Predictive-Quality Surface Reaction Chemistry in Real Reactor Models: Integrating First-Principles Kinetic Monte Carlo Simulations into Computational Fluid Dynamics
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High Resolution Image Download MS PowerPoint Slide We present a numerical framework to integrate first-principles kinetic Monte Carlo (1p-kMC) based microkinetic models into the powerful computational fluid dynamics (CFD) package CatalyticFoam. This allows for the simultaneous account of a predictive-quality surface reaction kinetics inside an explicitly described catalytic reactor geometry. Crucial means toward an efficient and stable implementation are the exploitation of the disparate time scales of surface chemistry and gas-phase transport, as well as the reliable interpolation of irregularly gridded 1p-kMC data by means of an error-based modified Shepard approach. We illustrate the capabilities of the framework using the CO oxidation at Pd(100) and RuO 2 (110) model catalysts in different reactor configurations and fluid dynamic conditions as showcases. These showcases underscore both the necessity and value of having reliable treatments of the surface chemistry and flow inside integrated multiscale catalysis simulations when aiming at an atomic-scale understanding of the catalytic function in near-ambient environments. Our examples highlight how intricately this function is affected by specifics of the reactor geometry and heat dissipation channels on the one end, and on the other end by characteristics of the intrinsic catalytic activity that are only captured by treatments beyond prevalent mean-field rate equations.
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Logarithmic transformations have been used for gas-phase mass fractions, and preprocessing data as log(r), log(p_i) and 1/T is well known to facilitate modeling of surface kinetics.
“Logarithmic transfor-mations have been used for gas-phase mass fractions 6,11,37 while preprocessing data as log(r), log(p i ) and 1/T is well known to facilitate modeling of surface kinetics 14,15,17,19,27,29 .”
From Efficient neural network models of chemical kinetics using a latent asinh rate transformation (2023) · cites this paper as [17]
Logarithmic transformations make the target function more linear over a wide range of reaction conditions.
“This can be accounted to the fact that it makes the target function more linear over a wide range of reaction conditions 17,29 as demonstrated in equations S1 -S3 in the ESI † .”
From Efficient neural network models of chemical kinetics using a latent asinh rate transformation (2023) · cites this paper as [17]
The (error-based modified) Shepard interpolation approach has been used to replace detailed kinetic Monte-Carlo calculations in reactor simulations.
“The (error-based modified) Shepard interpolation approach has been used to replace very demanding but detailed kinetic Monte-Carlo calculations in reactor simulations.17,32,33”
From Efficient neural network models of chemical kinetics using a latent asinh rate transformation (2023) · cites this paper as [17]
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Self-citation
- Authors
- Matera, S., Maestri, M., Cuoci, A., & Reuter, K.
- Affiliations
- Technical University of Munich (DE)
- Politecnico di Milano (IT)
- Corresponding author
- Matera, Sebastian
- Maestri, Matteo
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2014-10-24
- Volume
- 4
- Issue
- 11
- Pages
- 4081-4092
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2335186032
- Cited by
- 92
- References
- 34
- Citations by year
- 2026: 7 · 2025: 5 · 2024: 9 · 2023: 3 · 2022: 10 · 2021: 2 · 2020: 9 · 2019: 10 · 2018: 11 · 2017: 9 · 2016: 12 · 2015: 5
- FWCI
- 3.93
- Type
- journal article
- Language
- en
- Open access
- hybrid
- doi.org
- Licence
- Locations
- ACS Catalysis (publishedVersion, other-oa)
- Virtual Community of Pathological Anatomy (University of Castilla La Mancha) (submittedVersion, other-oa)
- Funders
- Leibniz-Gemeinschaft
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Catalytic Processes in Materials Science
- Physical Sciences › Engineering › Computational Mechanics › Heat and Mass Transfer in Porous Media
- Physical Sciences › Chemical Engineering › Catalysis › Catalysis and Oxidation Reactions
- Keywords
- microkinetic model, kinetic Monte Carlo, surface reaction kinetics, CO oxidation, Pd(100), RuO2(110), multiscale coupling, Shepard interpolation, reactor geometry, heat dissipation, gas-phase transport, time-scale separation
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