Applied Catalysis B: Environmental, Vol.232, 37-48, 2018
Promotional removal of HCHO from simulated flue gas over Mn-Fe oxides modified activated coke
A series of MnxFey/AC catalysts synthesized by impregnation method were investigated on the efficient and stable removal of HCHO in the fix-bed reactor. Extensive characterizations, BET, SEM, XRD, H-2-TPR, XPS and FT-IR, were conducted to study the physicochemical properties, HCHO oxidation and surface reaction of catalysts. The optimal Mn0.75Fe6.02/AC showed enhanced HCHO removal efficiency of 98.30%, as well as excellent performance for simultaneous removal of HCHO (89.96%) and Hg-0 (77.51%). NO and SO2 balanced in N-2 would inhibit the removal of HCHO, while the addition of 6% O-2 weakened the negative effect of SO2 and NO + 6% O-2 facilitated the removal of HCHO. Besides, the slight promotion effect of water vapor was contributed to the regeneration of consumed -OH via the activation of surface oxygen by adsorbed H2O. Characterization results indicated that Mn0.75Fe6.02/AC possessed larger BET surface area, well-developed porosity and better dispersion of active components. Mn0.75Fe6.02/AC exhibited higher reducibility due to the synergistic effect between MnOx and FeOx and the interaction between Mn-Fe oxides and AC support. At the same time, the oxygen-containing functional groups (C-O-, COO), abundant active surface oxygen and -OH facilitated both adsorption and oxidation of HCHO. Besides, the formate and carbonate intermediates formed on the surface of Mn0.75Fe6.02/AC in HCHO removal process, which could be further oxidized into CO2 and H2O. On the basis of above investigations, the mechanism of enhanced HCHO catalytic removal over MnxFey/AC was proposed.