One of the cost-effective mercury control technologies in coal-fired power plants is the enhanced oxidation of elemental mercury in selective catalytic reduction (SCR) followed by the capture of the oxidized mercury in the wet scrubber. To better understand Hg oxidation chemistry within a SCR, the Institute for Combustion Science and Environmental Technology at Western Kentucky University set up a pilot-scale SCR slipstream facility at a selected utility boiler burning bituminous coal. The greatest benefit of this scaled-down SCR slipstream test is the ability to investigate the effects of Hg oxidation in a SCR using actual flue gas with fly ash included and to isolate and control specific flue-gas compositions with spike gas additions. The average sulfur, chlorine, and mercury contents in the burned coal were 1.67% and 731 and 0.13 ppm, respectively. CaO and Fe 2 O 3 and loss on ignition of the fly ash, which are reported to possibly affect Hg speciation, are approximately 1.65, 14.6, and 2.6% on average, respectively. The maximum concentrations of spike gases were 500, 25, 2000, 50, and 15 ppm for HCl, Cl 2 , SO 2 , SO 3 , and HBr, respectively. Semicontinuous mercury emission monitors were used to monitor the variation of mercury speciation at the inlet and outlet of the SCR slipstream reactor, and the American Society for Testing and Materials certified Ontario hydro method was used for data comparison and validation. This paper is the first in a series of two in which the validation of the SCR slipstream test and Hg speciation variation in runs with or without SCR catalysts inside the SCR slipstream reactor under special gas additions (HCl, Cl 2 , SO 2 , and SO 3 ) are presented. Effects of HBr additions on mercury speciation within the SCR will be presented in the second part of the series. Tests indicate that the use of a catalyst in a SCR slipstream reactor can achieve greater than 90% NO reduction efficiency with a NH 3 /NO ratio of about 1. There is no evidence to show that the reactor material affects mercury speciation. Both SCR catalysts used in this study exhibited a catalytic effect on the elemental mercury oxidation but had no apparent adsorption effect. SCR catalyst 2 seemed more sensitive to the operational temperature. The spike gas tests indicated that HCl can promote Hg 0 oxidation but not Cl 2 . The effect of Cl 2 on mercury oxidation may be inhibited by higher concentrations of SO 2 , NO, or H 2 O in real flue-gas atmospheres within the typical SCR temperature range (300-350 °C). SO 2 seemed to inhibit mercury oxidation; however, SO 3 may have some effect on the promotion of mercury oxidation in runs with or without SCR catalysts.
An investigation of speciated mercury transformation with the addition of hydrogen bromide (HBr) at elevated temperatures was conducted in a slipstream reactor with real flue gas atmospheres. A real flue gas atmosphere is composed of bituminous coal (with high sulfur and high chlorine contents) and Powder River Basin (PRB) coal (with lower sulfur and chlorine contents). The average sulfur, chlorine, and mercury contents in the tested bituminous coal were 1.31% and 1328 and 0.11 ppm and 0.61% and 170 and 0.08 ppm, respectively, for tested PRB coal. The average CaO, Fe2O3, and loss on ignition in collected fly ash contents of tested bituminous coal were 1.71, 17.51, and 7.13% and 22.95, 4.91, and 0.64%, respectively, for tested PRB coal. The different contents of coal chlorine, CaO, and Fe2O3 in fly ash can be attributed to the different mercury speciations at baseline tests for these two coals in this study. The addition of HBr concentrations into the flue gas was controlled in the 3−15 ppm range. Semi-continuous mercury emission monitors were used to check the variation of mercury speciation at sampling locations. The Ontario Hydro Method (ASTM D6784-02) was used for data validation or comparison. For both methods, a high temperature inertial sampling probe was used to minimize the interference between vapor phase mercury and fly ash. Its temperatures were controlled consistently with flue gas temperatures at their installation locations in the slipstream reactor. Test results indicated that adding HBr into the flue gas at several parts per million strongly impacted the mercury oxidation and adsorption, which were dependent upon temperature ranges. Higher temperatures (in the range of 300−350 °C) promoted mercury oxidation by HBr addition but did not promote mercury adsorption. Lower temperatures (in a range of 150−200 °C) enhanced mercury adsorption on the fly ash by adding HBr. Test results also verified effects of flue gas atmospheres on the mercury oxidation by the addition of HBr, which included concentrations of chlorine and sulfur in the flue gas. Chlorine species seemed to be involved in the competition with bromine species in the mercury oxidation process. With the addition of HBr at 3 ppm at a temperature of about 330 °C, the additional mercury oxidation could be reached by about 55% in a flue gas atmosphere by burning PRB coal in the flue gas and by about 20% in a flue gas by burning bituminous coal. These are both greater than the maximum gaseous HgBr2 percentage in the flue gas (35% for PRB coal and 5% for bituminous coal) by thermodynamic equilibrium analysis predictions under the same conditions. This disagreement may indicate a greater complexity of mercury oxidation mechanisms by the addition of HBr. It is possible that bromine species promote activated chlorine species generation in the flue gas, where the kinetics of elemental mercury oxidation were enhanced. However, SO2 in the flue gas may involve the consumption of the available activated chlorine species. Thus, the higher mercury oxidation ...
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