Simultaneous removal of NO_x and Hg⁰ from simulated flue gas over Cu_aCe_bZr_cO₃/r-Al₂O₃ catalysts at low temperatures: performance, characterization, and mechanism

To optimize the simultaneous removal of NO_x and Hg⁰, a series of Cu_aCe_bZr_cO₃/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% Cu_1.4Ce_0.55Zr_0.25O₃/γ-Al₂O₃ resulted in the highest conversion efficiency for the simultaneous removal of NO_x (93%) and Hg⁰ (85%) at low temperatures (200 to 300 °C). Meanwhile, 15% Cu_1.4Ce_0.55Zr_0.25O₃/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% Cu_1.4Ce_0.55Zr_0.25O₃/γ-Al₂O₃ promoted the removal of NO_x and Hg⁰. The synergistic effect between CuO and CeO₂ in 15% Cu_1.4Ce_0.55Zr_0.25O₃/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 NO_x removal mechanisms were proposed as Hg (ad) + O* → HgO (ad) and 2NH₃/NH₄⁺ (ad) + NO₂/NO₃⁻ (ad) + NO→2N₂ + 3H₂O/2H⁺, respectively.