Multiscale kinetic modeling in catalysis ⇒ from microkinetics to computational fluid dynamics and process simulations

Problem statement

We envision multiscale modeling as critical enablers of reaction understanding, catalyst and reactor design, scale-up, and process optimization. The framework includes predicting the molecular reaction mechanism at the molecular level to the process optimization stage. As catalytic processes occur at the multiscale, we address these issues individually and collectively.

At the microkinetic level, our models resolve the rates of the individual elementary steps, rate-determining step (RDS), adsorption, and desorption mechanisms. We use quantum chemical calculations (density functional theory, DFT) to support our assumed kinetic pathways, original parameter estimations, and adsorption-desorption energies.

We incorporate thermodynamic constraints into our models. Once developed, the microkinetic model could guide the catalyst and reactor design. We also have experience developing Langmuir-Hinshelwood and Eley-Rideal types of kinetic models.

At the macrokineitc level, we develop lump-based and empirical models which, in some cases, are very robust and, together with other models, can be used to extract information such as mechanism change, optimize conditions, or for reactor pre-design.

We couple hydrodynamics, heat transfer, and reaction kinetics at the reactor level in computational fluid dynamic (CFD) simulations. Together with optimization algorithms, we aim to improve operating scenarios, develop innovative reactor prototypes, and predict process behaviors at the industrial scale.

Goals

  • Microkinetics I ⇒ key thermodynamic relationships
  • Microkinetics II ⇒ fitting, training, and optimization
  • Microkinetics III ⇒ ab initio kinetic modeling
  • Macrokinetics ⇒ complex reaction networks and population balances
  • CPFD ⇒ reactor modeling and scale-up
  • CFD ⇒ reactor modeling and optimization
  • CFD II ⇒ modeling operando reactors
  • Process system engineering ⇒ gPROMS

Related People

Related Publications

Microkinetic Modeling to Decode Catalytic Reactions and Empower Catalytic Design

by Kulkarni, Lezcano, Velisoju, Realpe, Castaño
ChemCatChem Year: 2024 DOI: https://doi.org/10.1002/cctc.202301720

Abstract

Kinetic model development is integral for designing, redesigning, monitoring, and optimizing chemical processes. Of the various approaches used within this field, microkinetic modeling is a crucial tool that focuses on surface events to analyze overall and preferential reaction pathways. This work covers noticeable features of microkinetic modeling for three critical case studies: (i) ammonia to hydrogen, (ii) oxidative coupling of methane to chemicals, and (iii) carbon dioxide hydrogenation for methanol synthesis. We analyze how microkinetic modeling enables predicting and optimizing complex reaction networks, allowing the design of efficient and tailored catalysts with enhanced activity and selectivity.

Keywords

MKM CO2 CHA AMD