The Active Thermochemical Tables (ATcT) provide benchmark-quality thermochemistry and rigorous uncertainty quantification for primarily gas-phase species by constructing, analyzing, and solving the underlying Thermochemical Network. To meet the needs of heterogeneous catalysis, we report the extension of ATcT to surface-bound species, beginning with a curated suite of Pt(111) adsorbates of high catalytic relevance.

Our workflow integrates first-principles calculations and experimental data to provide internally consistent enthalpies, entropies, and heat capacities referenced to the thermochemical standard, heats of formation. The resulting thermochemical values are embedded in the broader ATcT Thermochemical Network, enabling uncertainty-aware coupling between gas-phase and surface-bound species and supporting robust microkinetic modeling. In parallel, we propose practical conventions and machine-readable metadata for species definition (site specification, coverage annotation) to promote reuse across DFT and ML datasets and reactor models.

We will present the initial Pt(111) dataset, validation against independent constraints, and case studies illustrating the impact of uncertainty-quantified adsorbate thermochemistry. This work lays the groundwork for a further expansion of ATcT to adsorbates on diverse catalysts, helping catalysis researchers converge on best practices and standards for adsorbate thermochemistry.

Richard West

Northeastern University

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