n-butane partial oxidation in a fixed bed: A resolved particle computational fluid dynamics simulation

Maleic anhydride (MA) is an important chemical intermediate, which is mainly produced by the highly exothermic partial oxidation of n-butane in fixed bed reactors. Production of maleic anhydride is limited by problems of temperature control and loss of selectivity. Here we present three-dimensional resolved-particle computational fluid dynamics (CFD) simulations of n-butane partial oxidation in a randomly packed bed of 807 spherical catalyst particles. We used a semi-empirical two-site surface mechanism from the literature and obtained distributions of temperature, gas phase species, and surface species in the bed. The local selectivity patterns are strongly controlled by the changes in the gas phase flow field, the temperature in the fixed bed, and the weakly adsorbed oxygen surface coverage fraction ((O)) profiles inside the particles. Most of the selectivity loss due to product combustion happens in the interior of the catalyst particles, as opposed to the production of MA, which is mainly in the near-surface layers. We observed loss of selectivity and yield in the centre of the bed at increased bed depths, because of the temperature increase and decrease in gas phase oxygen there. The simulations show sharp (O) gradients inside the particles. Near the cooled tube wall (O) is strongly affected by the temperature, while at the bed centre gas phase oxygen diffusion limitations contribute to a depleted oxygen surface resulting in lower selectivity.