Fate of sulfur in coal-direct chemical looping systems

Abstract

The fate of sulfur in the coal-direct chemical looping system was investigated in the sub-pilot reactor system. The sulfur balance was successfully closed during the injection of high sulfur coal. More than 69% of the total amount of atomic sulfur in coal was released as SO2 and H2S from the reducer flue gas stream while less than 5% was emitted as SO2 from the combustor spent air. The remaining atomic sulfur was retained in coal ash as inorganic sulfur compounds. The finding suggests an acid gas removal system targeting both H2S and SO2 is required to meet the recommended quality of CO2 stream for sequestration and transportation. Using the determined ratio of SO2 and H2S, a properly designed Claus plant can enable the recovery of elemental sulfur as a value-added byproduct. The combustor spent air was found to comply with the US EPA sulfur emission regulation and can be released to the atmosphere without a costly acid removal system. The relationship between the sulfur and carbon capture efficiencies was established experimentally and was found to be proportional to each other throughout the experiment at a slope of 0.8 below 93% of carbon capture efficiency and near 1 above 93%. This was attributed to the delayed release of organic sulfur during incomplete char gasification in the reducer. The finding affirms the effectiveness of the counter-current moving bed design for minimizing the amount of carbon and sulfur emission in the combustor spent air with an average carbon and sulfur capture efficiency of 96.5 and 95%, respectively. Sulfur deposition on the iron based oxygen carriers did not affect the system performance, and complete removal of deposited sulfur was observed during oxidation in a thermogravimetric analyzer. Compared with chemical looping systems using circulating fluidized bed configuration, the use of a moving bed reducer has the additional benefit of minimizing slippage of char into the combustor due to the use of large oxygen carrier; resulting in lower sulfur emission in the combustor spent air. The findings demonstrate the robustness of the coal-direct chemical looping system to handle high sulfur coal without a complicated acid gas cleaning scheme or severe performance penalties.