Adsorbed species and surface chemistry plays an important role in a large range of applications and technologies, especially in catalysis and electrocatalysis, separations, and device fabrication through film growth. Due to its technological relevance, a tremendous effort has been made worldwide to determine and predict reactions rates and selectivity for networks of elementary surface reactions through microkinetic modeling. These models depend on accurate predictions of reaction rates and equilibrium constants both which depend on enthalpy and entropy of adsorbates. We have developed an easy to implement method to calculate entropy of adsorbates using standard DFT approaches. This model joins the two limiting cases for adsorbates on a surface, the 2D ideal lattice gas model and the 2D ideal gas model, making it valid over large temperature range and for a verity of adsorbates. To verify this model, density functional theory was used to calculate adsorbate entropies of four different adsorbate species and found to agree well with experimental results. This method has been implemented into free computational tools, ASE and CatMAP, making it widely available.

Computational approach to determine entropy of adsorbates in catalytic reactions

2019 Fall National Meeting

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