Experimental study on Hg0 removal from flue gas over columnar MnOx-CeO2/activated coke

Abstract

Mn-Ce mixed oxides supported on commercial columnar activated coke (MnCe/AC) were employed to remove elemental mercury (Hg0) at low temperatures (100–250°C) without the assistance of HCl in flue gas. The samples were characterized by X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption (TPD). Effects of some factors, including Mn-Ce loading values, active component, reaction temperatures and flue gas components (O2, SO2, NO, H2O), on Hg0 removal efficiency were investigated. Results indicated that the optimal Mn-Ce loading value and reaction temperature were 6% and 190°C, respectively. Considerable high Hg0 removal efficiency (>90%) can be obtained over MnCe6/AC under both N2/O2 atmosphere and simulated flue gas atmosphere at 190°C. Besides, it was observed that O2 and NO exerted a promotional effect on Hg0 removal, H2O exhibited a suppressive effect, and SO2 hindered Hg0 removal seriously when in the absence of O2. Furthermore, the XPS spectra of Hg 4f and Hg-TPD results showed that the captured mercury were existed as Hg0 and HgO on the MnCe6/AC, and HgO was the major species, which illustrated that adsorption and catalytic oxidation process were included for Hg0 removal over MnCe6/AC, and catalytic oxidation played the critical role. What's more, both lattice oxygen and chemisorbed oxygen or OH groups on MnCe6/AC contributed to Hg0 oxidation. MnCe6/AC, which exhibited excellent performance on Hg0 removal in the absence of HCl, appeared to be promising in industrial application, especially for low-rank coal fired flue gas.