Quantum-Designed Models of Bulk and Interfacial Solvation

体相和界面溶剂化的量子设计模型

• 批准号: 1955161
• 负责人: Thomas Beck
• 金额: $ 51万
• 依托单位: University of Cincinnati Main Campus
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-04-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955161&HistoricalAwards=false
• 关键词: Quantum; Designed; Models; Bulk; Interfacial

Thomas Beck of the University of Cincinnati is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop new theoretical and computational methods to better understand complex liquid mixtures. Beck and his research group develop and use advanced computer simulations to investigate how molecules interact with each other to produce the great complexity in living things, industrial chemistry, household chemicals such as soaps, and battery materials. They use these advanced methods to model the basic properties of various charged particles (ions) in water and near the water surface. They also extend these techniques to studies of ions in organic liquids that are used in lithium ion batteries. In addition, the Beck group employs the new calculations to model phase separation in liquid mixtures relevant to industrial chemical processes. Accuracy is important because slight changes in the force fields that describe interactions between molecules often lead to completely different theoretical behaviors of the mixture. Gaining more insight into the interactions and resulting system properties results, for example, in the development of more efficient and safer battery materials. Communicating this basic science to the broader community is increasingly important, and Beck oversees a program at the Cincinnati Museum Center that will train 10 Ph.D. students from his Department to engage in effective science demonstrations on the floor of the museum. Solvation and interfacial phenomena are central to a diverse array of physical, chemical, and biological systems including nanomaterials, surfactants, synthetic chemistry, membranes, proteins, and the energy sciences. While significant progress has been made in developing accurate models of complex ionic and molecular mixtures and interfaces, major challenges remain in building a predictive science of solvation. The principal objectives of this grant are threefold. The Beck group performs extensive ab initio quantum molecular dynamics simulations coupled with advanced statistical mechanical theories that establish a fundamental single-ion free energy scale in water and that explores the basic structure and dynamics of ion solvation in organic solvents. The team utilizes data from the ab initio simulations in constructing novel quantum-designed models that incorporate the essential physical components of solvation. They also applying these new models to challenging systems such as predicting liquid-liquid equilibrium and competitive solvent binding to ions in complex molecular mixtures. The theoretical methods employed include distributed charge multipole models and Drude oscillators optimized with evolutionary algorithms to mimic the electronic distributions in the condensed phase quantum simulation data. The resulting predictive computational models are employed in studies of interfacial electrostatics, specific ion effects in solution and near interfaces, and in ion solvation studies in organic solvents used in energy storage devices and in green chemistry processes.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.

辛辛那提大学的Thomas Beck得到了化学系化学理论、模型和计算方法项目的支持，以开发新的理论和计算方法来更好地理解复杂的液体混合物。贝克和他的研究小组开发并使用先进的计算机模拟来研究分子如何相互作用，从而在生物、工业化学、肥皂等家用化学品和电池材料中产生巨大的复杂性。他们使用这些先进的方法来模拟水中和水面附近各种带电粒子(离子)的基本性质。他们还将这些技术扩展到对用于锂离子电池的有机液体中的离子的研究。此外，Beck团队还使用新的计算方法对与工业化学过程相关的液体混合物中的相分离进行建模。准确性很重要，因为描述分子间相互作用的力场的微小变化往往会导致混合物的理论行为完全不同。对相互作用和由此产生的系统性能有更多的了解，例如，在开发更高效和更安全的电池材料方面。向更广泛的社区传播这一基础科学越来越重要，贝克在辛辛那提博物馆中心负责一个项目，该项目将培训他所在部门的10名博士生，让他们在博物馆的地板上进行有效的科学演示。溶剂化和界面现象是各种物理、化学和生物体系的核心，包括纳米材料、表面活性剂、合成化学、膜、蛋白质和能源科学。虽然在开发复杂的离子和分子混合物和界面的准确模型方面取得了重大进展，但在建立溶剂化预测科学方面仍然存在重大挑战。这笔赠款的主要目标有三个。Beck小组进行了大量的从头算量子分子动力学模拟，结合先进的统计力学理论，建立了水中基本的单离子自由能标度，并探索了有机溶剂中离子溶剂化的基本结构和动力学。该团队利用从头计算模拟的数据来构建新的量子设计模型，该模型包含了溶剂化的基本物理成分。他们还将这些新模型应用于具有挑战性的系统，如预测液-液平衡和复杂分子混合物中竞争溶剂与离子的结合。所采用的理论方法包括分布式电荷多极模型和用进化算法优化的Drude振子，以模拟凝聚相量子模拟数据中的电子分布。由此产生的预测计算模型被用于研究界面静电学、溶液和界面附近的特定离子效应，以及用于储能设备和绿色化学过程的有机溶剂中的离子溶剂化研究。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势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

Absolute ion hydration free energy scale and the surface potential of water via quantum simulation

通过量子模拟的绝对离子水合自由能尺度和水的表面电势

• DOI: 10.1073/pnas.2017214117
• 发表时间: 2020
• 期刊: Proceedings of the National Academy of Sciences
• 作者: Shi, Yu;Beck, Thomas L.
• 通讯作者: Beck, Thomas L.

Molecular Basis of CLC Antiporter Inhibition by Fluoride

• DOI: 10.1021/jacs.9b13588
• 发表时间: 2020-04-22
• 期刊: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
• 影响因子: 15
• 作者: Chiariello, Maria Gabriella;Bolnykh, Viacheslav;Carloni, Paolo
• 通讯作者: Carloni, Paolo

Quantum Simulations of Hydrogen Bonding Effects in Glycerol Carbonate Electrolyte Solutions

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
• 发表时间: 2021
• 期刊: The Journal of Physical Chemistry B
• 作者: Eisenhart, Andrew E.;Beck, Thomas L.
• 通讯作者: Beck, Thomas L.

Specific Ion Solvation and Pairing Effects in Glycerol Carbonate

碳酸甘油酯中的特定离子溶剂化和配对效应

• DOI: 10.1021/acs.jpcb.1c06575
• 发表时间: 2021
• 期刊: The Journal of Physical Chemistry B
• 作者: Eisenhart, Andrew E.;Beck, Thomas L.
• 通讯作者: Beck, Thomas L.