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Frontal polymerization in thin layers: Hydrodynamic effects and asymptotic dynamics.
R Tiani1, John A Pojman2, L Rongy1
1Nonlinear Physical Chemistry Unit, Université libre de Bruxelles (ULB), Faculté des Sciences, CP231, 1050 Brussels, Belgium.
The Journal of Chemical Physics
|March 26, 2025
Summary
Buoyancy-driven convection in thermal frontal polymerization (FP) creates complex reaction patterns. This study reveals a transition to an active chemo-hydrodynamic regime where convection slows polymerization, impacting front propagation speed.
Area of Science:
- Chemical Engineering
- Fluid Dynamics
- Polymer Science
Background:
- Buoyancy-driven convection arises from temperature gradients in thermal frontal polymerization (FP).
- The polymerization reaction front moves perpendicular to the gravity field.
- Reactant viscosity can increase with the degree of polymerization.
Purpose of the Study:
- To theoretically study the dynamics of buoyancy-driven convection in thermal frontal polymerization under adiabatic conditions.
- To investigate the transition between passive and active chemo-hydrodynamic regimes.
- To explain how hydrodynamic currents affect polymerization wave velocity.
Main Methods:
- Theoretical modeling of system dynamics.
- Analysis of reaction-diffusion and hydrodynamic interactions.
- Scaling analysis to explain the influence of convection on front speed.
Main Results:
- The reaction zone propagates as a hot spot with broken symmetry.
- A steady-state asymptotic dynamics is reached, characterized by a propagating front and a surrounding vortex.
- A transition occurs from a passive regime to an active chemo-hydrodynamic regime as vortex strength increases.
- In the active regime, increased convection intensifies and decreases the front speed.
- Increased polymer viscosity shifts flow ahead of the reaction zone, enhancing symmetry.
Conclusions:
- Buoyancy-driven convection significantly alters frontal polymerization dynamics.
- Hydrodynamic effects can lead to a decrease in polymerization wave velocity.
- The study provides insights into the interplay between reaction kinetics and fluid dynamics in FP systems.
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