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This study extends research previously reported from our laboratory [SAE 2009-01-0285] on diesel NOx control utilizing a new generation of Lean NOx Trap (LNT) plus in-situ Selective Catalytic Reduction (SCR) catalyst systems. Key findings from this work include 1) evidence for a “non-ammonia” reduction pathway over the SCR catalyst (in addition to the conventional ammonia pathway), 2) high NOx conversions utilizing LNT formulations with substantially lower platinum group metal (PGM) loadings than utilized in earlier systems, 3) ability of the downstream SCR catalyst to maintain high overall system NOx efficiency with aged LNTs, and 4) effectiveness of both Cu- and Fe-zeolite SCR formulations to enhance overall system NOx efficiency. FTP NOx conversion efficiencies in excess of 95% were obtained on two light-duty vehicle platforms with lab-aged catalyst systems, thus showing potential of the LNT+SCR approach for achieving the lowest U.S. emissions standards

Diesel NOx emissions control utilizing combined Lean NOx Trap (LNT) and so-called passive or in-situ Selective Catalytic Reduction (SCR) catalyst technologies (i.e. with reductant species generated by the LNT) has been the subject of several previous papers from our laboratory [ 1 - 2 ]. The present study focuses on hydrocarbon (HC) emissions control via the same LNT+SCR catalyst technology under FTP driving conditions. HC emissions control can be as challenging as NOx control under both current and future federal and California/Green State emission standards. However, as with NOx control, the combined LNT+SCR approach offers advantages for HC emission control over LNT-only aftertreatment. The incremental conversion obtained with the SCR catalyst is shown, both on the basis of vehicle and laboratory tests, to result primarily from HC adsorbed on the SCR catalyst during rich LNT purges that reacts during subsequent lean engine operation.

An alumina-based LNT is being developed through laboratory studies, for diesel vehicle applications. This LNT provides high NOx conversion efficiency at low temperature (150 to 350°C, especially below 200°C), which is very important for the exhaust-gas after-treatment of diesel passenger vehicles. Addition of 2 to 4 wt% of alkaline-earth metal oxide or other metal oxides to the alumina LNT formulation improves NOx reduction activity at the high end of its active temperature window. More significantly, the alumina-based LNT can undergo the de-SOx process (the process of removing sulfur from the catalytic surfaces) very efficiently: within 1 minute at the relatively low temperature of 500 to 650°C under slightly rich conditions (λ = 0.98 to 0.987). Such a mild de-SOx process imposes minimal thermal exposure, causing almost no thermal damage to the LNT, and helps minimize the associated fuel penalty.

Advanced Cu-zeolite based SCR (selective catalytic reduction) catalyst technologies were evaluated in a laboratory reactor as a component of a diesel LNT (lean NOx trap) plus in-situ SCR system (i.e., NH3 generation over the LNT vs injection via urea). New-generation LNT formulations, with lower desulfation temperatures and improved durability characteristics relative to previous LNTs, were also evaluated. The combined new-generation LNT+Cu-zeolite SCR systems showed a much wider temperature window of high NOx conversion compared to either LNT catalysts alone or LNT+SCR systems utilizing Fe-zeolite SCR catalysts. The new-generation Cu-zeolite SCR catalysts retained high activity even after repeated exposure to high-temperature rich DeSOx conditions in a laboratory 3-mode aging cycle simulating 120,000 mile vehicle driving.

The effects of PGM zoning and washcoat staging have been investigated as a means to lower the cost and simultaneously improve the performance of a lean NOx trap system. It is shown that reverse PGM zoning can be used to reduce the cost of the LNT while essentially maintaining the NOx performance of a similarly-sized trap with a uniformly high PGM loading. In addition, the effective temperature window of the trap can be expanded by staging different NOx trap formulations that are optimized for different temperature ranges. Alternatively, LNT washcoat staging can be used to improve the hydrocarbon conversion of the trap while maintaining good NOx performance. Laboratory data and vehicle data are presented for several NOx trap system combinations that demonstrate the improved performance that can be obtained from a combination of reverse PGM zoning and washcoat staging.

Desulfation characteristics of several model and fully-formulated monolithic lean NOx trap materials were studied in a laboratory flow reactor employing a chemical ionization mass spectrometer. For all samples, desulfation at elevated temperatures under reducing conditions resulted in appearance of sulfur dioxide (SO2) followed by carbonyl sulfide (COS) and hydrogen sulfide (H2S). The data appear consistent with a desulfation mechanism involving elimination of SO2 from stored sulfates under reducing conditions, followed by reaction of the SO2 with CO and H2 to produce COS and H2S, respectively. Based on these observations, several cyclic and multistage desulfation strategies were devised which greatly decreased H2S emissions while achieving relatively rapid and complete sulfur removal.