RESUMO
In the present study, the performance of a CaMn0.775Ti0.125Mg0.1O2.9-δ perovskite used as an oxygen carrier to burn sour gas with different H2S concentrations (up to 3000 vppm) in a continuous 500 Wth chemical looping combustion (CLC) prototype was investigated. After 29 h of sour gas combustion, the combustion efficiency had dropped by 18% in comparison with the reference test without sulfur addition. The characterization of the used particles of the perovskite confirmed that the presence of sulfur in the fuel gas had a poisonous effect through the formation of undesired compounds, such as CaSO4. The reactivity with CH4 and oxygen uncoupling capacity decreased, which could explain the decrease in the combustion efficiency. Two regeneration processes, one at high temperature (1273 K) and another one at low temperature (773-873 K), were carried out in a batch fluidized bed reactor to remove the amount of sulfur accumulated in the oxygen carrier particles. The detection of appreciable amounts of gaseous sulfur-based compounds (SO2 and H2S) during the experimentation and the postcharacterization results obtained through different techniques such as X-ray diffraction, ultimate analysis, and thermogravimetric analysis confirmed the effectiveness of both processes. Finally, the feasibility of implementation of the regeneration processes in a commercial CLC unit was thoroughly analyzed.
RESUMO
The heterogeneous reaction of soot with NO can be considered as a means of reduction of the emissions of both pollutants from combustion systems. In this paper, the influence of the presence of CO in the soot-NO reaction is studied. Soot was obtained by pyrolysis at 1373 K of 5000 ppmv acetylene in nitrogen. The study of the influence of CO on the soot-NO reaction was performed in experiments fixing NO concentration at 900 ppmv and introducing different CO concentrations among 0 and 9900 ppmv. An increase in both the carbon consumption rate and NO reduction by acetylene soot was observed as the concentration of CO increases. These results can be explained by the oxide-stripping reaction, CO+C(f)(O)-->CO(2)+C(f). The direct reaction of CO with NO catalyzed by the carbon surface, CO+NO-->CO(2)+1/2N(2) may not be considered in this case the dominant process due to the absence of mineral impurities in the acetylene soot. The influence of CO in the acetylene soot-NO reaction was also tested in the presence of oxygen (250-5000 ppmv). In these conditions and for relatively high CO/O(2) ratios, CO seems to also contribute to NO reduction by the previous oxide-stripping reaction.
