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Simultaneous Fixed Bed Removal of Nitrogen Oxides and Mercury Using Manganese and Cerium Mixed Metal Oxide Catalysts at Low Temperature SCR

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2018, MS, University of Cincinnati, Engineering and Applied Science: Chemical Engineering.
In the last few decades there has been increasing concern about the effects of air pollution on the environment and human health. It is important to control emissions from coal-fired power plants, which are one of the major sources of air pollution by the emission of NOx, mercury and other heavy metals such as arsenic. Cost effective technologies must be developed to curb this pollution to reduce the threat to the worldwide environment and to human health. In this work, manganese-cerium mixed-metal oxide catalysts were evaluated for simultaneous removal of nitrogen oxide and gas phase elemental mercury at low temperature selective catalytic reduction (LTSCR) conditions using ammonia as a reductant. The effect sulfur dioxide and water on LTSCR was also studied as these gases are also present in flue gas from power plants along with nitrogen oxide and mercury and affect the efficiency of LTSCR catalysts. The catalysts used in this study were MnOx-CeO2-MxOy (MxOy = Al2O3, HfO2, SiO2, ZrO2), identified as MCA, MCH, MCS, MCZ respectively. The simultaneous capacity of these materials to remove NO and Hg0 in the presence of SO2 and water was determined at 160°C. The material with highest performance at 160°C was MCA with 12 mg g-1 Hg0 adsorption and average NO removal of 75%. MCZ had 13.3 mg g-1 Hg0 adsorption and average NO removal of 68% followed by MCH with 10.4 mg g-1 Hg0 adsorption and average NO removal of 55%. MCS had 8 mg g-1 Hg0 adsorption and average NO removal of 58%. The influence of temperature on the simultaneous removal capacity of each material in the presence of SO2 and water was determined by lowering the catalyst bed temperature to 140°C and increasing the bed temperature to 200°C. At 140°C MCA had highest Hg0 adsorption at 10 mg g-1 Hg0 adsorption followed by MCA 8 mg g-1 Hg0 adsorption. The Hg0 adsorption for MCH and MCS was 6.5 mg g-1 and 4.2 mg g-1 respectively. When the bed temperature was increased to 200°C the Hg adsorption capacities increased remarkably. The NO catalytic removal for all materials in all three cases remained same. Hence, the presence of Hg0 does not affect the reduction of NO in simultaneous study. The simultaneous removal capacities decrease when SO2 and H2O was present in the inlet gas stream. The simultaneous removal capacities determined in this study in the presence of SO2 and H2O are much greater than previous studies completed and in the literature. In summary, the catalysts MnOx-CeO2-MxOy (MxOy = Al2O3, HfO2, SiO2, ZrO2) can simultaneously remove of NO and Hg0 in the presence of SO2 and water. These catalysts sustained their catalytic activity in simulated flue gas inlet concentrations much higher than observed in realistic applications. These materials can be a cost-effective alternative for multi-pollutant control in coal combustion.
Stephen Thiel, Ph.D. (Committee Chair)
Mingming Lu, Ph.D. (Committee Member)
Peter Panagiotis Smirniotis, Ph.D. (Committee Member)
108 p.

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Citations

  • Patil, A. (2018). Simultaneous Fixed Bed Removal of Nitrogen Oxides and Mercury Using Manganese and Cerium Mixed Metal Oxide Catalysts at Low Temperature SCR [Master's thesis, University of Cincinnati]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1530266242697853

    APA Style (7th edition)

  • Patil, Aniket . Simultaneous Fixed Bed Removal of Nitrogen Oxides and Mercury Using Manganese and Cerium Mixed Metal Oxide Catalysts at Low Temperature SCR. 2018. University of Cincinnati, Master's thesis. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=ucin1530266242697853.

    MLA Style (8th edition)

  • Patil, Aniket . "Simultaneous Fixed Bed Removal of Nitrogen Oxides and Mercury Using Manganese and Cerium Mixed Metal Oxide Catalysts at Low Temperature SCR." Master's thesis, University of Cincinnati, 2018. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1530266242697853

    Chicago Manual of Style (17th edition)