Experimental and density functional theory studies on Cu/Ba-coimpregnated γ-Al2O3 for low-temperature NOx storage and adsorbent regeneration

Abstract

Although the lean-NOx trap (LNT) has been used to reduce NOx emissions from diesel-powered vehicles, LNT application is limited because its performance degrades at low temperatures (e.g., during cold starting). Therefore, to enhance low-temperature NOx storage and adsorbent regeneration, γ-Al2O3 was coimpregnated with both Cu and Ba (Cu–Ba/γ-Al2O3). The experimentally measured NOx storage capacities (NSCs) and NOx storage efficiencies (NSEs) were compared. Density-functional-theory (DFT) calculations were performed to reveal the NOx storage mechanism. The Cu/Ba-coimpregnated γ-Al2O3 improved both NSC and NSE of NO storage and enhanced NSE of NO2 storage at initial stage. In addition, it desorbed NOx at lower temperatures than the conventional Ba-impregnated γ-Al2O3 (Ba/γ-Al2O3). The in-situ diffuse reflectance infrared Fourier-transform spectroscopy analysis and DFT calculations for NO storage showed that NO adsorption was superior on the Cu-compound surfaces and that stable hyponitrite was stored on the Ba-compound surfaces. In NO2 storage, Cu/Ba coimpregnation offered high preferential NO2 coverage on the CuO surface and produced the most stable ionic nitrate on the Ba-compound surfaces. The experimental and theoretical results confirmed that the Cu/Ba-coimpregnated adsorbent exhibited both superior NOx storage and adsorbent regeneration compared to the conventional Ba-containing LNT adsorbent.