Microkinetic modelling in computational homogeneous catalysis and beyond

Sciortino, Giuseppe; Maseras, Feliu

doi:10.1007/s00214-023-03044-2

Cited by 8 publications

(2 citation statements)

References 60 publications

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“…Today, the most established approach for incorporating these effects into computational catalysis is through explicit microkinetic modeling (MKM). [33][34][35][36][37][38][39][40][41][42][43] This framework allows for a comprehensive analysis of complex reaction mechanisms that offers direct access to the evolution of product concentrations over time. To accomplish this, however, MKM requires independently solving a system of differential equations for each free energy profile, which renders this method impractical for the high-throughput analysis of hundreds or thousands of candidate catalysts.…”

Section: Introductionmentioning

confidence: 99%

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Worakul,

Laplaza,

Das

et al. 2024

Preprint

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Molecular volcano plots, which facilitate the rapid prediction of the activity and selectivity of prospective catalysts, have emerged as powerful tools for computational catalysis. Here, we integrate microkinetic modeling into the volcano plot framework to develop "microkinetic molecular volcano plots." The resulting unified computational framework allows the influence of important reaction parameters, including temperature, reaction time, and concentration, to be quickly incorporated and more complex situations, such as off-cycle resting states and coupled catalytic cycles, to be tackled. Compared to previous generations of molecular volcanoes, these microkinetic counterparts offer a more comprehensive understanding of catalytic behavior, in which selectivity and product ratios can be explicitly determined by tracking the evolution of each product concentration over time. This is demonstrated by examining two case studies, rhodium-catalyzed hydroformylation and metal-catalyzed hydrosilylation, in which the unique insights provided by microkinetic modeling, as well as the ability to simultaneously screen catalysts and reaction conditions, is highlighted. To facilitate the construction of these plots/maps, we introduce mikimo, a Python program that seamlessly integrates with our previously developed automated volcano builder, volcanic.

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Section: Introductionmentioning

confidence: 99%

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Worakul,

Laplaza,

Das

et al. 2024

Preprint

View full text Add to dashboard Cite

show abstract

“…Other, potentially important physical factors, such as the influence of reactant concentration, cannot be described. Today, the most established approach for incorporating these effects into computational catalysis is through explicit microkinetic modeling (MKM). − This framework allows for a comprehensive analysis of complex reaction mechanisms that offers direct access to the evolution of product concentrations over time. To accomplish this, however, MKM first requires complete free energy profiles (often obtained through DFT computations) for each catalyst of interest, followed by solving a system of differential equations.…”

Section: Introductionmentioning

confidence: 99%

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Worakul,

Laplaza,

Das

et al. 2024

ACS Catal.

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Microkinetic Model as a Crucial Tool for Understanding Homogeneous Catalysis

Rama,

Nova,

Nicasio

2024

ChemCatChem

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Microkinetic modeling is a computational tool that allows simulating the evolution of the concentration of catalytically relevant species with time, providing a description of the catalytic system closer to the experimental. Microkinetic models have been mainly applied in organometallic catalysis as a means for validating mechanistic proposals by comparing experimental and computed rates and concentrations at a given time. However, this tool becomes very useful when studying complicated reaction mechanisms, aiding in identifying the catalyst resting state, optimizing reaction conditions or improving the catalyst design. In this Concept, we focus on these applications of microkinetic modeling through the discussion of some selected examples. In addition, we also point out some of the challenges and limitations we may face when building microkinetic models, which may explain why they are still underused.

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Microkinetic modelling in computational homogeneous catalysis and beyond

Cited by 8 publications

References 60 publications

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Microkinetic Molecular Volcano Plots for Enhanced Catalyst Selectivity and Activity Predictions

Microkinetic Model as a Crucial Tool for Understanding Homogeneous Catalysis

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