CAREER: Understanding the Influence of the Framework on Alkali Ion Diffusion in Polyanionic Intercalcation Electrodes

职业：了解框架对聚阴离子插层电极中碱离子扩散的影响

• 批准号: 1554204
• 负责人: Brent Melot
• 金额: $ 60万
• 依托单位: University of Southern California
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-03-01 至 2023-10-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1554204&HistoricalAwards=false
• 关键词: CAREER; Understanding; Influence; Framework; Alkali

Non-Technical AbstractFrom cellular phones to portable computers, many major technological advances in recent years have relied on the ability to store massive amounts of energy within extremely small batteries. These batteries operate by reversibly inserting and removing Li-ions from electrochemically active host materials. The goal of this work, supported by the Solid State and Materials Chemistry program within the Division of Materials Research, is to build a deeper understanding of what happens at the atomic level of these hosts as Li-ions move through their crystal structures. This fundamental knowledge is crucial for increasing the rate at which batteries can be (dis)charged as well as prolonging their operational lifetime. In parallel, this work seeks to use this understanding to identify new Earth-abundant electrode materials for Na-ion batteries in order to reduce the cost of producing large-scale energy storage systems for electric vehicles and the grid. This project also focuses on encouraging middle school students in the Native American communities located within the Los Angeles area to increase their participation in STEM disciplines. Hands-on teaching demonstrations and experiments are used to demystify the often puzzling world of electricity and energy sciences to engage students in science from an early age.Technical AbstractPolyanionic transition metal compounds (like phosphates, sulfates, and silicates) are of critical importance to energy storage because they do not release oxygen on decomposition, which can exacerbate thermal runaway during cell failure, and are therefore considerably safer than oxide-based electrodes. While a large body of work has been dedicated to optimizing the electrochemical performance of these materials, there is a fundamental lack of understanding about the mechanism for Li-ion transport in these materials. Unlike state-of-the-art oxides, which effectively exhibit isotropic changes in their oxygen sublattice, polyanionic electrodes respond to the removal or insertion of Li through cooperative rotations of their rigid oxoanionic subunits. This work is focused on investigating the mechanism of alkali-ion diffusion in polyanionic intercalation hosts using high-resolution X-ray and neutron diffraction techniques in order to characterize how the framework of these materials changes on charge and discharge. Understanding how these densely packed solids facilitate the motion of positively charged ions through their lattices is critical for accelerating the design of next-generation materials for batteries that can operate based on the transport of larger ions like Na.

从移动电话到便携式电脑，近年来许多重大的技术进步都依赖于在极小的电池中存储大量能量的能力。这些电池通过可逆地从电化学活性主体材料中插入和取出锂离子来工作。这项工作得到了材料研究部固态和材料化学项目的支持，其目标是更深入地了解当锂离子穿过它们的晶体结构时，在这些宿主的原子水平上发生了什么。这些基本知识对于提高电池的充放电率以及延长电池的使用寿命至关重要。与此同时，这项工作试图利用这种理解来确定新的地球丰富的钠离子电池电极材料，以降低为电动汽车和电网生产大规模储能系统的成本。该项目还侧重于鼓励位于洛杉矶地区的美国原住民社区的中学生增加他们对STEM学科的参与。动手教学演示和实验被用来揭开经常令人困惑的电力和能源科学世界的神秘面纱，让学生从小就参与科学。技术摘要：聚阴离子过渡金属化合物（如磷酸盐、硫酸盐和硅酸盐）对储能至关重要，因为它们在分解时不释放氧气，而氧气会加剧电池失效时的热失控，因此比基于氧化物的电极安全得多。虽然大量的工作致力于优化这些材料的电化学性能，但人们对这些材料中锂离子传输的机制缺乏基本的了解。与最先进的氧化物不同，它们在氧亚晶格中有效地表现出各向同性的变化，聚阴离子电极通过其刚性氧阴离子亚基的协同旋转来响应Li的移除或插入。本研究主要利用高分辨率x射线和中子衍射技术研究碱离子在多阴离子嵌入体中的扩散机制，以表征这些材料在充放电时的结构变化。了解这些密集堆积的固体如何促进带正电荷的离子通过其晶格的运动，对于加速下一代电池材料的设计至关重要，下一代电池材料可以基于Na等更大离子的传输来运行。

项目成果

Transition Metal Migration Can Facilitate Ionic Diffusion in Defect Garnet-Based Intercalation Electrodes

• DOI: 10.1021/acsenergylett.0c00376
• 发表时间: 2020-04
• 期刊: ACS Energy Letters
• 影响因子: 22
• 作者: Nicholas H. Bashian;S. Abdel-Latif;M. Zuba;Kent J. Griffith;A. Ganose;Joseph W. Stiles;Shiliang Zhou;D. Scanlon;L. Piper;B. Melot

Impact of Structural Deformations on the Performance of Li-Ion Insertion Hosts

• DOI: 10.1021/acs.chemmater.2c00331
• 发表时间: 2022-06-14
• 期刊: CHEMISTRY OF MATERIALS
• 影响因子: 8.6
• 作者: Andrews, Jessica L.;Brady, Michael J.;Melot, Brent C.
• 通讯作者: Melot, Brent C.

Reversible Intercalation of Li Ions in an Earth-Abundant Phyllosilicate Clay

地球上储量丰富的页硅酸盐粘土中锂离子的可逆嵌入

• DOI: 10.1021/acs.inorgchem.1c03834
• 发表时间: 2022
• 期刊: Inorganic Chemistry
• 影响因子: 4.6
• 作者: Stiles, Joseph W.;McClure, Eric T.;Bashian, Nicholas H.;Tappan, Bryce A.;Melot, Brent C.
• 通讯作者: Melot, Brent C.