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Introduction

Heterogeneous catalysis plays a central role in modern chemical technology, with CO\(_2\) conversion reactions being particularly important for addressing climate change and developing sustainable chemical processes. Among various catalyst systems, cobalt-based catalysts have shown promising activity for CO\(_2\) hydrogenation, producing valuable products such as methanol, methane, and carbon monoxide.

This second part of the tutorial is based on the computational methodologies and findings from two recent publications 1 2. This part introduces the additional complexity of spin polarization that must be handled when modeling magnetic materials like cobalt.

Catalysis Sketch Cobalt Silica

We will explore how to study cobalt-based catalysts at different scales - from single atoms to clusters to supported catalyst systems - culminating in the calculation of CO\(_2\) adsorption energies on a Co\(_{20}\)/SiO\(_2\) model. This multi-scale approach allows us to understand how the electronic and magnetic properties evolve from isolated atoms to catalytically active materials.

The referenced studies have demonstrated that the CO\(_2\) adsorption energy serves as an important descriptor that correlates with catalytic performance in CO\(_2\) hydrogenation reactions 2. Adsorption energies in general represent one of the most fundamental descriptors in heterogeneous catalysis, providing quantitative insight into the interaction strength between reactant molecules and catalyst surfaces. These energies are critical for understanding reaction mechanisms and predicting catalytic activity across different materials. According to the Sabatier principle, optimal catalysts bind reactants strongly enough to facilitate activation but weakly enough to allow product desorption, also directly quantifiable by adsorption energies. In practical applications, these energies serve as key inputs for microkinetic models that predict reaction rates and selectivity, enable computational screening of novel catalytic materials before experimental synthesis, and help explain structure-activity relationships that guide rational catalyst design.

  1. Belthle, K. S. et al., J. Am. Chem. Soc. 144 (46), 21232−21243 (2022). ↩

  2. Miyazaki, R. et al., J. Am. Chem. Soc. 146, 5433−5444 (2024). ↩↩