An integrated NOx adsorption-reduction process has been proposed in this study for the treatment of flue gases under lean-burn conditions by decoupling the adsorption and reduction into two different zones. The hypothesis has then been validated in a novel internal circulating fluidized bed. The adsorption and reaction performance of Fe/ZSM-5 for the selective catalytic reduction (SCR) of NOx with propylene was investigated in a fixed bed reactor. The fine Fe/ZSM-5(Albemarle) catalyst showed reasonable NOx adsorption capacity, and the adsorption performance of the catalyst was closely related to the particle size and other catalyst properties. Fe/ZSM-5 catalyst was sensitive to the reaction temperature and space velocity, and exhibited acceptable activity when O₂ concentration was controlled at a low level. Water in the flue gas was found to slightly enhance the reactivity of Fe/ZSM-5(Albemarle), while the presence of CO₂ showed little effect. SO₂ severely inhibited the reactivity of Fe/ZSM-5(Albemarle), and the deactivated catalyst could be only partially regenerated. Configurations of the reactor influenced the hydrodynamic performance significantly in a cold model internal circulating fluidized bed (ICFB) reactor. For all configurations investigated, the high gas bypass ratio from the annulus to draft tube (RAD) and low draft tube to annulus gas bypass ratio (RDA) were observed, with the highest RDA associated with the conical distributor which showed the flexible and stable operation over a wide range of gas velocities. Solids circulation rates increased with the increase of gas velocities both in the annulus and the draft tube. Gas bypass was also studied in a hot model ICFB reactor. The results showed that the orientation of perforated holes on the conical distributor could be adjusted to reduce RAD and/or enhance RDA. Coarse Fe/ZSM-5(PUC) and fine Fe/ZSM-5(Albemarle) catalysts were used in an ICFB and a conventional bubbling fluidized bed to test the NOx reduction performance. Coarse Fe/ZSM-5(PUC) catalyst showed poor catalytic activity, while fine Fe/ZSM-5(Albemarle) catalyst exhibited promising NOx reduction performance and strong inhibiting ability to the negative impact of excessive O₂ in the ICFB reactor, proving that the adsorption-reduction two-zone reactor is effective for the NOx removal from oxygen-rich combustion flue gases.

An integrated NOx adsorption-reduction process has been proposed in this study for the treatment of flue gases under lean-burn conditions by decoupling the adsorption and reduction into two different zones. The hypothesis has then been validated in a novel internal circulating fluidized bed. The adsorption and reaction performance of Fe/ZSM-5 for the selective catalytic reduction (SCR) of NOx with propylene was investigated in a fixed bed reactor. The fine Fe/ZSM-5(Albemarle) catalyst showed reasonable NOx adsorption capacity, and the adsorption performance of the catalyst was closely related to the particle size and other catalyst properties. Fe/ZSM-5 catalyst was sensitive to the reaction temperature and space velocity, and exhibited acceptable activity when O₂ concentration was controlled at a low level. Water in the flue gas was found to slightly enhance the reactivity of Fe/ZSM-5(Albemarle), while the presence of CO₂ showed little effect. SO₂ severely inhibited the reactivity of Fe/ZSM-5(Albemarle), and the deactivated catalyst could be only partially regenerated. Configurations of the reactor influenced the hydrodynamic performance significantly in a cold model internal circulating fluidized bed (ICFB) reactor. For all configurations investigated, the high gas bypass ratio from the annulus to draft tube (RAD) and low draft tube to annulus gas bypass ratio (RDA) were observed, with the highest RDA associated with the conical distributor which showed the flexible and stable operation over a wide range of gas velocities. Solids circulation rates increased with the increase of gas velocities both in the annulus and the draft tube. Gas bypass was also studied in a hot model ICFB reactor. The results showed that the orientation of perforated holes on the conical distributor could be adjusted to reduce RAD and/or enhance RDA. Coarse Fe/ZSM-5(PUC) and fine Fe/ZSM-5(Albemarle) catalysts were used in an ICFB and a conventional bubbling fluidized bed to test the NOx reduction performance. Coarse Fe/ZSM-5(PUC) catalyst showed poor catalytic activity, while fine Fe/ZSM-5(Albemarle) catalyst exhibited promising NOx reduction performance and strong inhibiting ability to the negative impact of excessive O₂ in the ICFB reactor, proving that the adsorption-reduction two-zone reactor is effective for the NOx removal from oxygen-rich combustion flue gases.

An integrated NOx adsorption-reduction process has been proposed in this study for the treatment of flue gases under lean-burn conditions by decoupling the adsorption and reduction into two different zones. The hypothesis has then been validated in a novel internal circulating fluidized bed. The adsorption and reaction performance of Fe/ZSM-5 for the selective catalytic reduction (SCR) of NOx with propylene was investigated in a fixed bed reactor. The fine Fe/ZSM-5(Albemarle) catalyst showed reasonable NOx adsorption capacity, and the adsorption performance of the catalyst was closely related to the particle size and other catalyst properties. Fe/ZSM-5 catalyst was sensitive to the reaction temperature and space velocity, and exhibited acceptable activity when O₂ concentration was controlled at a low level. Water in the flue gas was found to slightly enhance the reactivity of Fe/ZSM-5(Albemarle), while the presence of CO₂ showed little effect. SO₂ severely inhibited the reactivity of Fe/ZSM-5(Albemarle), and the deactivated catalyst could be only partially regenerated. Configurations of the reactor influenced the hydrodynamic performance significantly in a cold model internal circulating fluidized bed (ICFB) reactor. For all configurations investigated, the high gas bypass ratio from the annulus to draft tube (RAD) and low draft tube to annulus gas bypass ratio (RDA) were observed, with the highest RDA associated with the conical distributor which showed the flexible and stable operation over a wide range of gas velocities. Solids circulation rates increased with the increase of gas velocities both in the annulus and the draft tube. Gas bypass was also studied in a hot model ICFB reactor. The results showed that the orientation of perforated holes on the conical distributor could be adjusted to reduce RAD and/or enhance RDA. Coarse Fe/ZSM-5(PUC) and fine Fe/ZSM-5(Albemarle) catalysts were used in an ICFB and a conventional bubbling fluidized bed to test the NOx reduction performance. Coarse Fe/ZSM-5(PUC) catalyst showed poor catalytic activity, while fine Fe/ZSM-5(Albemarle) catalyst exhibited promising NOx reduction performance and strong inhibiting ability to the negative impact of excessive O₂ in the ICFB reactor, proving that the adsorption-reduction two-zone reactor is effective for the NOx removal from oxygen-rich combustion flue gases. / Applied Science, Faculty of / Chemical and Biological Engineering, Department of / Graduate