Development of Optimal Catalyst Designs and Operating Strategies for Lean NOx Reduction in Coupled LNT-SCR Systems

Oxides of nitrogen in the form of nitric oxide (NO) and nitrogen dioxide (NO2) commonly referred to as NOx, is one of the two chemical precursors that lead to ground-level ozone, a ubiquitous air pollutant in urban areas. A major source of NOx} is generated by equipment and vehicles powered by diesel engines, which have a combustion exhaust that contains NOx in the presence of excess O2. Catalytic abatement measures that are effective for gasoline-fueled engines such as the precious metal containing three-way catalytic converter (TWC) cannot be used to treat O2-laden exhaust containing NOx. Two catalytic technologies that have emerged as effective for NOx abatement are NOx storage and reduction (NSR) and selective catalytic reduction (SCR). NSR is similar to TWC but requires much larger quantities of expensive precious metals and sophisticated periodic switching operation, while SCR requires an on-board source of ammonia which serves as the chemical reductant of the NOx. The fact that NSR produces ammonia as a byproduct while SCR requires ammonia to work has led to interest in combining the two together to avoid the need for the cumbersome ammonia generation system. In this project a comprehensive study was carried out of the fundamental aspects and application feasibility of combined NSR/SCR. The project team, which included university, industry, and national lab researchers, investigated the kinetics and mechanistic features of the underlying chemistry in the lean NOx trap (LNT) wherein NSR was carried out, with particular focus on identifying the operating conditions such as temperature and catalytic properties which lead to the production of ammonia in the LNT. The performance features of SCR on both model and commercial catalysts focused on the synergy between the LNT and SCR converters in terms of utilizing the upstream-generated ammonia and alternative reductants such as propylene, representing the hydrocarbon component of diesel exhaust. First-principle models of the LNT and SCR converters, which utilized the mechanistic-based kinetics and realistic treatments of the flow and transport processes, in combination with bench-scale reactor experiments helped to identify the best designs for combining the NSR and SCR catalysts over a range of operating conditions encountered in practice. This included catalysts having multiple zones and layers and additives with the focus on determining the minimal precious metal component needed to meet emission abatement targets over a wide range of operating conditions. The findings from this study provide diesel vehicle and catalyst companies valuable information to develop more cost effective diesel emissions catalysts which helps to expand the use of more fuel efficient diesel power. The fundamental modeling and experimental tools and findings from this project can be applied to catalyst technologies used in the energy and chemical industries. Finally, the project also led to training of several doctoral students who were placed in research jobs in industry and academia.