Faculty of Chemistry, University of Bucharest, 4-12 Regina Elisabeta Bd., 030018 Bucharest, Romania.
Horia Hulubei National Institute of Research and Development for Physics and Nuclear Engineering, 30 Reactorului Str., 077125 Magurele, Romania.
Int J Mol Sci. 2023 Aug 25;24(17):13214. doi: 10.3390/ijms241713214.
Polychlorinated dibenzo-p-dioxins (PCDD) are persistent organic pollutants which result as byproducts in industrial or combustion processes and induce toxicity in both wildlife and humans. In this study, all seven PCDD, tetrachlorinated dibenzo-p-dioxins (TCDD), pentachlorinated dibenzo-p-dioxins (P5CDD), hexachlorinated dibenzo-p-dioxins (H6CDD), heptachlorinated dibenzo-p-dioxins (H7CDD), and octachlorinated dibenzo-p-dioxins (OCDD) were studied in interaction with two cyclodextrins, β-CD and γ-CD, resulting in a total of 40 host-guest complexes. The flexibility of the cyclodextrins was given by the number of glucose units, and the placement of the chlorine groups on the dioxins structure accounted for the different complex formed. Various geometries of interaction obtained by guided docking were studied, and the complexation and binding energy were calculated in the frame of MM+ and OPLS force fields. The results show that the recognition of the PCDD pollutants by the CD may be possible through the formation of PCDD:CD inclusion complexes. This recognition is based on the formation of Coulombic interactions between the chlorine atom of the PCDD and the primary and secondary hydroxyl groups of the CD and van der Waals interaction of the CD hydrophobic cavity with PCDD aromatic structures. Both MM+ and OPLS calculus resulted in close values for the complexation and binding energies. Molecular mechanics calculations offer a proper insight into the molecular recognition process between the PCDD compounds and CD molecules, proved by a good description of the C-H···O bonds formed between the guest and host molecules. It was shown for the first time that CD may efficiently trap PCCDs, opening the way for their tremendous potential use in environmental remediation.
多氯二苯并对二恶英(PCDD)是在工业或燃烧过程中作为副产品产生的持久性有机污染物,对野生动物和人类都具有毒性。在这项研究中,研究了所有七种 PCDD、四氯二苯并对二恶英(TCDD)、五氯二苯并对二恶英(P5CDD)、六氯二苯并对二恶英(H6CDD)、七氯二苯并对二恶英(H7CDD)和八氯二苯并对二恶英(OCDD)与两种环糊精β-CD 和 γ-CD 的相互作用,共形成了 40 个主体-客体配合物。环糊精的灵活性取决于葡萄糖单元的数量,而二恶英结构上氯原子的位置决定了形成的不同配合物。通过引导对接研究了获得的各种相互作用几何形状,并在 MM+和 OPLS 力场框架中计算了配合物和结合能。结果表明,通过形成 PCDD:CD 包合物,CD 可能有可能识别 PCDD 污染物。这种识别基于 PCDD 中氯原子与 CD 的伯羟基和仲羟基之间形成的库仑相互作用以及 CD 疏水性空腔与 PCDD 芳构结构之间的范德华相互作用。MM+和 OPLS 计算都得出了相近的配合物和结合能值。分子力学计算为 PCDD 化合物与 CD 分子之间的分子识别过程提供了恰当的见解,这通过对客体和主体分子之间形成的 C-H···O 键的良好描述得到了证明。首次表明 CD 可能有效地捕获 PCCDs,为其在环境修复中的巨大应用潜力开辟了道路。