed on the HEU-type zeolite. Various aspects of zeolite properties, such as the distribution of Al atoms within the zeolite framework, the prediction of the non-Löwenstein structure, and the presence of aromatic compounds within the cavity, were investigated. Calculation of the initial HEU framework shows that the Al atoms occupy the T2 and T3 sites in the most stable structure. Additionally, a non-Löwenstein structure was predicted for the first time to give a relatively stable HEU structure containing the Al–O–Al configuration. The preferred location of various aromatic compounds, namely, benzene, toluene and naphthalene, could be modeled in the 10-member ring channel to represent a host-guest system in this zeolite with a Si/Al ratio of 10. The results exemplify the importance of understanding the crystal structure of zeolites and the effect it has because of the presence of Al atoms and adsorbate molecules within the zeolite frameworks.

堇青石型沸石（HEU）是一类重要的天然沸石材料。高Si / Al比的合成HEU沸石的最新开发为各种应用提供了新的可能性。在此，对HEU型沸石进行了具有色散校正方案的周期性密度泛函理论（DFT-D3）。研究了沸石性能的各个方面，例如沸石骨架中Al原子的分布，非洛文斯坦结构的预测以及模腔中芳族化合物的存在。初始HEU框架的计算表明，Al原子在最稳定的结构中占据T2和T3位置。此外，首次预测了非洛因斯坦结构，从而给出了包含Al–O–Al构型的相对稳定的HEU结构。