Structure, Reactivity and Transport at Surfaces and Interfaces of Doped Ceria Electrolytes and Cermets: An In Situ Atomic Resolution Investigation

掺杂二氧化铈电解质和金属陶瓷表面和界面的结构、反应性和传输：原位原子分辨率研究

• 批准号: 1308085
• 负责人: Peter Crozier
• 金额: $ 52万
• 依托单位: Arizona State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-01 至 2019-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1308085&HistoricalAwards=false
• 关键词: Structure; Reactivity; Transport; Surfaces; Interfaces

NON-TECHNICAL DESCRIPTION: Developing efficient methods for generating electricity is a critical goal as society moves towards sustainable energy. Solid oxide fuel cells are a promising approach for efficiently converting the energy stored in chemical fuels directly to electricity. These ceramic cells run at high temperatures and can utilize a wide range of fuels such as natural gas, biofuels and gasoline. This fuel flexibility is a significant advantage of solid oxide fuel cells compared to other fuel cell technologies. Unfortunately, these devices are expensive and do not show long term stability because of their high operating temperatures. Many of these issues may be solved by developing new materials that would allow reliable operation of the solid oxide fuel cell at lower temperatures. Development of novel materials requires information on the behavior of materials under the harsh conditions present in a fuel cell. This project utilizes a powerful technique, electron microscopy which enables direct observation of atomic level changes taking place in materials under conditions similar to those present in a real fuel cell. This information provides a fundamental understanding of how the structural re-arrangements result in positive or negative materials functionalities. In turn, this information is being used to help in the design of new materials for improved fuel cell performance. Graduate, undergraduate and high school students are involved in this research. These research activities help them to understand how materials research can be employed to address important societal problems like the development of sustainable energy technologies.TECHNICAL DETAILS: Ionic transport properties and chemical reactivity are key factors impacting solid oxide fuel cell technologies. Cost and long-term stability problems associated with high temperature operation are unresolved materials design challenges. These issues have motivated the development of so-called intermediate temperature solid oxide fuel cells which employ novel materials that can deliver high ionic conductivity and catalytic activity at lower temperatures (500 - 700 C). Doped cerias are nonstoichiometric rare earth oxides which show high ionic conductivity and desirable catalytic properties making them potential candidates for use in intermediate temperature applications. However, there are important unresolved scientific questions related to interactions across grain boundaries in electrolytes as well as ceramic-metal and solid-gas interfaces in anodes. This project addresses these questions by using in situ aberration corrected electron microscopy along with monochromated electron energy-loss spectroscopy to develop a fundamental atomic level understanding of these interfacial processes. The nanoscale structures and chemistries affecting ionic conductivity and the reactivity in electrolytes and anode cermets are being determined. A new experimental approach is being developed to allow in situ atomic resolution observations of electroceramics under electrochemical conditions. This research is potentially transformative because it is providing new information on the dynamic processes relating structure and chemistry with electrochemical and electroceramic functionalities. This research project is training graduate and undergraduate students to learn about and contribute to the developments in energy-related oxide materials.

非技术描述：随着社会向可持续能源发展，开发有效的发电方法是一个关键目标。固体氧化物燃料电池是一种很有前途的方法，可以有效地将储存在化学燃料中的能量直接转化为电能。这些陶瓷电池在高温下运行，可以使用多种燃料，如天然气、生物燃料和汽油。与其他燃料电池技术相比，这种燃料灵活性是固体氧化物燃料电池的显著优势。不幸的是，这些设备价格昂贵，并且由于其高工作温度而不表现出长期稳定性。许多这些问题可以通过开发新的材料来解决，这些材料可以使固体氧化物燃料电池在较低的温度下可靠地运行。新材料的开发需要有关材料在燃料电池中存在的恶劣条件下的行为的信息。这个项目利用了一种强大的技术——电子显微镜，它可以直接观察材料在类似于真实燃料电池的条件下发生的原子水平变化。这些信息提供了对结构重新排列如何导致积极或消极材料功能的基本理解。反过来，这些信息被用来帮助设计新材料，以提高燃料电池的性能。研究对象包括研究生、本科生和高中生。这些研究活动帮助他们了解如何利用材料研究来解决重要的社会问题，如可持续能源技术的发展。技术细节：离子传输特性和化学反应性是影响固体氧化物燃料电池技术的关键因素。与高温操作相关的成本和长期稳定性问题是尚未解决的材料设计挑战。这些问题推动了所谓的中温固体氧化物燃料电池的发展，这种电池采用了新型材料，可以在较低温度（500 - 700℃）下提供高离子电导率和催化活性。掺杂铈是一种非化学计量稀土氧化物，具有高离子电导率和理想的催化性能，使其成为中温应用的潜在候选者。然而，关于电解质中跨晶界的相互作用以及阳极中的陶瓷-金属和固体-气体界面，还有一些重要的未解决的科学问题。该项目通过使用原位像差校正电子显微镜以及单色电子能量损失光谱来解决这些问题，以发展对这些界面过程的基本原子水平的理解。纳米级结构和化学影响离子电导率和反应性的电解质和阳极陶瓷被确定。一种新的实验方法正在开发，允许在电化学条件下的电陶瓷的原位原子分辨率观察。这项研究具有潜在的变革性，因为它提供了与电化学和电陶瓷功能相关的结构和化学动态过程的新信息。该研究项目旨在培养研究生和本科生了解能源相关氧化物材料的发展并为之做出贡献。

项目成果

Atomic Level Strain Induced by Static and 1 Dynamic Oxygen Vacancies on Reducible Oxide Surfaces

可还原氧化物表面上静态和动态氧空位引起的原子级应变

• 发表时间: 2023
• 期刊: arXivorg
• 作者: Piyush Haluai, Tara M.

Atomic Scale Characterization of Fluxional Cation Behavior on Nanoparticle Surfaces: Probing Oxygen Vacancy Creation/Annihilation at Surface Sites

• DOI: 10.1021/acsnano.0c07584
• 发表时间: 2021-01-28
• 期刊: ACS NANO
• 影响因子: 17.1
• 作者: Lawrence, Ethan L.;Levin, Barnaby D. A.;Crozier, Peter A.
• 通讯作者: Crozier, Peter A.

Tracking the picoscale spatial motion of atomic columns during dynamic structural change

• DOI: 10.1016/j.ultramic.2020.112978
• 发表时间: 2020-06-01
• 期刊: ULTRAMICROSCOPY
• 影响因子: 2.2
• 作者: Levin, Barnaby D. A.;Lawrence, Ethan L.;Crozier, Peter A.
• 通讯作者: Crozier, Peter A.

Quantifying Structural Transformations from Redox Reactions in TiO 2

量化 TiO 2 中氧化还原反应的结构转变

• DOI: 10.1017/s1431927619008110
• 发表时间: 2019
• 期刊: Microscopy and Microanalysis
• 影响因子: 2.8
• 作者: Shindel, Benjamin;Haluai, Piyush;Liu, Qianlang;Levin, Barnaby D.A.;Boland, Tara;Crozier, Peter A.
• 通讯作者: Crozier, Peter A.

New Data-Driven Interacting-Defect Model Describing Nanoscopic Grain Boundary Compositions in Ceramics

新的数据驱动的相互作用缺陷模型描述陶瓷中的纳米晶界成分

• DOI: 10.1021/acs.jpcc.0c05713
• 发表时间: 2020
• 期刊: The Journal of Physical Chemistry C
• 作者: Tong, Xiaorui;Bowman, William J.;Mejia-Giraldo, Alejandro;Crozier, Peter A.;Mebane, David S.
• 通讯作者: Mebane, David S.