离子液体混合体系（ILMs）具有“小差异大变化”的特性，被称之为第四代功能离子液体和“软物质“。目前，尽管人们对ILMs的物理化学性质有一定了解，但对其混合组分分子间相互作用、不同尺度团簇/聚集体结构和动态变化的研究还十分有限。本项目拟从前期工作出发，基于相互作用力拟合（FM）方法，建立更为严谨的“自下而上”的极化电荷力场模型，CG-EEM-FM。准确模拟ILMs的超额性质、离子缔合、极化效应等，统计分析研究团簇/聚集体在不同尺度上静态或动态的不均匀结构。实验上精准测量ILMs的热力学和传输性质，DLS和SAXS等光谱分析研究ILMs中颗粒大小、纳微结构和组成的关系。最后全方位综合实验和理论结果，明确ILMs中离子对、团簇/聚集体、纳微粒子等多尺度结构的形成和演变，提出ILMs混合机制和相分离过程的理论本质等。拓宽ILMs在气体吸收、生物质溶解、电化学、反应介质等方面的应用。

Recently, interest has tremendously increased in the ionic liquid mixtures (ILMs), which have been widely considered as the 4th Evolution of ionic Liquids and soft materials due to their “small difference, and then big change”properties. Although the physicochemical properties of ILMs has been received much attention, knowledge about the intermolecular force and static structures and dynamic changes of aggregations at the different scale in ILMs is a requisite for understanding the ILMs properties. In this project, we combine the application of experiments, theoretical model, and multiscale molecular dynamics (MD) to explore the structure-function relationship. First, a new “bottom-up”polarizable model, CG-EEM-FM, is developed for ILMs, based on the application of a force-matching method to the trajectories and forces obtained from the atomistic trajectory and force data for the CG sites of the ILMs. The excess properties, ionic association, polarizable effect, spatial distribution function are clearly described. The static and dynamic heterogeneous structures of aggregations at the different scale have been explored by the statistical analysis. Second, the values of thermodynamic and transferable properties are measured by experiments, and small angle x-ray scattering (SAXS) and dynamic light scattering (DLS) have been used to study the particle distributions and nanostructures. Finally, by the result of experiments and MD simulations, the formation and change of ionic pairs, aggregations, nanostructures have been clearly understood and supported, and the theoretical nature of solvation and separation mechanics of ILMs has been validated. Our study is aimed to broaden the ILMs’ applications in the areas of gas capture, biomaterials dissolution, reaction medium, electrochemistry, and this is most encouraging.