Process Analysis And Simulation For The Catalytic Coupling Reaction Of Carbon Monoxide To Diethyl Oxalate

Synthesis of oxygenates from carbon monoxide continues to an area of both academic and industrial activity. In this context, synthesis of diethyl oxalate from carbon monoxide in a gaseous phase at atmospheric pressure has precently received growing attention. This work aims mainly at practical use in commercialization. Based on previous researches, thermodynamic analysis of the coupling reaction and regeneration reaction system was performed according to thermodynamic data obtained in these years and new species identified recently. Moreover, reaction behaviors with respect to operating parameters and feed composition were investigated in a fixed-bed reactor. Starting from different plausible mechanisms, twenty-three rate expressions were derived. The parameters in each proposed rate expression were estimated from the nonlinear regression. The appropriate mechanism was picked out according to the its physical meaning of the parameters and the statistic test results. It was discovered that ethyl nitrite dissociates into adsorbed ethoxy radical (EtO-) and NO, whereupon ethoxy radical reacts with absorbed carbon monoxide to absorbed alkoxycarboxide (COOEt), which further associates to diethyl oxalate. The surface reaction is the sole rate-determining step. The intrinsic kinetics was obtained from the above mechanism and the experimental data. Furthermore, by use of the nonlinear functional analysis approach-the method of adjoint operators, the sensitivity analysis for CO coupling is comprehensively carried out in order to reveal important parameters in the research of reaction mechanism and in the design and operation of a tubular reactor. Meanwhile, Steady-state simulation on the basis of industrial application were carried out with the aid of a multipurpose process simulator in order to realize the proper match of coupling reaction and regeneration reaction. The effect of all main operating parameters on the process behaviors was investigated and the suitable operation parameters were obtained. All these lay a solid fundation for realization of the two reactions' poper match and the zero-effluent of hazardous gases in this industrial process.