Mercury oxidation promoted by a selective catalytic reduction catalyst under simulated Powder River Basin coal combustion conditions.
A bench-scale reactor consisting of a natural gas burner and an electrically heated reactor housing a selective catalytic reduction (SCR) catalyst was constructed for studying elemental mercury (Hg(o)) oxidation under SCR conditions. A low sulfur Powder River Basin (PRB) subbituminous coal combustion fly ash was injected into the entrained-flow reactor along with sulfur dioxide (SO2), nitrogen oxides (NOx), hydrogen chloride (HCl), and trace Hg(o). Concentrations of Hg(o) and total mercury (Hg) upstream and downstream of the SCR catalyst were measured using a Hg monitor. The effects of HCl concentration, SCR operating temperature, catalyst space velocity, and feed rate of PRB fly ash on Hg(o) oxidation were evaluated. It was observed that HCl provides the source of chlorine for Hg(o) oxidation under simulated PRB coal-fired SCR conditions. The decrease in Hg mass balance closure across the catalyst with decreasing HCl concentration suggests that transient Hg capture on the SCR catalyst occurred during the short test exposure periods and that the outlet speciation observed may not be representative of steady-state operation at longer exposure times. Increasing the space velocity and operating temperature of the SCR led to less Hg(o) oxidized. Introduction of PRB coal fly ash resulted in slightly decreased outlet oxidized mercury (Hg2+) as a percentage of total inlet Hg and correspondingly resulted in an incremental increase in Hg capture. The injection of ammonia (NH3) for NOx reduction by SCR was found to have a strong effect to decrease Hg oxidation. The observations suggest that Hg(o) oxidation may occur near the exit region of commercial SCR reactors. Passage of flue gas through SCR systems without NH3 injection, such as during the low-ozone season, may also impact Hg speciation and capture in the flue gas.
Lee
Chun W
CW
U.S. Environmental Protection Agency, Office of Research and Development, National Risk Management Research Laboratory, Research Triangle Park, NC 27711, USA. lee.chun-wai@epa.gov
Serre
Shannon D
SD
Zhao
Yongxin
Y
Lee
Sung Jun
SJ
Hastings
Thomas W
TW
D000393:Air Pollutants; D000397:Air Pollution / Q000517:prevention & control*; D002384:Catalysis; D003031:Coal; D006851:Hydrochloric Acid; D008628:Mercury / Q000737:chemistry*; D017672:Nitrogen Compounds; D010084:Oxidation-Reduction; D011210:Power Plants; D045483:Rivers; D013455:Sulfur; D013458:Sulfur Dioxide; D013696:Temperature
D000393:Air Pollutants; D003031:Coal; D017672:Nitrogen Compounds; D013458:Sulfur Dioxide; D013455:Sulfur; D008628:Mercury; D006851:Hydrochloric Acid