EAGER: Mesoscopic modeling of complex chemical-physical processes at interfaces

EAGER：界面处复杂化学物理过程的介观建模

• 批准号: 2034154
• 负责人: Emily Ryan
• 金额: $ 15.5万
• 依托单位: Trustees of Boston University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2034154&HistoricalAwards=false
• 关键词: EAGER; Mesoscopic; modeling; complex; chemical

In many engineering systems, the physics and chemistry occurring at interfaces in a component are critical to the system’s performance, such as the electrochemical reactions in batteries, cavitation in fuel injectors, pumps and blood vessels, or reactions in chemical reactors. Understanding the physical phenomena and interactions between phases at the interfacial level is critical to designing more efficient systems and new technologies, such as high energy density batteries and drug delivery methods. With computational methods, we can visualize the physical nature of interfaces, making it well positioned to study interfacial processes and to isolate critical phenomena to better understand the chemical-physical driving forces within a system. Additionally, modeling can complement experimental work on elucidating the fundamental chemical-physical processes at the core of many complex engineering systems. For instance, in battery electrodes, optimal performance requires balancing the surface area available for reactions, the pore space available for transport of reactive species, and the connectivity of the solid electrode for charge transport. Neglecting any of these critical phenomena reduces battery performance. This study focuses on developing the computational methods needed to resolve chemical-physical processes at interfaces in the air electrode of high energy density lithium batteries. The project focuses on models that explicitly resolve the interfaces and surrounding regions within the complex porous geometry of the air electrode in a lithium-air battery. In this project, meso-scale model development will focus on modeling the air electrode of a lithium metal battery using smoothed particle hydrodynamics, a Lagrangian particle-based modeling method. The air electrode is a porous carbon-based material and the interfacial region where the air, electrolyte and electrode meet, is the site of the electrochemical reactions. During discharge, Li+ ions travel through the electrolyte to the air electrode where they react with oxygen. In an aprotic electrolyte design, the electrochemical reactions result in non-soluble lithium peroxide (Li2O2). The buildup of Li2O2 passivates the surface of the cathode and can lead to clogging of the pores. This limits the capacity of the battery over multiple charge/discharge cycles as the incomplete dissolution of Li2O2 decreases the capacity. The meso-scale model will focus on modeling the meso-scale behavior of the electrode to resolve the interfacial chemical-physical processes such as transport of species and charge to the reaction sites and the electrochemical reactions that produce Li2O2. The model will be used to investigate the meso-scale physics by explicitly resolving the interface and will study how the interplay between the electrode microstructure, electrolyte and reaction site concentration and locations affect electrode performance.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.

在许多工程系统中，组件界面处发生的物理和化学反应对于系统的性能至关重要，例如电池中的电化学反应、燃料喷射器、泵和血管中的空化，或化学反应器中的反应。界面水平上各相之间的相互作用对于设计更高效的系统和新技术（例如高能量密度电池和药物输送方法）至关重要，通过计算方法，我们可以可视化界面的物理性质，使其能够很好地研究界面。过程和此外，建模可以补充阐明许多复杂工程系统核心的基本化学物理过程的实验工作，例如，在电池电极中，最佳性能需要。平衡可用于反应的表面积、可用于传输活性物质的孔隙空间以及用于电荷传输的固体电极的连接性。本研究的重点是开发解决这些问题所需的计算方法。空气界面的化学物理过程该项目的重点是明确解析锂空气电池中空气电极复杂多孔几何结构内的界面和周围区域的模型。在该项目中，细观模型的开发将侧重于建模。使用平滑粒子流体动力学（一种基于拉格朗日粒子的建模方法）的锂金属电池的空气电极。空气电极是一种多孔碳基材料，空气、电解质和电极相遇的界面区域是在放电过程中，Li+ 离子穿过电解质到达空气电极，在非质子电解质设计中，电化学反应会生成不溶性的过氧化锂 (Li2O2)，从而使表面钝化。由于 Li2O2 的不完全溶解会降低容量，因此这会限制电池在多个充电/放电循环中的容量。介观尺度模型将侧重于对电极的介观尺度行为进行建模，以解决界面化学物理过程，例如物质和电荷向反应位点的传输以及产生Li2O2的电化学反应。通过明确解析界面来研究介观尺度物理，并将研究电极微观结构、电解质和反应位点浓度和位置之间的相互作用如何影响电极性能。该奖项是 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准。

项目成果

SPH simulation of diffusion and coupled concentration dependent ionic migration with precipitation and dissolution

扩散和耦合浓度依赖性离子迁移与沉淀和溶解的 SPH 模拟

• 发表时间: 2021-01
• 期刊: Proceedings of the 15th International SPHERIC Workshop
• 作者: Cannon, Andrew;Ryan, Emily
• 通讯作者: Ryan, Emily

Characterizing the Microstructure of Separators in Lithium Batteries and Their Effects on Dendritic Growth

锂电池隔膜微观结构的表征及其对枝晶生长的影响

• DOI: 10.1021/acsaem.1c00144
• 发表时间: 2021-08-23
• 期刊: ACS Applied Energy Materials
• 影响因子: 6.4
• 作者: Andrew Cannon;E. Ryan
• 通讯作者: E. Ryan

Interfacial studies on the effects of patterned anodes for guided lithium deposition in lithium metal batteries

图案化阳极对锂金属电池引导锂沉积影响的界面研究

• DOI: 10.1063/5.0073358
• 发表时间: 2022-01
• 期刊: The Journal of Chemical Physics
• 作者: Morey, Madison;Loftus, John;Cannon, Andrew;Ryan, Emily
• 通讯作者: Ryan, Emily

Glass-fiber-reinforced polymeric film as an efficient protecting layer for stable Li metal electrodes

玻璃纤维增​​强聚合物薄膜作为稳定锂金属电极的有效保护层

• DOI: 10.1016/j.xcrp.2021.100534
• 发表时间: 2021-01
• 期刊: Cell reports physical science
• 影响因子: 8.9
• 作者: Gao, Shilun;Cannon, Andrew;Sun, Feiyuan;Pan, Yiyang;Yang, Dandan;Ge, Sirui;Liu, Nian;Sokolov, Alexei;Ryan, Emily;Yang, Huabin;et al
• 通讯作者: et al

Smoothed Particle Hydrodynamics Modeling of Electrodeposition and Dendritic Growth Under Migration- and Diffusion-Controlled Mass Transport

迁移和扩散控制的传质下电沉积和枝晶生长的平滑粒子流体动力学模型

• DOI: 10.1115/1.4056327
• 发表时间: 2023-11
• 期刊: Journal of Electrochemical Energy Conversion and Storage
• 影响因子: 2.5
• 作者: Cannon, Andrew;McDaniel, James G.;Ryan, Emily
• 通讯作者: Ryan, Emily