Collaborative Research: GOALI: Identifying the roles of atomically dispersed Rh, support interactions, and environmental conditions in automotive NO reduction catalysis

多相催化在保持环境清洁方面起着至关重要的作用。例如，汽车上的催化转换器通过将废气成分转化为危害较小的气体，大大减少了运输部门对环境的影响。自20世纪70年代以来，在洛杉矶盆地等地，空气质量的显著改善凸显了多相催化对日常生活的巨大影响。了解催化剂的原子结构和功能之间的关系是开发更有效的催化过程和设计新的催化材料的关键。期望在本研究项目中获得的见解将为指导设计更有效的催化剂提供必要的信息，从而提高催化转化器的性能和效率。为了推广该研究项目提供的独特教育机会，加州大学圣巴巴拉分校和佛罗里达大学的研究生将在每年夏天访问福特汽车公司位于密歇根州迪尔伯恩的研究与创新中心三个月，以访问学者的身份继续研究。本科生将参与研究项目，并通过课堂模块学习主题。三元催化剂是催化转化器的主要组成部分，实现同时氧化和减少污染物到更少有害的物种。在三元催化剂活性位点上的典型金属是铂（Pt）、钯（Pd）和铑（Rh）。虽然Pt和Pd通常促进氧化反应，但Rh在商业催化剂中起着至关重要的作用，因为它能够将一氧化二氮（NO）还原为二氮（N2）。尽管具有重要的商业意义，但在相关的汽车工作条件下，NO在Rh活性位点上的还原机制仍然难以捉摸。在这个项目中，学术研究人员将与一个工业合作伙伴对接，以获得原子分散的Rh物种在商业三元催化剂中的作用的关键机制见解。本文将对原子分散的Rh和Rh团簇在实际条件下的NO还原化学性能和机理进行严格的比较，作为环境条件和支持成分的函数。研究方法将结合动力学研究、原位红外和x射线吸收光谱以及密度泛函理论计算。本研究结果将有助于指导三元催化剂和催化转化器控制系统的设计，以提高其性能。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

Heterogeneous catalysis plays a vital role in keeping the environment clean. For example, catalytic converters in automobiles significantly reduce the environmental impact of the transportation sector by converting exhaust components to less harmful gases. Dramatic improvements in air quality since the 1970s in locations such as the Los Angeles basin underscore the enormous impact of heterogeneous catalysis on everyday life. Critical to the development of more efficient catalytic processes and the design of new catalytic materials is understanding the relationship between a catalyst's atomic structure and its function. It is expected that insights obtained during this research project will provide necessary information to guide the design of more effective catalysts, thereby enabling improvements in the performance and efficiency of catalytic converters. To promote unique educational opportunities provided by this research project, graduate students from the University of California-Santa Barbara and the University of Florida will visit Ford Motor Company's Research and Innovation Center in Dearborn, MI for three months each summer to continue research as visiting scholars. Undergraduate students will be involved in the research project and will learn from the topic through in-class modules. Three-way catalysts are the workhorse components of catalytic converters that achieve simultaneous oxidation and reduction of pollutants to less harmful species. Typical metals at the active sites of three-way catalysts are Platinum (Pt), Palladium (Pd) and Rhodium (Rh). While Pt and Pd typically promote oxidation reactions, Rh plays a crucial role in commercial catalysts because of its ability to reduce nitrous oxide (NO) to dinitrogen (N2). Despite its commercial importance, the mechanism of NO reduction on Rh active sites has remained largely elusive under relevant automotive working conditions. In this project, academic researchers will interface with an industrial partner to gain crucial mechanistic insights into the role of atomically dispersed Rh species in commercial three-way catalysts. Rigorous comparisons of the performance and mechanism of NO reduction chemistry under realistic conditions on atomically dispersed Rh and Rh clusters, as a function of environmental conditions and support composition, will be made. The research approach will combine kinetic studies, in-situ infrared and X-ray absorption spectroscopy, and density functional theory calculations. Results of this study will help guide the design of three-way catalysts and catalytic converter control systems for improved performance.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.