CAREER: Rational Design of Defect-Ordered Architectures in Oxygen-Deficient Perovskites to Control the Oxygen-Evolution Activity

可用于能源相关工艺和设备的新材料的发现对全球能源格局、繁荣和福利的未来产生重大影响。例如，需要具有特定性能的新材料来更好地促进水分解成其基本成分，这对于从可再生资源中产生氢气和氧气非常重要。一个同样重要的性质是某些固体材料中的电荷传导，这是许多能源设备（如电池和燃料电池）必不可少的现象。研究这些属性的基本方面是这个职业奖的中心。该奖项由材料研究部的固态和材料化学计划，刺激竞争性研究的既定计划（EPSCoR）和化学部的化学催化计划共同支持。根据该奖项，Ramezanipour教授的研究小组制定了功能材料合理设计的指导方针，通过改变化合物中原子的排列来控制和修改重要的能量相关特性。该项目推进了对功能材料的基本理解，并发现了有助于能源相关应用领域科学和技术进步的新型化合物。此外，作为该奖项的一部分，教育计划帮助学生提高他们的实验室技能，促进他们的学术成功，并为他们在需要实验室专业知识的领域的潜在职业做好准备。此外，为代表性不足的少数民族学生开展的外联活动向这些学生介绍了基础研究，提高了科学素养，激发了他们对化学的兴趣。这些推广活动，以及让女学生参与实践研究的实习计划，扩大了该项目的影响，并有助于增加STEM领域的多样性。有了这个职业奖，由材料研究部的固态和材料化学计划，刺激竞争力研究的既定计划（EPSCoR）和化学部的化学催化计划共同支持，研究人员致力于揭示允许合理设计和合成缺陷的基本参数，有序结构和缺陷排列对功能性质的影响，特别是电荷传输和氧释放活性。具体的重点是设计和合成的缺陷有序的缺氧钙钛矿，最近已经显示出突出的电催化活性的析氧反应（OER）的水裂解。到目前为止，控制其OER活性的基本结构-性质关系在很大程度上仍未被探索。这类材料的关键特征是存在由于缺氧而产生的缺陷。缺陷的不同排列导致不同类型的有序结构。在这里，Ramezanipour教授和他的团队研究了如何控制缺陷的排列和排序，并探索了缺陷排列在指导缺氧钙钛矿的OER活性中的作用。此外，他们还研究了缺陷排列和电荷传输之间的关系，这是影响OER活性的另一个属性。总的来说，多方面和全面的方法涉及材料的设计，合成和结构顺序，价态，电子结构，电荷传输的变化，以及这些参数对OER属性的影响的研究。该奖项反映了NSF的法定使命，并已被认为是值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估的支持。

NON-TECHNICAL SUMMARY:Discovery of new materials that can be used in energy-related processes and devices has a major impact on the future of global energy landscape, prosperity and welfare. For example, new materials with specific properties are needed to better facilitate splitting of water into its basic components, which is important for the generation of hydrogen and oxygen from renewable sources. A similarly important property is the conduction of charges in certain solid materials, a phenomenon that is essential to many energy devices such as batteries and fuel cells. Studying fundamental aspects of these properties is at the center of this CAREER award. The award is jointly supported by the Solid State and Materials Chemistry program in the Division of Materials Research, the Established Program to Stimulate Competitive Research (EPSCoR), and the Chemical Catalysis Program in the Division of Chemistry. Under this award the research group of Prof. Ramezanipour develops guidelines for rational design of functional materials, where important energy-related properties are controlled and modified by changing the arrangements of atoms within the compounds. This project advances fundamental understanding of functional materials and results in discovery of novel compounds that contribute to the progress of science and technology in the field of energy-related applications. In addition, as part of this award an educational plan helps students to enhance their laboratory skills, facilitates their academic success, and prepares them for potential careers in areas that require expertise in a laboratory setting. Furthermore, outreach activities for underrepresented minority students introduce these students to basic research, increase the scientific literacy, and spark interest in chemistry. These outreach activities, and an internship program for female students to participate in hands-on research, broaden the impact of the project and help increase diversity in STEM fields.TECHNICAL SUMMARY:With this CAREER award, jointly supported by the Solid State and Materials Chemistry program in the Division of Materials Research, the Established Program to Stimulate Competitive Research (EPSCoR), and the Chemical Catalysis Program in the Division of Chemistry, researchers work to uncover the fundamental parameters that allow for rational design and synthesis of defect-ordered architectures and the impact of defect-arrangement on functional properties, in particular the charge-transport and oxygen-evolution activity. The specific focus is on design and synthesis of defect-ordered oxygen-deficient perovskites, which have recently shown outstanding electrocatalytic activity for oxygen-evolution reaction (OER) of water splitting. Until now the fundamental structure-property relationships that control their OER activity have remained largely unexplored. The key characteristic of this class of materials is the presence of defects, created due to oxygen-deficiency. Various arrangements of defects lead to different types of ordered structures. Here Prof. Ramezanipour and his group investigate how the arrangement and ordering of defects can be controlled and explore the role of defect-arrangement in directing the OER activity of oxygen-deficient perovskites. In addition, they investigate the relationship between defect-arrangement and charge-transport, which is another property that affects the OER activity. Overall, the multifaceted and comprehensive approach involves material design, synthesis and study of the changes in structural order, valence-state, electronic structure, charge-transport, and the impact these parameters have on OER properties.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.