Quantum Simulations of Hydrogen Bonding Effects in Glycerol Carbonate Electrolyte Solutions
Quantum Simulations of Hydrogen Bonding Effects in Glycerol Carbonate Electrolyte Solutions
复制标题
碳酸甘油酯电解质溶液中氢键效应的量子模拟
DOI：
10.1021/acs.jpcb.0c10942
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发表时间：
2021
期刊：
影响因子：
--
通讯作者：
Beck, Thomas L.
中科院分区：
文献类型：
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作者：
Eisenhart, Andrew E.;Beck, Thomas L.
在电化学和其他领域中对环境友好的非水溶剂的需求激发了最近对候选有机液体的分子水平溶剂化结构、热力学和动力学的研究。在本文中，我们提出了量子密度泛函理论模拟的结果，碳酸甘油酯（GC），分子已被提议作为溶剂的绿色工业化学，非水的替代品的生物催化反应，和液体介质中的能量存储设备。我们调查的结构和动力学的纯GC液体和电解质溶液中含有KF和KCl离子对。这些模拟揭示了氢键的重要性，控制纯液体和离子缔合的电解质溶液中的结构和动力学行为。结果表明，与经典的复杂的有机溶剂建模的困难。模拟导致更好地理解背后的机制先前观察到的奇特的离子特定的行为在GC电解质溶液。
The need for environmentally friendly nonaqueous solvents in electrochemistry and other fields has motivated recent research into the molecular-level solvation structure, thermodynamics, and dynamics of candidate organic liquids. In this paper, we present the results of quantum density functional theory simulations of glycerol carbonate (GC), a molecule that has been proposed as a solvent for green industrial chemistry, nonaqueous alternatives for biocatalytic reactions, and liquid media in energy storage devices. We investigate the structure and dynamics of both the pure GC liquid and electrolyte solutions containing KF and KCl ion pairs. These simulations reveal the importance of hydrogen bonding that controls the structural and dynamic behavior of the pure liquid and ion association in the electrolyte solutions. The results illustrate the difficulties associated with classical modeling of complex organic solvents. The simulations lead to a better understanding of the underlying mechanisms behind the previously observed peculiar ion-specific behavior in GC electrolyte solutions.