离子液体作为一种新型绿色溶剂，具有低的蒸汽压、高的化学稳定性和可设计性等优点，在诸多领域展现出巨大的应用潜力。离子液体的优良特性与其自身复杂的分子间作用是分不开的，如阴阳离子间的长程静电作用、独特的氢键作用以及色散作用等，其中氢键作用在反应、与有机小分子分离或水分子混合中都起到重要的作用。分子模拟作为原子尺度的研究手段，有助于分析离子液体体系的相互作用、建立结构-性质关系。鉴于离子液体氢键的重要性，对常用的咪唑类离子液体，本论文建立了其氢键力场，通过分子动力学模拟获得准确物性并分析了局部结构与离子液体性质之间的关系；另外针对应用中常见的离子液体与水的混合体系，研究了离子液体在水溶液中形成团簇结构并着重分析了囊泡结构的形成机理与渗透行为；最后，为离子液体大规模计算，构建了粗粒化力场并优化参数。主要研究内容如下：（1）离子液体氢键力场的开发。针对1-烷基-3-甲基咪唑氯盐（[Rmim][Cl]）这类存在强氢键作用的体系，提出了平均极化（电荷）与局部极化（氢键）共存的分子力场开发方案。通过从头计算分子动力学模拟计算多离子对的液相结构，拟合其静电势获得原子电荷；氢键势函数采用角度修正的三体Morse势函数的形式，其参数通过分析离子对的氢键能量，并结合力场中的相关作用参数共同优化获得。在后续的分子动力学模拟中，分析了氢键位置的径向分布函数，与从头计算分子动力学的模拟结果对比，验证了结构的合理性。对[Emim][Cl]离子液体的分子动力学模拟，研究径向分布函数和空间分布函数，发现阳离子之间存在π-π堆积的结构；另外计算了阴离子在阳离子周围的分布情况，发现氢键结构具有一定局域性，与静电结构不同。通过对结构的分析，发现阴阳离子的动力学性质（粘度和自扩散系数）与离子对的作用时间具有良好的线性关联。（2）离子液体结构对粘度的影响。采用分子动力学模拟和量子化学计算的方法，系统地研究了[Bim][NTf2]、[Bmim][NTf2]和[Bmmim][NTf2]三种含有不同氢键强度和氢键数目的体系的粘度与离子对结构、氢键数目、能量以及作用时间之间的关系，并通过量子化学研究阳离子结构与粘度之间的关系。在粘度性质的计算中，采用周期性微扰的方法，系统地分析了模拟体系大小、微扰加速度振幅对粘度计算值的影响。发现在模拟体系中粒子的速度场呈现完美的余弦函数形式时粘度的计算值最可信，并且微扰加速度振幅合理的选择值与模拟体系z轴方向大小呈现对应关系。离子液体的粘度与离子的空间分布有明显的关系，即阴离子在阳离子周围分布越广则体系粘度越低；粘度与离子对的作用时间存在线性关联，粘度的大小与氢键的作用时间相关。另外，分析阳离子的结构发现，结构对称、各作用点的强度相当且分布均匀的离子液体，其粘度较低。（3）离子液体在水溶液体系中团簇结构研究。发现[C12mim][Sal]离子液体在水溶液体系中可以形成胶束结构，调整初始结构及模拟条件，可形成平面、带状、管状和囊泡的团簇结构。通过分子动力学模拟，直观地看到离子液体囊泡形成的全过程，研究发现囊泡的结构是双分子层结构，其中亲水的基团分布在离子液体与水界面处；能量分析表明阴阳离子间的相互作用是囊泡体系稳定的关键。针对模拟中观察到的水分子透过囊泡现象，研究了不同温度下囊泡内水分子的扩散行为，发现在不破坏囊泡结构的前提下，升高温度会使得囊泡内外水分子交换加快。最后模拟计算了两个囊泡的融合过程。（4）离子液体粗粒化模型与团簇结构策略。针对[C12mim][Br]-水体系，划分粗粒模型片段，通过全原子分子动力学模拟获得的结构信息，采用IBI的方法拟合粗粒化模型的势函数。拟合中不断地调整参数最终使得径向分布函数的误差最小，各部分间的有效势函数收敛。粗粒化力场势函数应用到分子动力学模拟中，并通过密度、自扩散系数和结构等结果验证其正确性。最后采用粗粒化势函数，对离子液体的大规模体系进行模拟研究，发现离子液体可以形成棒状的簇结构，本工作为后续研究离子液体的大规模计算有一定的指导作用。 ;Room temperature ionic liquids (ILs) are special class of molten salts composed solely of ions (cations and anions), which are in the liquid state at temperature less than 373K. As novel solvents, it is widely believed that ILs are low volatility, high thermal stability, non-flammability, high conductivity, designable characteristic and they have been successfully used as catalysts, solvents, and electrolytes. The unique properties of ILs are decided by their special structures, the various interactions between cation and anion, such as electrostatic interaction, hydrogen bond interaction and dispersion interaction. Molecular dynamic simulation, as a method based on atom or molecular model, play an important role in recent studies of ILs. Molecular dynamic could supply help for investigation on the interaction and structure-properties relationship between ILs. In this work, we have developed an all-atom force field with three-body hydrogen bond model for 1-alkyl-3-methyl-imidazolium chloride ([Rmim][Cl]), predicted the experimental dynamic viscosity successfully and calculated the relationship between dynamic properties and ion pair lifetime by using molecular dynamics simulation. And the effect of local hydrogen bonding structure of ILs on the viscosities was studied. For the application of ILs in water system, the aggergation structures were simulated and the formation mechanism and transport properties of vesicle were further analyzed. Finally, a coarse grain model of [C12mim][Br]-water was developed and the potential profiles were optimized. The main contents and results are as follow:(1) Designing of force field with three-body hydrogen bond model and the study on the relationship between ion pairs and dynamic properties of ILs. A refined non-polarizable force field was proposed, which combined the mean polarizable effect on the scaled charge strategy and local polarizable effect on the hydrogen bond model. Ab initio molecular dynamic simulation of 32 ion pairs was carried out and then fitted the charges distribution, the statistics of various configurations and different ions surround environment for a long real time enable to represent the mean polarizability much more reality. Considering the local unique hydrogen bonding interactions, a modified Morse Potential Hydrogen Bond interaction model was adopted into force field for describing the hydrogen bond interaction, and the parameters were optimized by calculated the hydrogen bonding ion pair structure. The force field was verified by comparing the radial distribution function of hydrogen atom in imidazolium ring and anions with the AIMD results. And the calculated densities were agreement with the experimental values. The structure of [Emim][Cl] was further studied by radial distribution function and space distribution functions, finding the π-π stack of cations. Furthermore, the distributions of anions around the cation were displayed. The shear viscosity was calculated by using Green-Kubo relations, considering statistics based on the time decomposition method. And the shear viscosities computed by using the force fields with hydrogen bond model showed very good agreement with experimental data. The lifetime of ion pairs were also calculated and the results were in linear relation with dynamic properties.(2) Study on the influence of the local hydrogen bond structure on the shear viscosity of ILs by using molecular dynamics and quantum mechanism. The shear viscosity was calculated by using periodic perturbation method, and the parameters for obtaining accurate calculated viscosity value was evaluated. The results indicated that the perfect cosine-like velocity profile was the key to get the reasonable calculated viscosity. And the amplitude of perturbation acceleration is directly related to the z-direction length of the simulated box. And the accurate viscosities were obtained correspond to the experimental values. Furthermore, the calculated viscosities correlated to the lifetime of ion pairs. The structure of three ionic liquids were analyzed by Radial distribution functions and space distribution functions. And the structural distribution differences could be used to explain viscosities, the local aggregation of anions in certain site of cation prevent the ion movement and increase the viscosity. The hydrogen bond interactions were further analyzed to reveal the relationship between viscosities and local structure. The multiple interaction site and modest strength of interacting energy difference lead the lower viscosities of [Bmim][NTf2]. This is an indication for the design of lower viscosity ionic liquids.(3) Study on the aggregation structure of ionic liquid in aqueous system. It was found that [C12mim][Sal] ionic liquid could form the aggregation structure as the micelle and vesicle in aqueous by using molecular dynamic simulations. The structure and interaction energy of the ionic liquid unilamellar vesicle were then investigated and indicated that the vesicle was a perfect bilayer structure and interaction energy of cation and anion played an important role in stabilizing the structure. Then the entire forming process of vesicle from the random distribution of ILs were simulated and reveal the formation mechanism. For application, the permeability of vesicle were further analyzed by computing time correlation function of water molecules inside the vesicle at a series different temperatures. The results indicated that water could be rapid exchange as the temperature increase, while the vesicle structure still maintain. Finally, the fusion simulation of two vesicles were further carried out.(4) Study on coarse grain force field and further molecular dynamic simulation. For large scale and length time simulation, the coarse grain force field were developed by using Iterative Boltzmann Inversion method. The potential energy function for coarse grain model were optimized after 120 iteration, and the RDF obtained from the coarse grain model were consistent with the all-atom force field results. The molecular dynamic simulations based on coarse grain force field were carried out, and the densities at different temperature were in good agreement with the all-atom force field results. The self-diffusion coefficient was a little larger as the coarse grain model was much simpler, and the freedom was decreased. The further simulation on larger system and found the aggregation structure of ionic liquids.