gases to less than 100 ppmv over five cycles. Actual breakthrough time for formulation C6-2-1100 was as high as 73% of breakthrough time based on wt% Mn in sorbent at 600 o C. Regeneration tests determined that loaded pellets can be essentially completely regenerated in an air/steam mixture at 750 o C with minimal sulfate formation. The leading formulation (designated C6-2) from the fixed-bed tests was then further tested under varying sorbent induration temperature, sulfidation temperature and superficial gas velocity. Four tests were conducted with each test consisting of four cycles of sulfidation and regeneration. Results showed that the induration temperature of the sorbent and the reaction temperature greatly affected the H 2 S removal capacity of the sorbent while the superficial gas velocity between 1090 and 1635 cm/min had minimal affect on the sorbent's breakthrough capacity. Testing showed that the sorbent's strength was a strong function of the sorbent induration temperature. Sorbent also showed 30 to 53% loss of its strength over four cycles of sulfidation and regeneration. The former being sorbent indurated at 1115 o C and the prior being sorbent indurated at 1100 o C. A mathematical model was developed to describe the reaction of H 2 S with the mixed metal oxide in a fixed-bed reactor, where the individual pellets react according to the shrinking core model. The effective diffusivity within a single pellet was estimated by adjusting its value until a good match between the experimental and model H 2 S breakthrough curves was obtained. Predicted sorbent conversion at the conclusion of test FB3A compared well with experimental sulfur analysis.
This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of thei employees, makes any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. y, F?
Manganese (Mn) based hot-gas-desulfurization sorbents are under investigation for use fn Integrated Gasification Combined Cycle (IGCC) advanced electric-power-generation systems. The objective of this project is to develop a regenerable Mn-based pellet formulation that can achieve low sulfur partial pressures, has a high capacity for sulfur and sufficient strength for potential use in fluidized beds, and can be regenerated for many cycles. Fifteen different formulations of manganese sesquioxide, each with either titania or alumina, were prepared and characterized at the University of Minnesota. Each formulation was indurated under conditions sufficient to achieve 1 Ib/pellet/mm of diameter crush strength. Sulfidation screening was performed in a thermogravimetric analyzer (TGA) at 500 to 900 "C. A sorbent containing MnCO, and TiO,, which showed superior crush strength and reactivity, was selected for multi-cycle fixed-bed testing at the Morgantown Energy Technology Center (METC). excellent efficiency and capacity for sulfur removal. Good regenerabiiity was achieved with air-steam at 871 "C. Four cycles of sulfidation showed that the sorbent had
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