| In this paper,based on SAPO-34 molecular sieve,the intrinsic kinetics and deactivation mechanics of methanol to olefin(MTO)reaction were studied in an isothermal tubular fixed bed reactor(4×1-L300mm).The intrinsic kinetics and deactivation mechanics models were established,which were well compatible with the experimental data.The results of statistical tests(complex correlation index R2 and F statistics)and residual analysis show that the model is reliable.Based on the single factor experiment method,the effects of temperature(400?-485?),space velocity(3.66×103h-1-1.22×106h-1)and raw material composition(methanol 60%-100%,water vapor 0-25%)on the MTO process were investigated,which laid the foundation for the selection of MTO kinetic conditions.Under the conditions of atmospheric pressure,400-485?,water vapor mole fraction 0-25%,methanol mole fraction 60-100%and space velocity 120000 h-1,the intrinsic kinetics of MTO was studied.Based on the reaction mechanism of hydrocarbon pool and the water weakening equation,a five lumped intrinsic kinetic model of MTO was constructed,which aimed at CH3OH,CH4,C2H4,C3H6 and other components.The parameters of the kinetic model are estimated by the fourth-order longkouta integral method and the ion group algorithm.The results of statistical test(complex correlation index R2 and F statistics)and residual analysis show that the model is reliable.Under the conditions of atmospheric pressure,400-485?,water vapor mole fraction 0-25%,methanol mole fraction 60-100%and space velocity 120000 h-1,the kinetic characteristics of MTO deactivation were studied.A kinetic model of MTO deactivation with time-varying deactivation coefficient is established.The parameters of the model are estimated by difference method and ion group algorithm.The results of statistical test(complex correlation index R2 and F statistics)and residual analysis show that the calculated values of the model are consistent with the experimental values and are reliable. |
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