Effect of Reactor Heat Transfer Limitations on Co Preferential Oxidation

Our recent studies of CO preferential oxidation (PrOx) identified systemic differences between the characteristic curves of CO conversion for a microchannel reactor with thin-film wall catalyst and conventional packed-bed lab reactors (m-PBR’s). Strong evidence has suggested that the reverse water-gas-shift (r-WGS) side reaction activated by temperature gradients in m-PBR’s is the source of these differences. In the present work, a quasi-3D tubular non-isothermal reactor model based on the finite difference method was constructed to quantitatively study the effect of heat transport resistance on PrOx reaction behavior. First, the kinetic expressions for the three principal reactions involved were formed based on the combination of experimental data and literature reports and their parameters were evaluated with a nonlinear regression method. Based on the resulting kinetic model and an energy balance derived for PrOx, the finite difference method was then adopted for the quasi-3D model. This model was then used to simulate both the microreactor and m-PBR’s and to gain insights into their different conversion behavior. Simulation showed that the temperature gradients in m-PBR’s favor the reverse water-gas-shift (r-WGS) reaction, thus causing a much narrower range of permissible operating temperature compared to the microreactor. Accordingly, the extremely efficient heat removal of the microchannel/thin-film catalyst system eliminates temperature gradients and efficiently prevents the onset of the r-WGS reaction.