Unraveling Mechanisms of Strongly Correlated Dynamics in Ionic Systems

揭示离子系统中强相关动力学的机制

• 批准号: 2102425
• 负责人: Alexei Sokolov
• 金额: $ 49.95万
• 依托单位: University of Tennessee Knoxville
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-08-15 至 2024-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102425&HistoricalAwards=false
• 关键词: Unraveling; Mechanisms; Strongly; Correlated; Dynamics

In this project funded by the Chemical Structure Dynamics and Mechanisms-A (CSDM-A) program of the Chemistry Division, Professors Alexei Sokolov and Stephen Paddison of the University of Tennessee will combine experimental and computational studies to develop a fundamental understanding of the mechanisms controlling correlations in ion dynamics in concentrated ionic systems. These correlations strongly influence ionic conductivity, and their mechanism remains a mystery. Using a broad array of experimental techniques combined with high fidelity simulations, a detailed molecular-level description of the distinct ion-ion correlations that may enhance or suppress conductivity in liquid and solid electrolytes is being developed. The results of these studies will likely impact the fundamentals of a wide range of ion conducting materials and will be important for rational design of novel electrolytes for various electrical energy storage technologies. The students and postdoc engaged in this project will gain valuable experience in sophisticated experimental and computational research. The Sokolov research group is also engaged in various outreach activities targeted at K-12 audiences.This project focuses on synergistic experimental and computational studies of ion and charge transport in ionic liquids, polymerized ionic liquids and organic ionic plastic crystals. Experiments involve Broadband Dielectric Spectroscopy, neutron scattering, and NMR will be combined with ab initio and classical atomistic molecular dynamics (MD) simulations and electronic structure calculations. The proposed study will likely provide a comprehensive knowledge of the role of ion size, disparity in the ion and counter-ion mobility, and electrostatic interactions on ionic correlations. The results will also reveal specific structure or compositions that may tune ion-ion correlations from negative (suppressing conductivity) to positive (enhancing conductivity). This study will help to develop design criteria for novel electrolytes that may be utilized in solid state batteries, flow batteries and other electrochemical applications, and provide good opportunities for the training of graduate students and postdoctoral researchers.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在这个由化学系化学结构动力学和机制-A（CSDM-A）计划资助的项目中，田纳西大学的Alexei Sokolov教授和Stephen Paddison教授将联合收割机实验和计算研究相结合，以发展对浓缩离子系统中离子动力学相关性控制机制的基本理解。这些相关性强烈影响离子电导率，其机制仍然是一个谜。使用广泛的实验技术结合高保真度模拟，一个详细的分子水平的描述不同的离子-离子的相关性，可能会提高或抑制液体和固体电解质的导电性正在开发。这些研究的结果可能会影响广泛的离子传导材料的基本原理，并且对于合理设计用于各种电能存储技术的新型电解质非常重要。参与该项目的学生和博士后将获得在复杂的实验和计算研究的宝贵经验。 Sokolov研究小组还参与了针对K-12受众的各种外联活动。该项目侧重于离子液体、聚合离子液体和有机离子塑料晶体中离子和电荷传输的协同实验和计算研究。实验涉及宽带介电谱，中子散射和NMR将结合从头算和经典原子分子动力学（MD）模拟和电子结构计算。拟议的研究可能会提供一个全面的知识的作用，离子的大小，差距的离子和反离子的流动性，和静电相互作用的离子相关性。结果还将揭示可以将离子-离子相关性从负（抑制导电性）调整到正（增强导电性）的特定结构或组成。这项研究将有助于开发可用于固态电池、液流电池和其他电化学应用的新型电解质的设计标准，并为研究生和博士后研究人员的培训提供良好的机会。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Exploration of phase diagram, structural and dynamic behavior of [HMG][FSI] mixtures with NaFSI across an extended composition range

探索 [HMG][FSI] 与 NaFSI 混合物在扩展组成范围内的相图、结构和动态行为

• DOI: 10.1039/d2cp01910h
• 发表时间: 2022
• 期刊: Physical Chemistry Chemical Physics
• 影响因子: 3.3
• 作者: Biernacka, Karolina;Makhlooghiazad, Faezeh;Popov, Ivan;Zhu, Haijin;Chotard, Jean-Noël;O’Dell, Luke A.;Sokolov, Alexei P.;Pringle, Jennifer M.;Forsyth, Maria
• 通讯作者: Forsyth, Maria