Interaction between transport and reaction generates a variety of complex spatio-temporal patterns in chemical reactors. These patterned states, which are typically initiated by autocatalytic effects and sustained by differences in diffusion/local mixing rates, often cause undesired effects in the reactor. In this work, we analyze the dynamic evolution of mixing-limited spatial pattern formation in fast, homogeneous autocatalytic reactions occurring in isothermal tubular reactors using two-dimensional (2-D) convection-diffusion-reaction (CDR) models that are obtained through rigorous spatial averaging of the three-dimensional (3-D) CDR model using Liapunov-Schmidt technique of bifurcation theory. We use the spatially-averaged 2-D CDR model (and its "regularized" form) to perform steady-state bifurcation analysis that captures the region of multiple solutions, and we analyze the stability of these multiple steady states to transverse perturbations using linear stability analysis. Parametric analyses of the steady-state bifurcation diagrams and stability boundaries show that when transverse mixing is significantly slower than the rate of autocatalytic reaction, mixing-limited patterns emerge from the unstable middle branch that connects the ignition and extinction points of an S-shaped bifurcation curve. Our dynamic simulations show the emergence of three different types of spatial patterns namely, Band, Anti-phase and Target, depending on the nature of transverse perturbation. The temporal evolution of these patterns consists of rapid intensification of the concentration-segregation process (especially when transverse mixing is much slower than reaction) followed by slow diffusion-mediated return to symmetry that occurs at time scales much larger than the reactor residence time. Our parametric analysis of the dynamics reveals that while larger Péclet numbers (both axial and transverse) increase the stability and decay time of the patterned states, larger Damköhler numbers lead to faster ignition resulting in the opposite effect.
Spontaneous pattern formation upon incoherent waves: From modulation-instability to steady-state