Simultaneous removal of NOx and Hg0 from simulated flue gas over CuaCebZrcO3/r-Al2O3 catalysts at low temperatures: performance, characterization, and mechanism.

Abstract

To optimize the simultaneous removal of NOx and Hg0, a series of CuaCebZrcO3/γ-Al2O3 catalysts prepared by the impregnation method were explored and their physical and chemical properties were analyzed by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) analysis, X-ray photoelectron spectroscopy (XPS), NH3-temperature-programmed desorption (NH3-TPD), H2-temperature-programmed reduction (H2-TPR), in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFT), and Fourier transform infrared spectroscopy (FT-IR). The results showed that 15% Cu1.4Ce0.55Zr0.25O3/γ-Al2O3 resulted in the highest conversion efficiency for the simultaneous removal of NOx (93%) and Hg0 (85%) at low temperatures (200 to 300°C). Meanwhile, 15% Cu1.4Ce0.55Zr0.25O3/γ-Al2O3 showed good stability and resistance to SO2 and H2O, which is due to its low crystallinity, good textural performance, and strong redox ability. According to the TPD, TPR, and XPS results, the strong acidic character of 15% Cu1.4Ce0.55Zr0.25O3/γ-Al2O3 promoted the removal of NOx and Hg0. The synergistic effect between CuO and CeO2 in 15% Cu1.4Ce0.55Zr0.25O3/γ-Al2O3 can increase the mobility of chemically adsorbed oxygen and activates lattice oxygen, leading to an excellent performance. The DRIFT results showed that NH3, NH4+, nitrate, and nitrite participated in the selective catalytic reduction (SCR) reaction. On the basis of our experimental results, Hg0 and NOx removal mechanisms were proposed as Hg (ad) + O* → HgO (ad) and 2NH3/NH4+ (ad) + NO2/NO3- (ad) + NO→2N2 + 3H2O/2H+, respectively.