Simultaneous Removal of NOx and Mercury in Low Temperature Selective Catalytic and Adsorptive Reactor

Pinto, Neville G. ; Smirniotis, Panagiotis G.

University of Cincinnati

关键词: Nitrogen Oxides;    Catalytic Effects;    Carbon Monoxide;    01 Coal, Lignite, And Peat;    Reducing Agents;   

DOI  :  10.2172/895484
RP-ID  :  None
RP-ID  :  FG26-04NT42180
RP-ID  :  895484

美国|英语

来源: UNT Digital Library

【 摘 要 】

The results of a 18-month investigation to advance the development of a novel Low Temperature Selective Catalytic and Adsorptive Reactor (LTSCAR), for the simultaneous removal of NO{sub x} and mercury (elemental and oxidized) from flue gases in a single unit operation located downstream of the particulate collectors, are reported. In the proposed LTSCAR, NO{sub x} removal is in a traditional SCR mode but at low temperature, and, uniquely, using carbon monoxide as a reductant. The concomitant capture of mercury in the unit is achieved through the incorporation of a novel chelating adsorbent. As conceptualized, the LTSCAR will be located downstream of the particulate collectors (flue gas temperature 140-160 C) and will be similar in structure to a conventional SCR. That is, it will have 3-4 beds that are loaded with catalyst and adsorbent allowing staged replacement of catalyst and adsorbent as required. Various Mn/TiO{sub 2} SCR catalysts were synthesized and evaluated for their ability to reduce NO at low temperature using CO as the reductant. It has been shown that with a suitably tailored catalyst more than 65% NO conversion with 100% N{sub 2} selectivity can be achieved, even at a high space velocity (SV) of 50,000 h-1 and in the presence of 2 v% H{sub 2}O. Three adsorbents for oxidized mercury were developed in this project with thermal stability in the required range. Based on detailed evaluations of their characteristics, the mercaptopropyltrimethoxysilane (MPTS) adsorbent was found to be most promising for the capture of oxidized mercury. This adsorbent has been shown to be thermally stable to 200 C. Fixed-bed evaluations in the targeted temperature range demonstrated effective removal of oxidized mercury from simulated flue gas at very high capacity ({approx}>58 mg Hg/g adsorbent). Extension of the capability of the adsorbent to elemental mercury capture was pursued with two independent approaches: incorporation of a novel nano-layer on the surface of the chelating mercury adsorbent to achieve in situ oxidation on the adsorbent, and the use of a separate titania-supported manganese oxide catalyst upstream of the oxidized mercury adsorbent. Both approaches met with some success. It was demonstrated that the concept of in situ oxidation on the adsorbent is viable, but the future challenge is to raise the operating capacity beyond the achieved limit of 2.7 mg Hg/g adsorbent. With regard to the manganese dioxide catalyst, elemental mercury was very efficiently oxidized in the absence of sulfur dioxide. Adequate resistance to sulfur dioxide must be incorporated for the approach to be feasible in flue gas. A preliminary benefits analysis of the technology suggests significant potential economic and environmental advantages.