Cold-Start NO_x Mitigation by Passive Adsorption Using Pd-Exchanged Zeolites: From Material Design to Mechanism Understanding and System Integration

It remains a major challenge to abate efficiently the harmful nitrogen oxides (NO_x) in low-temperature diesel exhausts emitted during the cold-start period of engine operation. Passive NO_x adsorbers (PNA), which could temporarily capture NO_x at low temperatures (below 200 °C) and release the stored NO_x at higher temperatures (normally 250-450 °C) to downstream selective catalytic reduction unit for complete abatement, hold promise to mitigate cold-start NO_x emissions. In this review, recent advances in material design, mechanism understanding, and system integration are summarized for PNA based on palladium-exchanged zeolites. First, we discuss the choices of parent zeolite, Pd precursor, and synthetic method for the synthesis of Pd-zeolites with atomic Pd dispersions, and review the effect of hydrothermal aging on the properties and PNA performance of Pd-zeolites. Then, we show how different experimental and theoretical methodologies can be integrated to gain mechanistic insights into the nature of Pd active sites, the NO_x storage/release chemistry, as well as the interactions between Pd and typical components/poisons in engine exhausts. This review also gathers several novel designs of PNA integration into modern exhaust after-treatment systems for practical application. At the end, we discuss the major challenges, as well as important implications, for the further development and real application of Pd-zeolite-based PNA in cold-start NO_x mitigation.