A series of nanosized (Fe3-xMnx)1-δO4 (x = 0, 0.2, 0.5, and 0.8) were synthesized for elemental mercury capture from the flue gas. Cation vacancies on (Fe3-xMnx)1-δO4 can provide the active sites for elemental mercury adsorption, and Mn(4+) cations on (Fe3-xMnx)1-δO4 may be the oxidizing agents for elemental mercury oxidization. With the increase of Mn content in the spinel structure, the percents of Mn(4+) cations and cation vacancies on the surface increased. As a result, elemental mercury capture by (Fe3-xMnx)1-δO4 was obviously promoted with the increase of Mn content. (Fe2.2Mn0.8)1-δO4 showed an excellent capacity for elemental mercury capture (>1.5 mg g(-1) at 100-300 °C) in the presence of SO2 and HCl. Furthermore, (Fe2.2Mn0.8)1-δO4 with the saturation magnetization of 45.6 emu g(-1) can be separated from the fly ash using magnetic separation, leaving the fly ash essentially free of sorbent and adsorbed Hg. Therefore, nanosized (Fe2.2Mn0.8)1-δO4 may be a promising sorbent for the control of elemental mercury emission.
In order to facilitate the removal of elemental mercury (Hg(0)) from coal-fired flue gas, catalytic oxidation of Hg(0) with manganese oxides supported on inert alumina (alpha-Al2O3) was investigated at lower temperatures (373-473 K). To improve the catalytic activity and the sulfur-tolerance of the catalysts at lower temperatures, several metal elements were employed as dopants to modify the catalyst of Mn/alpha-Al2O3. The best performance among the tested elements was achieved with molybdenum (Mo) as the dopant in the catalysts. It can work even better than the noble metal catalyst Pd/alpha-Al2O3. Additionally, the Mo doped catalyst displayed excellent sulfur-tolerance performance at lower temperatures, and the catalytic oxidation efficiency for Mo(0.03)-Mn/alpha-Al2O3 was over 95% in the presence of 500 ppm SO2 versus only about 48% for the unmodified catalyst. The apparent catalytic reaction rate constant increased by approximately 5.5 times at 423 K. In addition, the possible mechanisms involved in Hg(0) oxidation and the reaction with the Mo modified catalyst have been discussed.
Catalytic conversion of elemental mercury (Hg(0)) to its oxidized form has been considered as an effective way to enhance mercury removal from coal-fired power plants. In order to make good use of the existing selective catalytic reduction of NO(x) (SCR) catalysts as a cobenefit of Hg(0) conversion at lower level HCl in flue gas, various catalysts supported on titanium dioxide (TiO(2)) and commercial SCR catalysts were investigated at various cases. Among the tested catalysts, ruthenium oxides (RuO(2)) not only showed rather high catalytic activity on Hg(0) oxidation by itself, but also appeared to be well cooperative with the commercial SCR catalyst for Hg(0) conversion. In addition, the modified SCR catalyst with RuO(2) displayed an excellent tolerance to SO(2) and ammonia without any distinct negative effects on NO(x) reduction and SO(2) conversion. The demanded HCl concentration for Hg(0) oxidation can be reduced dramatically, and Hg(0) oxidation efficiency over RuO(2) doped SCR catalyst was over 90% even at about 5 ppm HCl in the simulated gases. Ru modified SCR catalyst shows a promising prospect for the cobenefit of mercury emission control.
A stoichiometric nanosized MnÀFe spinel (Fe 2.2 Mn 0.8 O 4 ) was synthesized using a coprecipitation method. After the thermal treatment at 400 °C under air, chemical heterogeneity deriving from the oxidation kinetic difference between Fe 2+ and Mn 2+ /Mn 3+ was observed in (Fe 2.2 Mn 0.8 ) 1-δ O 4 . XPS and TEM analyses both pointed a Mn enrichment (especially Mn 4+ cation) on the particle's surface. Furthermore, the percent of cation vacancy on the surface increased obviously due to the enrichment of Mn 4+ cation on the surface. As a result, the capacity of (Fe 2.2 Mn 0.8 ) 1-δ O 4 -400 for elemental mercury capture was generally much better than those of MnO x /γ-Fe 2 O 3 , (Fe 2.2 Mn 0.8 ) 1-δ O 4 -200 and Fe 2.2 Mn 0.8 O 4 . Furthermore, the saturation magnetization of (Fe 2.2 Mn 0.8 ) 1-δ O 4 obviously increased after the thermal treatment under air at 400 °C, which made it easier to separate the sorbent and adsorbed mercury from the fly ash for recycling, regeneration, and safe disposal of the adsorbed mercury. Therefore, (Fe 2.2 Mn 0.8 ) 1-δ O 4 -400 may be a promising sorbent for elemental mercury capture.
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