College of Chemistry and Chemical Engineering, Northwest Normal University, Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional Materials, Lanzhou, Gansu, 730070, China.
College of Chemistry and Chemical Engineering, Northwest Normal University, Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional Materials, Lanzhou, Gansu, 730070, China.
J Mol Graph Model. 2024 Jul;130:108782. doi: 10.1016/j.jmgm.2024.108782. Epub 2024 Apr 26.
The interactions of the micro-mechanism of hydroxymethanesulfonic acid (HMSA) with the typical small organic molecule in atmospheric (X = methanol, formaldehyde, formic acid, methyl formate, dimethyl ether, acetone) has been investigated by density functional theory (DFT), quantum theory of atoms in molecules (QTAIM), Generalized Kohn-Sham Enery Decomposition Analysis (GKS-EDA) and the atmospheric clusters dynamic code (ACDC). The results of DFT show that the stable six- to eight-membered ring structures are easily formed in HMSA-X clusters. According to the topological analysis results of the AIM theory and the IRI method, a strong hydrogen bonding interaction is present in the complex. GKS-EDA results show that electrostatic energy is the main contributor to the interaction energy as it accounts for 51 %-55 % of the total attraction energy. The evaporation rates of HMSA-HMSA and HMSA-HCOOH clusters were much lower than those of the other HMSA complexes. In addition, the Gibbs energy of formation (ΔG) of HMSA-X dimers is investigated under atmosphere temperature T = 217-298 K and p = 0.19-1.0 atm, the ΔG decreased with decreasing of the atmosphere temperature and increased with the decrease of atmospheric pressure, indicating that the low temperature and high pressure may significantly facilitate to the formation of dimers.
采用密度泛函理论(DFT)、原子在分子中的量子理论(QTAIM)、广义 Kohn-Sham 能量分解分析(GKS-EDA)和大气团簇动力学代码(ACDC)研究了羟甲基磺酸(HMSA)与大气中典型小分子(X=甲醇、甲醛、甲酸、甲酸甲酯、二甲醚、丙酮)的微观机制相互作用。DFT 的结果表明,在 HMSA-X 团簇中容易形成稳定的六至八元环结构。根据 AIM 理论和 IRI 方法的拓扑分析结果,复合物中存在强氢键相互作用。GKS-EDA 结果表明,静电能是相互作用能的主要贡献者,占总吸引能的 51%-55%。HMSA-HMSA 和 HMSA-HCOOH 团簇的蒸发速率远低于其他 HMSA 配合物。此外,还研究了大气温度 T=217-298 K 和 p=0.19-1.0 atm 下 HMSA-X 二聚体的形成吉布斯自由能(ΔG),ΔG 随着大气温度的降低和大气压力的降低而降低,表明低温和高压可能显著促进二聚体的形成。