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

合作研究：GOALI：确定原子分散的 Rh、支持相互作用和环境条件在汽车 NO 还原催化中的作用

• 批准号: 1803165
• 负责人: David Hibbitts
• 金额: $ 22.54万
• 依托单位: University of Florida
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2018
• 资助国家: 美国
• 起止时间: 2018-09-15 至 2022-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1803165&HistoricalAwards=false
• 关键词: Collaborative; Research; GOALI; Identifying; roles

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.

多相催化在保持环境清洁方面发挥着至关重要的作用。例如，汽车中的催化转化器通过将废气成分转化为危害较小的气体，显着减少了运输行业对环境的影响。自 20 世纪 70 年代以来，洛杉矶盆地等地空气质量的显着改善凸显了多相催化对日常生活的巨大影响。开发更有效的催化过程和设计新催化材料的关键是了解催化剂的原子结构与其功能之间的关系。预计该研究项目中获得的见解将为指导更有效的催化剂的设计提供必要的信息，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，加州大学圣塔芭芭拉分校和佛罗里达大学的研究生将每年夏天前往福特汽车公司位于密歇根州迪尔伯恩的研究与创新中心进行为期三个月的访问，以访问学者的身份继续进行研究。本科生将参与研究项目，并通过课堂模块学习该主题。三效催化剂是催化转化器的主要部件，可实现同时氧化和将污染物还原为危害较小的物质。 三元催化剂活性位点的典型金属是铂 (Pt)、钯 (Pd) 和铑 (Rh)。虽然 Pt 和 Pd 通常会促进氧化反应，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)。 尽管具有商业重要性，但在相关的汽车工作条件下，Rh 活性位点上 NO 还原的机制在很大程度上仍然难以捉摸。在该项目中，学术研究人员将与工业合作伙伴合作，以获得关于原子分散的 Rh 物种在商业三效催化剂中的作用的重要机制见解。将对原子分散的 Rh 和 Rh 簇的实际条件下 NO 还原化学的性能和机制进行严格的比较，作为环境条件和载体组成的函数。该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。这项研究的结果将有助于指导三效催化剂和催化转化器控制系统的设计，以提高性能。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力优点和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Theoretical and Experimental Characterization of Adsorbed CO and NO on γ-Al 2 O 3 -Supported Rh Nanoparticles

γ-Al 2 O 3 负载的 Rh 纳米粒子吸附 CO 和 NO 的理论和实验表征

• DOI: 10.1021/acs.jpcc.1c05160
• 发表时间: 2021
• 期刊: The Journal of Physical Chemistry C
• 作者: Hoffman, Alexander J.;Asokan, Chithra;Gadinas, Nicholas;Kravchenko, Pavlo;Getsoian, Andrew “Bean”;Christopher, Phillip;Hibbitts, David
• 通讯作者: Hibbitts, David