SAPO-34 zeolite as an excellent catalyst for methanol-to-olefins (MTO) reaction suffers rapid deactivation by prevalent coking. Herein, regeneration of coked-SAPO-34 in a fluidized-bed reactor was successfully intensified by altering temperature (550–650 °C) and oxygen content (7–21 vol.%). Fresh, used, and regenerated catalysts were characterized by different methods to understand the correlation between regeneration conditions, coke content, and catalyst performance. The minor residual coke over the regenerated catalyst comprised active hydrocarbon pool intermediates (like naphthalene, benzaldehyde, phenol, and derivatives), which increased by decreasing regeneration temperature and promoted the selectivity to light olefins at earlier reaction times. The restored microporosity and lifetime of regenerated catalyst were superior by increasing temperature. However, higher attrition at 650 °C, as confirmed by SEM images, caused a partial weight loss of the catalyst and a slight decline in relative crystallinity, hence 600 °C was preferred with additional advantage of less energy consumption. Meanwhile, introducing lower oxygen not only moderated the coke oxidation rate but also enhanced the recovery of beneficial catalytic features for the MTO conversion. Consequently, considering an excellent regeneration as well as lower emission of CO2 detected in the flue gas, diluted air containing 14 vol.% O2 at 600 °C was suggested as the most promising method.
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