(24g) Comparative Investigation on Chemical Looping Combustion of Coal-Derived Synthesis Gas Containing H2s Over Supported Fe2O3 - MnO2 Oxygen Carrier

Poston, J. - Presenter, National Energy Technology Laboratory, U.S. Department of Energy
Ksepko, E. - Presenter, Institute for Chemical Processing of Coal
Siriwardane, R. V. - Presenter, National Energy Technology Laboratory, U.S. Department of Energy
Simonyi, T. - Presenter, RDS, Parsons Infrastructure & Technology Group, Inc
Marek, S. - Presenter, Institute for Chemical Processing of Coal

The paper contains results of collaborative research work on novel combustion technology known as chemical looping combustion (CLC). The objective of paper was to prepare Fe2O3 - MnO2 supported on ZrO2/Al2O3/Sepiolite (ICPC, Poland) oxygen carriers and to evaluate the performance (NETL, US DOE) of these for the CLC process with synthesis gas/air. Thermo gravimetric analysis (TGA) and low pressure (10 psi) bench scale flow reactor tests were conducted to evaluate the performance. Multi cycle tests were conducted in an atmospheric TGA with oxygen carriers utilizing simulated synthesis gas with & without H2S. Effect of H2S impurities on both the stability and the oxygen transport capacity was evaluated. Multi cycle CLC tests were also conducted in the bench scale flow reactor at 800 °C with selected samples. Chemical phase composition was investigated by X-Ray diffraction (XRD) technique.

Five Cycle TGA tests at 800 °C indicated that all oxygen carriers had a stable performance at 800 °C. It was interesting to note that there was complete reduction/oxidation of the oxygen carrier during the 5-cycle test. The fractional reduction, fractional oxidation and global reaction rates were calculated from the data. It was found, that support had a significant effect on both fractional reduction/oxidation and the reaction rate. The oxidation reaction was significantly faster than the reduction reaction for all oxygen carriers.  The reaction profile was changed by the presence of H2S but there was no effect on the reaction rate due to presence of H2S in syntheses gas. Low pressure bench scale flow reactor data indicated stable reactivity, full consumption of oxygen from oxygen carrier and complete combustion of H2 and CO.  XRD data of samples after multi-cycle test showed stable crystalline phases without any formation of sulfides or sulfites/sulfates and complete regeneration of the oxygen carrier after multi-cycle tests.