RUI: Using graph theory measures to probe oxygen vacancy and proton conduction in perovskites and double perovskites

RUI：利用图论方法探测钙钛矿和双钙钛矿中的氧空位和质子传导

• 批准号: 1709975
• 负责人: Maria Gomez
• 金额: $ 20.13万
• 依托单位: Mount Holyoke College
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-07-15 至 2021-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1709975&HistoricalAwards=false
• 关键词: RUI; Using; graph; theory; measures

NONTECHNICAL SUMMARYThe Division of Materials Research and the Chemistry Division contribute funds to this award, which supports theoretical research and education on the conduction properties of materials used in fuel- and solar cells. Limitations in the supply of fossil fuels, environmental considerations, and the relative inefficiency of burning fuel to produce electricity have sparked considerable efforts in developing alternative sources of energy. Combustion is inherently inefficient due to the number of energy transfer steps. Fuel cells avoid the entire combustion process by directly converting chemical energy into electricity, significantly increasing efficiency. Solar cells directly convert light energy into electrical energy and, while not as efficient as fuel cells, they make use of a renewable resource. Both processes emit significantly fewer pollutants than combustion and reduce dependence on petroleum products. A solid oxide fuel cell is comprised of two electron-conductive surfaces (electrodes) sandwiching a conductor (electrolyte) of ions. Electricity production is substantially determined by how fast the ions move through the electrolyte. In solar cells, electricity production is limited by missing oxygen atoms in the material, which comprise mobile atom-lattice defects. Overall, understanding ion or ion-defect motion through a material is important for optimizing the performance of these devices. This project will clarify how changes in structure near an ion or vacancy influence conduction pathways. Simulations of specific materials as well as the simulation methods developed in this project will be useful in furthering our knowledge and understanding of conduction, and help engineer more efficient conductors for use in fuel- and solar cells. This project will include training undergraduate women at Mount Holyoke College in computational chemistry, programming, and the associated mathematics. These undergraduates will attend the annual MERCURY conference organized for undergraduates doing research in computational chemistry by the MERCURY consortium, of which the PI is one of the founding members. An extension to the PI's Passport to Chemistry Adventure outreach program targeting high-school students will be developed and sent to the eleven western Massachusetts libraries participating in the program. TECHNICAL SUMMARYThe Division of Materials Research and the Chemistry Division contribute funds to this award, which supports computational research and education on oxygen-vacancy and proton conduction in perovskites and double perovskites. Charged-defect conduction is essential to the functioning of many devices. For example, protons and oxygen vacancies are sometimes the main conductors in fuel-cell membranes; oxygen-vacancy transport is essential for oxygen reduction at the cathode of a fuel cell. Furthermore, band gaps in solar cells are sometimes tuned by oxygen-vacancy concentration. The project will further computational investigations to understand how charged-defect conduction paths in perovskite and double-perovskite materials change with lattice restructuring near the defect, as well as with charge-defect correlation during the conduction process. The project will extend the uses of the PI's defect conduction path finding methods and centrality measures based on time. Centrality measures will be used to not only predict traps, key nexuses, and pathways, but to also predict correlated motion including proton/proton correlation and proton/oxygen-vacancy correlation in acceptor-doped barium zirconate. Complementary techniques such as accelerated dynamics techniques on an empirical potential will be used to determine how well graph-theory-based methods work.This project will include training undergraduate women at Mount Holyoke College in computational chemistry, programming, and the associated mathematics. These undergraduates will attend the annual MERCURY conference organized for undergraduates doing research in computational chemistry by the MERCURY consortium, of which the PI is one of the founding members. An extension to the PI's Passport to Chemistry Adventure outreach program targeting high-school students will be developed and sent to the eleven western Massachusetts libraries participating in the program.

非技术性总结材料研究部和化学部为该奖项提供资金，该奖项支持燃料和太阳能电池中使用的材料的导电性能的理论研究和教育。化石燃料供应的限制、环境考虑以及燃烧燃料以产生电力的相对低效率已经引发了在开发替代能源方面的相当大的努力。由于能量传递步骤的数量，燃烧本质上是低效的。燃料电池通过直接将化学能转化为电能，避免了整个燃烧过程，大大提高了效率。太阳能电池直接将光能转化为电能，虽然效率不如燃料电池，但它们利用了可再生资源。 这两个过程排放的污染物都比燃烧少得多，并减少了对石油产品的依赖。固体氧化物燃料电池由两个电子导电表面（电极）组成，其中包含离子导体（电解质）。电的产生基本上取决于离子在电解质中移动的速度。在太阳能电池中，电力生产受到材料中缺失氧原子的限制，这包括移动的原子晶格缺陷。 总的来说，了解离子或离子缺陷在材料中的运动对于优化这些器件的性能非常重要。这个项目将阐明离子或空位附近的结构变化如何影响传导途径。特定材料的模拟以及本项目中开发的模拟方法将有助于加深我们对传导的了解和理解，并帮助设计用于燃料和太阳能电池的更有效的导体。该项目将包括培训霍利奥克山学院的女本科生学习计算化学、编程和相关数学。这些本科生将参加由MERCURY财团为本科生组织的年度MERCURY会议，MERCURY财团是PI的创始成员之一。PI的护照化学冒险推广计划的目标是高中学生的扩展将被开发和发送到11个西部马萨诸塞州图书馆参与该计划。材料研究部和化学部为该奖项提供资金，该奖项支持钙钛矿和双钙钛矿中氧空位和质子传导的计算研究和教育。带电缺陷传导对于许多器件的功能是必不可少的。例如，质子和氧空位有时是燃料电池膜中的主要导体;氧空位传输对于燃料电池阴极的氧还原至关重要。此外，太阳能电池中的带隙有时通过氧空位浓度来调节。该项目将进一步进行计算研究，以了解钙钛矿和双钙钛矿材料中的带电缺陷传导路径如何随着缺陷附近的晶格重构以及传导过程中的电荷-缺陷相关性而变化。该项目将扩展PI的缺陷传导路径查找方法和基于时间的中心性测量的使用。中心性的措施将被用来不仅预测陷阱，关键的关系，和途径，但也预测相关的运动，包括质子/质子相关和质子/氧空位相关的受体掺杂锆酸钡。补充技术，如加速动力学技术的经验潜力将被用来确定如何以及基于图论的方法working.This项目将包括培训本科女生在蒙特霍利奥克学院在计算化学，编程，以及相关的数学。这些本科生将参加由MERCURY财团为本科生组织的年度MERCURY会议，MERCURY财团是PI的创始成员之一。PI的护照化学冒险推广计划的目标是高中学生的扩展将被开发和发送到11个西部马萨诸塞州图书馆参与该计划。

项目成果

Cooperative origin of proton pair diffusivity in yttrium substituted barium zirconate

钇取代的锆酸钡中质子对扩散率的合作起源（开放获取）

• DOI: 10.1038/s42005-020-00464-5
• 发表时间: 2020-11-04
• 期刊: COMMUNICATIONS PHYSICS
• 影响因子: 5.5
• 作者: Du, Peng;Chen, Qianli;Braun, Artur
• 通讯作者: Braun, Artur

Low‐energy Sr 2 MSbO5.5 (M = Ca and Sr) structures show significant distortions near oxygen vacancies

低能 Sr 2 MSbO5.5（M = Ca 和 Sr）结构在氧空位附近表现出明显的扭曲

• DOI: 10.1002/qua.26356
• 发表时间: 2020
• 期刊: International Journal of Quantum Chemistry
• 影响因子: 2.2
• 作者: Patel, Megha;Zhong, Jiayun;Gomez‐Haibach, Konrad S.;Gomez, Maria A.;King, Graham
• 通讯作者: King, Graham

Graph analysis of proton conduction pathways in scandium-doped barium zirconate

• DOI: 10.1063/5.0039103
• 发表时间: 2021-02-21
• 期刊: JOURNAL OF CHEMICAL PHYSICS
• 影响因子: 4.4
• 作者: Gomez, Maria A.;Brooks-Randall, Sophia;Khan, Samira
• 通讯作者: Khan, Samira

Oxygen Vacancies Altering the Trapping in the Proton Conduction Landscape of Doped Barium Zirconate

• DOI: 10.1021/acs.jpcc.0c09461
• 发表时间: 2020-12-24
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY C
• 影响因子: 3.7
• 作者: Lin, Ziqing;Lin, Shiyun;Gomez, Maria A.
• 通讯作者: Gomez, Maria A.