多相反应过程中的表界面结构和相际传递现象研究

By exploring the structures of fluids on the material surfaces/interfaces and the multi-phase reaction processes, especially for the formation of surface/interface structures, transfer phenomena between different phases and the coupling relation between the transfer and reaction processes, we aim at establishing (1) multi-scale equilibrium density functional theory; (2) non-equilibrium statistical mechanics models; (3) multi-scale simulation method of combining the quantum chemistry calculations and molecular simulations. We would also develop the corresponding experimental techniques in meso-scale to investigate the structures and kinetics of fluids on the surfaces/interfaces, and further verify the theoretical models and simulation methods constructed. By combining these theoretical, simulation and experimental investigations, we would explore the mechanism of molecular aggregation behavior in the surfaces/interfaces, and the effects of molecular interactions and configuration entropy on the formation of surface/interface structure in the meso-scale, and further study the effects of the formed surface/interface structure on the transfer behavior between different phases. The understanding of the microscopic behavior will be also applied to investigate the mcroscopic phenomena including the influence of the solid-fluid interface structure on the particle aggregation and the influence of adsorption and diffusion of reactants on the surfaces/interfaces on the catalytic efficiency of the catalysts. The success of this project will provide solid support and theoretical guidance for development of multiphase transfer and reaction process intensification techniques in meso-sacle.

本项目针对材料表界面介尺度，围绕多相反应过程中的表界面结构、相际传递过程及其与反应过程的耦合，建立多尺度的平衡态密度泛函理论、非平衡态统计力学理论的新框架、量子化学计算和分子模拟结合的多尺度模拟方法，开发多相系统界面结构、界面性质、跨膜传递分离过程的多尺度实验方法。采用理论分析、计算机分子模拟和实验研究相结合的方法，在分子、表界面和固体颗粒群三个尺度上揭示表界面区域的分子聚集结构、分子间相互作用和分子构像熵效应对表界面结构的影响、表界面结构对相际传递过程的影响、固液界面液体结构对固体颗粒相互作用的影响、流动介质中固体颗粒的动态聚团行为、多孔材料中物质传递与界面催化反应的相互作用，为多相传递和反应过程强化技术的开发提供理论指导。

本项目聚焦多相反应过程中的表界面结构和相际传递现象，建立了描述多尺度表界面结构和性质的密度泛函理论统一框架，在此框架下发展了气体混合物吸附分离用多孔材料快速筛选的经典密度泛函理论方法、超级电容器材料结构与储能性能关系的密度泛函理论和固体表面锚接高分子刷智能响应的格子高分子密度泛函理论，建立了描述界面传递现象和膜分离过程的动态密度泛函理论，采用量子化学计算和分子模拟结合的多尺度模拟方法，模拟研究了固体表面性质对界面结构及传递特性的影响。在理论指导下，合成了多种新型多孔材料，在气体分离、膜分离、荧光检测等方面具有很好的应用潜力。项目执行期间，在AIChEJ、Angm. Chem. Intl. Ed.、Adv. Mater.等发表相关学术论文73余篇，出版《密度泛函理论》专著1部，培养博士生15名，硕士生5名，项目组成员曹大鹏教授获国家杰出青年科学基金资助。

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