Higuchi Chisa, Yoshizawa Kazunari
Institute for Materials Chemistry and Engineering and IRCCS, Kyushu University, Nishi-ku, Fukuoka 819-0395, Japan.
Langmuir. 2021 Jul 20;37(28):8417-8425. doi: 10.1021/acs.langmuir.1c00635. Epub 2021 Jul 9.
We investigate the adhesive interaction energy (Δ) between an epoxy resin and a silica surface using pair interaction energy decomposition analysis (PIEDA), which decomposes Δ into four components: electrostatic (Δ), exchange repulsion (Δ), charge-transfer (Δ), and dispersion (Δ) energies based on quantum chemistry. Our previous study with PIEDA showed that synergistic effects of Δ and Δ are critical at the interface between an epoxy resin fragment and a hydrophilic surface. The present study is designed to show in detail that the synergistic effects are significant at the interface between an epoxy layer model consisting of 20 epoxy monomers and a hydrophilic silica surface. The ratio of the dispersion energies to the total interaction energies of the layer model shows good agreement with experimental values, that is, the dispersion ratio of the work of adhesion (). The 20 epoxy molecules in the layer model are investigated individually to closely correlate the four decomposed energies with their structural features. Our energy-decomposition analyses show that H-bonding and OH-π interactions play important roles at the interface between an epoxy resin and a silica surface. PIEDA calculations for the epoxy layer model also show that the region 3.6 Å from the silica surface accounts for more than 99% of the total interaction energies.
我们使用成对相互作用能分解分析（PIEDA）研究环氧树脂与二氧化硅表面之间的粘附相互作用能（Δ），该方法基于量子化学将Δ分解为四个分量：静电能（Δ）、交换排斥能（Δ）、电荷转移能（Δ）和色散能（Δ）。我们之前使用PIEDA的研究表明，Δ和Δ的协同效应在环氧树脂片段与亲水性表面之间的界面处至关重要。本研究旨在详细表明，在由20个环氧单体组成的环氧层模型与亲水性二氧化硅表面之间的界面处，协同效应非常显著。层模型的色散能与总相互作用能的比值与实验值吻合良好，即粘附功的色散比（）。对层模型中的20个环氧分子进行单独研究，以将四个分解能与其结构特征紧密关联起来。我们的能量分解分析表明，氢键和OH-π相互作用在环氧树脂与二氧化硅表面之间的界面处起重要作用。环氧层模型的PIEDA计算还表明，距离二氧化硅表面3.6 Å的区域占总相互作用能的99%以上。
