CAREER: Analytical Cryo-Scanning Transmission Electron Microscopy for Understanding Physical and Chemical Processes at Liquid/Solid Interfaces

职业：分析冷冻扫描透射电子显微镜，用于了解液/固界面的物理和化学过程

• 批准号: 1654596
• 负责人: Lena Kourkoutis
• 金额: $ 55万
• 依托单位: Cornell University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-04-01 至 2023-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1654596&HistoricalAwards=false
• 关键词: CAREER; Analytical; Cryo; Scanning; Transmission

Non-technical summary: Interfaces and surfaces play a special role in synthesizing novel materials, enabling chemical reactions, designing electronic devices, and determining the mechanical stability of structural materials. To realize the goal of understanding processes at interfaces between liquids and solids, processes that for example determine how batteries function and how they fail, the objective of this project is to develop and apply novel electron microscopy techniques that allow not only solid/solid, but also liquid/solid and soft/hard interfaces to be studied at the nanometer to atomic scale. This project will have an impact on science and technology by providing high-resolution characterization techniques of materials that are of interest for a wide range of technologies thereby promoting the progress of sciences, materials discovery and applications. The project will also provide stimulating and authentic experiences for freshmen, K-12 students and teachers with the goal of motivating a new generation of scientists. Microscopy will play a central role in these efforts, which include the development of a freshman laboratory module and a microscopy-based science kit for K-12 teachers nationwide. Technical summary: Recent advances in electron microscopy have opened a new era of atomic resolution imaging and spectroscopy inside solids. Liquid/solid interfaces have yet to be imaged at high spatial resolution but play a critical role in a range of biological, chemical and physical processes from catalysis to electrochemical energy storage to the formation of biominerals. Inspired by electron microscopy of biological systems, with this CAREER award, the PI develops new sample preparation techniques that use rapid freezing to stabilize the soft and liquid components of composite systems in a vitreous state enabling structural and spectroscopic studies by cryo-STEM. Materials that are sufficiently thin for direct analysis in the microscope such as nanostructured electrode materials in liquid electrolytes, the crystal structure and defects of the inorganic crystalline components and the surrounding liquid will be simultaneously imaged. For thicker samples, including lithium-metal batteries, cryo-focused ion beam lift-out will be developed to gain access to the internal liquid/solid interfaces. This characterization platform will be used to study the early stages of dendrite formation at lithium-metal/electrolyte interfaces to gain a fundamental understanding of the mechanisms governing their formation and growth. The ability to identify nucleation sites for dendritic growth will shed new light on a central challenge in developing high-energy rechargeable metal batteries.With the goal of creating a broader, more diverse workforce, this project focuses on attracting and recruiting students into the fields of science, technology, engineering and mathematics at an earlier stage. K-12 teacher development is supported through MicroWorld, a microscopy-based module that will be adapted to meet the challenges of the Next Generation Science Standards. This module will benefit teacher workshops for K-12 teachers who work in minority-serving schools and will also be made available to teachers nationwide through the CCMR Lending Library of Experiments. Freshmen will benefit from the development of FLAME, a new Freshman Lab on Advanced Microscopy with Electrons. This project will therefore impact science, technology, engineering and mathematics education, both at the K-12 and the college level.

非技术性总结：界面和表面在合成新材料、实现化学反应、设计电子器件和确定结构材料的机械稳定性方面发挥着特殊作用。为了实现理解液体和固体之间界面的过程的目标，例如确定电池如何工作以及如何失败的过程，该项目的目标是开发和应用新型电子显微镜技术，不仅允许固体/固体，而且允许液体/固体和软/硬界面在纳米到原子尺度上进行研究。该项目将对科学和技术产生影响，提供对各种技术感兴趣的材料的高分辨率表征技术，从而促进科学、材料发现和应用的进步。该项目还将为新生，K-12学生和教师提供刺激和真实的体验，以激励新一代科学家。显微镜将在这些努力中发挥核心作用，其中包括为全国K-12教师开发新生实验室模块和基于显微镜的科学工具包。电子显微镜的最新进展开启了固体内部原子分辨率成像和光谱学的新时代。液/固界面尚未在高空间分辨率下成像，但在从催化到电化学储能到生物矿物形成的一系列生物，化学和物理过程中发挥着关键作用。受到生物系统电子显微镜的启发，凭借这项职业奖，PI开发了新的样品制备技术，该技术使用快速冷冻将复合系统的软质和液体成分稳定在玻璃态，从而通过cryo-STEM进行结构和光谱研究。对于在显微镜中直接分析的足够薄的材料，例如液体电解质中的纳米结构电极材料，无机晶体成分和周围液体的晶体结构和缺陷将同时成像。对于较厚的样品，包括锂金属电池，将开发低温聚焦离子束提离，以进入内部液体/固体界面。该表征平台将用于研究锂-金属/电解质界面处枝晶形成的早期阶段，以从根本上了解其形成和生长的机制。该项目旨在培养更广泛、更多样化的劳动力队伍，旨在吸引和招募科学、技术、工程和数学等领域的学生，并在早期阶段就将这些学生纳入研究领域。K-12教师的发展是通过微观世界，一个基于显微镜的模块，将被调整，以满足下一代科学标准的挑战支持。这一模块将使在少数民族学校工作的K-12教师的教师讲习班受益，并将通过CCMR实验借阅图书馆向全国教师提供。新生将受益于火焰的发展，一个新的新生实验室先进的电子显微镜。因此，该项目将影响K-12和大学一级的科学，技术，工程和数学教育。

项目成果

Probing the Native Structure and Chemistry of Dendrites and SEI Layers in Li-Metal Batteries by Cryo-FIB Lift-Out and Cryo-STEM

通过 Cryo-FIB Lift-Out 和 Cryo-STEM 探测锂金属电池中枝晶和 SEI 层的天然结构和化学性质

• DOI: 10.1017/s1431927618008073
• 发表时间: 2018
• 期刊: Microscopy and Microanalysis
• 影响因子: 2.8
• 作者: Zachman, Michael J.;Tu, Zhengyuan;Archer, Lynden A.;Kourkoutis, Lena F.
• 通讯作者: Kourkoutis, Lena F.

Nanoscale Elemental Mapping of Intact Solid–Liquid Interfaces and Reactive Materials in Energy Devices Enabled by Cryo-FIB/SEM

通过 Cryo-FIB/SEM 实现能源设备中完整固液界面和反应材料的纳米级元素测绘

• DOI: 10.1021/acsenergylett.0c00202
• 发表时间: 2020
• 期刊: ACS Energy Letters
• 影响因子: 22
• 作者: Zachman, Michael J.;Tu, Zhengyuan;Archer, Lynden A.;Kourkoutis, Lena F.
• 通讯作者: Kourkoutis, Lena F.

Designing Artificial Solid-Electrolyte Interphases for Single-Ion and High-Efficiency Transport in Batteries

• DOI: 10.1016/j.joule.2017.06.002
• 发表时间: 2017-10-11
• 期刊: JOULE
• 影响因子: 39.8
• 作者: Tu, Zhengyuan;Choudhury, Snehashis;Archer, Lynden A.
• 通讯作者: Archer, Lynden A.

Stabilizing polymer electrolytes in high-voltage lithium batteries

• DOI: 10.1038/s41467-019-11015-0
• 发表时间: 2019-07-12
• 期刊: NATURE COMMUNICATIONS
• 影响因子: 16.6
• 作者: Choudhury, Snehashis;Tu, Zhengyuan;Archer, Lynden A.
• 通讯作者: Archer, Lynden A.

Co-precipitation induces changes to iron and carbon chemistry and spatial distribution at the nanometer scale

共沉淀引起纳米尺度铁和碳化学和空间分布的变化

• DOI: 10.1016/j.gca.2021.09.003
• 发表时间: 2021
• 期刊: Geochimica et Cosmochimica Acta
• 影响因子: 5
• 作者: Possinger, Angela R.;Zachman, Michael J.;Dynes, James J.;Regier, Tom Z.;Kourkoutis, Lena F.;Lehmann, Johannes
• 通讯作者: Lehmann, Johannes