Pynta─An Automated Workflow for Calculation of Surface and Gas-Surface Kinetics.

Area of Science:

• Computational Chemistry
• Materials Science
• Chemical Engineering

Background:

• Industrial processes heavily rely on heterogeneous catalysis, but experimental optimization is often impractical.
• Microkinetic models are essential for exploring numerous catalysts and conditions but require accurate parameter estimation.
• Manual calculation of thermochemical and kinetic parameters is laborious, time-consuming, and prone to errors.

Purpose of the Study:

• To introduce Pynta, a novel workflow software designed to automate the calculation of surface and gas-surface reaction parameters.
• To enable efficient and accurate generation of microkinetic models for heterogeneous catalytic systems.
• To address the limitations of manual parameter estimation in computational catalysis.

Main Methods:

• Pynta automates the generation of initial guesses for species and saddle points, followed by optimization, frequency, and IRC calculations.
• It computes thermochemistry and rate coefficients, considering all unique adsorption configurations for adsorbates and saddle points.
• Pynta implements harmonically forced saddle point searching (HFSP), a novel, reaction-class-agnostic method for fast and reliable saddle point guess generation using GFN1-xTB.

Main Results:

• Pynta successfully demonstrated on 11 diverse reactions across various species (monodentate, bidentate, gas-phase) and reaction classes.
• The software handled both low and high index facets of Copper (Cu), showcasing its versatility.
• Results highlight the critical importance of considering all unique adsorbate configurations for interadsorbate group transfers and reactions on high-index surfaces.

Conclusions:

• Pynta significantly streamlines the computational workflow for microkinetic modeling in heterogeneous catalysis.
• The HFSP method provides an efficient and robust approach to saddle point identification.
• Comprehensive consideration of adsorption configurations is vital for accurate microkinetic modeling, especially for complex surfaces and reactions.