Maghami Mahboobeh, Abdelrasoul Amira
Department of Chemical and Biological Engineering, University of Saskatchewan, 57 Campus Drive, Saskatoon, Saskatchewan, S7N 5A9, Canada.
Department of Chemical and Biological Engineering, University of Saskatchewan, 57 Campus Drive, Saskatoon, Saskatchewan, S7N 5A9, Canada; Global Institute of Water Security, 11 Innovation Blvd, Saskatoon, Saskatchewan, S7N 3H5, Canada.
J Mol Graph Model. 2020 May;96:107540. doi: 10.1016/j.jmgm.2020.107540. Epub 2020 Jan 18.
The origins of low and high interactions of polar groups with water molecules are still unknown and need to be further examined for effective future membrane synthesis and modification. The primary aim of this research study is to provide a comprehensive overview of the interactions at the molecular level occurring between water molecules and the fragments of hydrophobic and hydrophilic membranes based on pair interaction energy decomposition analysis (PIEDA) as part of the fragment molecular orbital (FMO) method's framework. This direction is critical, since a research study of the reasons for water and membrane interactions can help design groundbreaking membranes with superior hydrophilicity characteristics. To accomplish this, the computational studies, the Polyvinylidene fluoride (PVDF [H(-CH-CF-)CH]) and Polyacrylonitrile (PAN [(H(-CH-CH(CN)-)CH]) membranes were considered as models for hydrophobic and hydrophilic membranes, respectively. Density-functional theory (DFT), based on B3LYP functional and split-valance 6-311+G (d,p) basis sets, was used in order to optimize the geometry of PAN, PVDF, and their complexes with different numbers of water molecules. Furthermore, fragment molecular orbit (FMO) and the Pair Interaction Energy Decomposition Analysis (PIEDA) were carefully interrogated. These types of analyses included the inter fragment interaction energy (IFIE), like the electrostatic (ES), exchange repulsion (EX), charge-transfer and mixing term (CT + mix) energies. Furthermore, the hydrophilicity and hydrophobicity of the origins of membrane function groups were experimentally evaluated through Fourier-transform infrared spectroscopy (FTIR- ATR), C cross polarization magic angle spinning (C CP MAS) Solid State Nuclear magnetic resonance SSNMR, and Fourier transform Raman (FT-Raman) spectroscopies. Confocal microscopic approach was used to interrogate water transport and the interactions between fluorescence particles and membrane layers. Furthermore, the Infrared (IR) spectroscopy was performed to investigate interaction between water molecules and PVDF and PAN. The theoretical results had a good agreement with experimental result.
极性基团与水分子之间低相互作用和高相互作用的起源仍然未知，为了未来有效地进行膜的合成和改性，需要进一步研究。本研究的主要目的是基于片段分子轨道（FMO）方法框架中的对相互作用能分解分析（PIEDA），全面概述水分子与疏水和亲水膜片段之间在分子水平上的相互作用。这个方向至关重要，因为对水与膜相互作用原因的研究有助于设计出具有卓越亲水性特征的开创性膜。为实现这一目标，计算研究中分别将聚偏氟乙烯（PVDF [H(-CH-CF-)CH]）和聚丙烯腈（PAN [(H(-CH-CH(CN)-)CH]）膜视为疏水膜和亲水膜的模型。基于B3LYP泛函和分裂价6-311+G(d,p)基组的密度泛函理论（DFT），用于优化PAN、PVDF及其与不同数量水分子形成的复合物的几何结构。此外，还仔细研究了片段分子轨道（FMO）和对相互作用能分解分析（PIEDA）。这些类型的分析包括片段间相互作用能（IFIE），如静电（ES）、交换排斥（EX）、电荷转移和混合项（CT + mix）能量。此外，通过傅里叶变换红外光谱（FTIR-ATR）、碳交叉极化魔角旋转（C CP MAS）固体核磁共振（SSNMR）和傅里叶变换拉曼（FT-拉曼）光谱，对膜功能基团起源的亲水性和疏水性进行了实验评估。采用共聚焦显微镜方法研究水的传输以及荧光颗粒与膜层之间的相互作用。此外，进行红外（IR）光谱研究水分子与PVDF和PAN之间的相互作用。理论结果与实验结果吻合良好。
