Steady-state and cyclic studies of Pt/BaO/Al2O 3 lean NOx traps
by Clayton, Robert Dale, Ph.D., UNIVERSITY OF HOUSTON, 2008, 402 pages; 3382498

Abstract:

Comprehensive steady-state experiments of the selective catalytic reduction of NO on a series of Pt, Pt/BaO, and BaO monolithic catalysts were carried out. The reaction between NO and H2 produces a mixture containing N2O, NH3, and N2, the composition of which is a function of the catalyst temperature and NO/H2 ratio in the feed. NO inhibits the reaction at low temperatures as revealed by light-off temperature and supporting kinetic data. NH3 is a major product under O2 deficient conditions typical of the rich pulse in NSR. NH3 oxidation ignites on Pt catalysts at 170-180°C; in the ignited state a mixture of N2, NO, NO2 and N2O is produced, the composition of which is sensitive to the NH3/O 2 feed ratio and temperature. Experiments involving a feed containing H2, NH3, and NO reveal that H2 is a much more effective reductant than NH3.

NSR experiments were replicated for a series of monoliths of progressively decreasing length, enabling the construction of spatio-temporal profiles of reactant and product concentrations. The results show that there are two primary competing routes to the desired N2 product; specifically a direct route from the reduction of stored NOx by H2 (H2 + NOx → N2) or by a sequential route through NH3 (H2 + NOx → NH 3; NH3 + NOx → N 2). A comparison between H2 and NH3 as reductants during NSR revealed H2 is a more effective reductant in terms of NOx conversion for temperatures below approximately 230°C.

The impact of Pt dispersion on NH3 formation and NOx storage and reduction was evaluated. As the dispersion increased, the amount of NOx stored and regenerated increased. For both anaerobic and aerobic regeneration feeds, the most (net) NH3 was generated by the 50% dispersion catalyst at the lowest temperature, by the 3% dispersion catalyst at the highest temperature, and by the 10% dispersion catalyst at the intermediate temperatures.

The performance of a Pt/BaO/Al2O3 monolith catalyst was studied using H2 as the reductant. The dependence of product selectivities on operating parameters is reported; including the durations of regeneration and storage times, feed composition and temperature, and monolith temperature. NOx reduction efficiency and product distribution are also compared with and without water in the feed.

 
Advisor
SchoolUNIVERSITY OF HOUSTON
SourceDAI/B 70-10, p. , Dec 2009
Source TypeDissertation
SubjectsChemical engineering
Publication Number3382498
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