Development of Imidazolium-Based Parameters for AMOEBA-IL.
Development of Imidazolium-Based Parameters for AMOEBA-IL.
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DOI：
10.1021/acs.jpcb.3c00986
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发表时间：
2023-06
期刊：
影响因子：
--
通讯作者：
José Enrique Vázquez-Cervantes;G. Cisneros
中科院分区：
文献类型：
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作者：
José Enrique Vázquez-Cervantes;G. Cisneros
提出了一种新的可极化离子液体势能的有效参数化方法--阿米巴-IL，并将其应用于咪唑基阳离子参数的确定。新的方法依赖于片段参数的开发，这些片段可以被转移来产生新的分子。该参数化使用了原始的阿米巴-IL参数化方法，包括对永久多极子使用高斯静电模型-分布多极子(GEM-DM)，以及使用量子力学能量分解分析(QM-EDA)数据近似van der Waals参数。在此基础上，将所选择的初始结构的官能团作为构筑块来开发具有较长烷基的新型咪唑基阳离子(对称或不对称)的参数。通过对称性适应微扰理论(SAPT)的能量分解分析和平衡校正的总分子间相互作用，将该方法得到的参数与QM文献的分子间相互作用进行了比较。通过对一系列含有不同阴离子的咪唑基离子液体进行分子动力学模拟，比较了密度ρ、蒸发热Δ、径向分布函数g(R)和扩散系数D±等热力学和输运性质，验证了新的参数化阳离子的有效性。总体而言，计算的气相和体积性质与参考数据吻合较好。新的程序提供了一种直接的方法来产生任何咪唑基阳离子所需的阿米巴-IL参数。
A new approach for the efficient parametrization of the polarizable ionic liquid potential AMOEBA-IL and its application to develop parameters for imidazolium-based cations is presented. The new approach relies on the development of parameters for fragments that can be transferred to generate new molecules. The parametrization uses the original AMOEBA-IL parametrization approach, including the use of Gaussian electrostatic model-distributed multipoles (GEM-DM) for the permanent multipoles and approximation of the van der Waals parameters using quantum mechanics energy decomposition analysis (QM-EDA) data. Based on this, functional groups of the selected initial structures are employed as building blocks to develop parameters for new imidazolium-based cations (symmetric or asymmetric) with longer alkyl chains. The parameters obtained with this proposed method were compared with intermolecular interactions from QM references via energy decomposition analysis using symmetry adapted perturbation theory (SAPT) and counterpoise-corrected total intermolecular interactions. The validation of the new parametrized cations was carried out by running molecular dynamics simulations on a series of imidazolium-based ionic liquids with different anions to compare selected thermodynamic and transport properties, including density ρ, enthalpy of vaporization ΔHvap, radial distribution function g(r), and diffusion coefficients D±, with experimental data. Overall, the calculated gas-phase and bulk properties show good agreement with the reference data. The new procedure provides a straightforward approach to generating the required AMOEBA-IL parameters for any imidazolium-based cation.