Trans-level multi-scale simulation of porous catalytic systems: Bridging reaction kinetics and reactor performance

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2023-03, Vol.455, p.140745, Article 140745
• Main Authors: Li, Chengxiang, Xu, Ji, Qiu, Tianhao, Sun, Zikang, Zhang, Haolei, Ge, Wei
• Format: Article
• Language: English
• Subjects: Catalyst; Mesoscale; Molecular dynamics simulation; Multi-scale model; Reaction kinetics
• ISSN: 1385-8947
• DOI: 10.1016/j.cej.2022.140745

[Display omitted] •Modeling trans-level multi-scale coupled of reaction, diffusion and fluid flow.•Apparent reaction kinetics at multi-scales obtained from intrinsic kinetics.•Effect of complex pore structure and its continuous size distribution on diffusion.•Multi-scale transport makes much difference in reaction rate & products selectivity. Multi-scale porous structures inside and/or between the catalyst pellets or particles are found in many chemical processes, where strong coupling of reaction and transport results in complex apparent reaction kinetics influential to the reactor performance. Traditional continuum-based porous media models and simulation methods can hardly describe such structures and their scale effects faithfully. A trans-level multi-scale discrete computational framework is hence proposed to address this complexity and implemented for an olefin catalytic cracking (OCC) process. The apparent reaction kinetics at the REV (representative elementary volume) scale is obtained by hard-sphere pseudo-particle modeling (HS-PPM), and coupled with computational fluid dynamics / discrete element method (CFD-DEM) for the reactor-level hydrodynamics via a one-dimensional (1D) finite difference scheme for particle-level diffusion. The mesoscales of the REVs and the flow networks between the particles are thus covered by the framework, which are previously described by simple average quantities in the continuum methods. The reactant conversion rate and target product selectivity obtained agree well with experimental results, while a continuum approach may give significantly different and unreasonable results. The multi-scale method is, therefore, demonstrated to be necessary and effective for bridging the intrinsic reaction kinetics with the performance of porous catalytic reactors.