Abstract
Gaseous elemental mercury (Hg0) from industrial flue gas is difficult to be synergistically removed by existing flue gas purification equipment. In this paper, Mn-based oxides were used for the modification of SAPO-34 molecular sieve to enhance Hg0 oxidation and adsorption performances. The results showed that when 5 % Mn dropped on the surface of SAPO-34, it had the highest Hg0 removal efficiency and exhibited a better Hg0 removal performance at lower temperature (<150 °C). SO2 would compete for active adsorption sites of Hg0, while H2O vapor had little influence on Hg0 removal. The Hg0 removal mechanism was discussed based on experiment and characterization results and density functional theory calculation. The larger surface area and pore volume of Mn/SAPO-34 benefited the physical adsorption process. The surface MnOx particles enhanced the oxidation of Hg0 to Hg2+ and the oxygen site can further bond with Hg2+ to form stable HgO. In addition, the larger desorption peak of HgO (487 °C) and the more negative adsorption energy (-1.21 eV) revealed the dominant role of chemical adsorption of Hg0 over Mn/SAPO-34. Thus, the Mn/SAPO-34 is a potential catalyst for Hg0 removal from industrial flue gas.
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