In this work, the steady-state performance of zeolite-based Cu-ZSM-5, vanadium based honeycomb monolith catalysts (V), vanadium-titanium based pillared inter layered clay catalyst (V-Ti PLIC) and vanadium-titanium-tungsten-based honeycomb monolith catalysts (V-Ti-W) was investigated in the selective catalytic reduction process (SCR) for NO removal using NH3 in presence of oxygen. The objective is to obtain the expression that would predict the conversion performance of the catalysts for different values of the SCR process parameters, namely temperature, inlet oxygen concentration and inlet ammonia concentration.
The NOx emission, its formation and control methods are discussed briefly and then the fundamentals of the SCR process are described. Heat transfer based and chemical kinetics based SCR process models are discussed and widely used rate order based model are reviewed.
Based on the experimental data, regression analysis was performed that gives an expression for predicting the SCR rate for the complete temperature range and the rate order with respect to inlet oxygen and ammonia concentration. The average activation energy for the SCR process was calculated and optimum operating conditions were determined for each of the catalyst.
The applicable operating range for the catalyst depends on the NO conversion as well as on the ammonia slip and the N2O and NO2 emission. The regression analysis was repeated for the applicable range and an expression was obtained that can be used to estimate the catalyst performance.
For the Cu-ZSM-5, the best performance was observed for 400oC, 660 ppm inlet ammonia concentration and 0.1% inlet oxygen concentration. For the V based honeycomb monolith catalyst, the best performance was observed for 300oC, 264 ppm inlet ammonia concentration and 3% inlet oxygen concentration. For the V-Ti based PLIC catalyst, the best performance was observed for 350oC, 330 ppm inlet ammonia concentration and 3% inlet oxygen concentration. For the V-Ti-W based honeycomb monolith catalyst, the best performance was observed for 300oC, 330 ppm inlet ammonia concentration and 3% inlet oxygen concentration. The conversion performance of all of these catalysts is satisfactory for the industrial application. At the operating conditions listed above, the N2O emission is less than 20 ppm and the NO2 emission is less than 10 ppm.
The results were validated by comparing the findings with the similar work by other research groups. The mechanism of SCR process is discussed for each of the catalyst. The probable reactions are listed and adsorption and desorption process are studied. The various mechanisms proposed by the researchers are discussed briefly.
It is concluded that V-Ti-W and Cu-ZSM-5 catalyst are very promising for SCR of NOx. The expressions can be used to estimate the conversion performance and can be utilized for optimal design and operation. The expressions relate the SCR rate to the input parameters such as temperature and inlet oxygen and ammonia concentration hence by controlling these parameters desired NOx reduction can be achieved with minimal cost and emission.
| Identifer | oai:union.ndltd.org:tamu.edu/oai:repository.tamu.edu:1969.1/2785 |
| Date | 01 November 2005 |
| Creators | Sharma, Giriraj |
| Contributors | Caton, J. A. |
| Publisher | Texas A&M University |
| Source Sets | Texas A and M University |
| Language | en_US |
| Detected Language | English |
| Type | Book, Thesis, Electronic Thesis, text |
| Format | 1854038 bytes, electronic, application/pdf, born digital |
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