Sulfur removal from hot coal gas is one of important technologies for highly efficient coal-based energy system. H2S-absorption and oxidation-regeneration behavior of Ni-doped ZnO-based sorbents supported on SBA-15 (ZnNi/SBA-15) was analyzed in this work. The results indicate that ZnNi/SBA-15 shows highest H2S-uptake capacity (16 g S/100 g sorbent) and lowest amount of produced COS (0.0004 g COS/100 g sorbent) when used for desulfurization at 500 °C. Removal of H2S at 700 °C leads to lowest breakthrough sulfur capacity of sorbents. It is ascribed to the destruction of typical microscopic morphology of SBA-15. Boltzmann function is suitable for modeling the H2S-absorption behavior of ZnNi/SBA-15. The evolution rate of H2S for sorbents varies from 0.096 to 0.228 min−1 at 400–700 °C. H2S-CO and H2S-CO2 reactions both contribute to the formation of COS at the stage of H2S-absorption saraturation. Increase of temperature from 550 to 600 °C results in the disappearance of ZnS in regenerated ZnNi/SBA-15. Moreover, most of plugged pore structure caused by sulfidation reaction could restore after regeneration at 600 °C. Further increase of regeneration temperature causes the decline of regeneration efficiency and less porous sorbent. Additionally, the sorbents have stable desulfurization ability and low COS emission during multiple sulfidation-regeneration cycles.
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