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Sulfidation kinetics of dolomite at high pressure and high temperature

Santhosh K. Misro, Raja A. Jadhav, Himanshu Gupta, R. Agnihotri, S. Chauk, Long Fan

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Abstract

Kinetic studies of the dolomite sulfidation reaction are carried out at high pressure (15 atm) and high temperature (600--900 C) in a differential bed flow-through reactor. The dolomite particles are exposed to simulated coal gas environments and the extent of conversion determined. Experiments are carried out to determine the influence of total pressure, reaction temperature and partial pressure of H{sub 2}S on the extent of fully calcined dolomite (FCD) sulfidation. Based on the grain theory it is found that towards the later stages of the reaction the FCD sulfidation is product layer diffusion controlled. The reaction is found to be first order with respect to H{sub 2}S partial pressure. A low apparent activation energy of 4.6 kcal/gmol for the product layer diffusion controlled reaction is attributed to the presence of porous MgO along with the low porosity CaS product layer. A comparison of the performance of dolomite and limestone as sorbents for desulfurization shows that dolomite is a better sorbent with higher conversions even at higher CO{sub 2} partial pressures. The high pressure sulfidation kinetic data obtained in this study would be useful in understanding and optimizing the in-gasifier H{sub 2}S capture using dolomite sorbents.

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Kinetic studies of the dolomite sulfidation reaction are carried out at high pressure (15 atm) and high temperature (600--900 C) in a differential bed flow-through reactor. The dolomite particles are exposed to simulated coal gas environments and the extent of conversion determined. Experiments are carried out to determine the influence of total pressure, reaction temperature and partial pressure of H{sub 2}S on the extent of fully calcined dolomite (FCD) sulfidation. Based on the grain theory it is found that towards the later stages of the reaction the FCD sulfidation is product layer diffusion controlled. The reaction is found to be first order with respect to H{sub 2}S partial pressure. A low apparent activation energy of 4.6 kcal/gmol for the product layer diffusion controlled reaction is attributed to the presence of porous MgO along with the low porosity CaS product layer. A comparison of the performance of dolomite and limestone as sorbents for desulfurization shows that dolomite is a better sorbent with higher conversions even at higher CO{sub 2} partial pressures. The high pressure sulfidation kinetic data obtained in this study would be useful in understanding and optimizing the in-gasifier H{sub 2}S capture using dolomite sorbents.

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Available abstract

Kinetic studies of the dolomite sulfidation reaction are carried out at high pressure (15 atm) and high temperature (600--900 C) in a differential bed flow-through reactor. The dolomite particles are exposed to simulated coal gas environments and the extent of conversion determined. Experiments are carried out to determine the influence of total pressure, reaction temperature and partial pressure of H{sub 2}S on the extent of fully calcined dolomite (FCD) sulfidation. Based on the grain theory it is found that towards the later stages of the reaction the FCD sulfidation is product layer diffusion controlled. The reaction is found to be first order with respect to H{sub 2}S partial pressure. A low apparent activation energy of 4.6 kcal/gmol for the product layer diffusion controlled reaction is attributed to the presence of porous MgO along with the low porosity CaS product layer. A comparison of the performance of dolomite and limestone as sorbents for desulfurization shows that dolomite is a better sorbent with higher conversions even at higher CO{sub 2} partial pressures. The high pressure sulfidation kinetic data obtained in this study would be useful in understanding and optimizing the in-gasifier H{sub 2}S capture using dolomite sorbents.

Key concepts: Sulfidation, Dolomite, Porosity, Partial pressure, Sorbent, Diffusion, Chemistry, Mineralogy

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