Crystallography & Geomaterials Research, Faculty of Geosciences, University of Bremen, Klagenfurter Straße 2-4, 28359, Bremen, Germany.
Bremen Center for Computational Materials Science, University of Bremen, 28359, Bremen, Germany.
Chemphyschem. 2023 May 2;24(9):e202300022. doi: 10.1002/cphc.202300022. Epub 2023 Feb 9.
The anticonvulsant drug carbamazepine (-) is an emerging contaminant of considerable concern due to its hazard potential and environmental persistence. Previous experimental studies proposed hydrophobic zeolites as promising adsorbents for the removal of carbamazepine from water, but only a few framework types were considered in those investigations. In the present work, electronic structure calculations based on dispersion-corrected density functional theory (DFT) were used to study the adsorption of CBZ in eleven all-silica zeolites having different pore sizes and connectivities of the pore system (AFI, ATS, BEA, CFI, DON, FAU, IFR, ISV, MOR, SFH, SSF framework types). It was found that some zeolites with one-dimensional channels formed by twelve-membered rings (IFR, AFI) exhibit the highest affinity towards CBZ. A "good fit" of CBZ into the zeolite pores that maximizes dispersion interactions was identified as the dominant factor determining the interaction strength. Further calculations addressed the role of temperature (for selected systems) and of guest-guest interactions between coadsorbed CBZ molecules. In addition to predicting zeolite frameworks of particular interest as materials for selective CBZ removal, the calculations presented here also contribute to the atomic-level understanding of the interaction of functional organic molecules with all-silica zeolites.
抗惊厥药物卡马西平 (-) 是一种新兴的污染物，由于其潜在的危害和环境持久性而引起了相当大的关注。先前的实验研究提出，疏水沸石是一种很有前途的吸附剂，可以从水中去除卡马西平，但在这些研究中只考虑了少数几种骨架类型。在本工作中，基于色散校正密度泛函理论 (DFT) 的电子结构计算被用于研究 11 种具有不同孔径和孔系统连接性的全硅沸石（AFI、ATS、BEA、CFI、DON、FAU、IFR、ISV、MOR、SFH、SSF 骨架类型）中 CBZ 的吸附。结果发现，一些由十二元环形成的一维通道的沸石（IFR、AFI）对 CBZ 表现出最高的亲和力。将 CBZ 很好地适配到沸石孔中，以最大化分散相互作用，被确定为决定相互作用强度的主要因素。进一步的计算还考虑了温度（对于选定的体系）和共吸附的 CBZ 分子之间的客体-客体相互作用的作用。除了预测作为选择性 CBZ 去除材料的特定沸石骨架外，这里的计算还有助于深入了解功能有机分子与全硅沸石的相互作用。
