Assessing the reliability of calculated catalytic ammonia synthesis rates

TLDR

The study introduces a general method for estimating uncertainty in calculated materials properties from DFT and an approach to evaluate the probability that a catalyst outperforms a known standard. The method is illustrated by calculating the catalytic rate of ammonia synthesis over a range of transition‑metal catalysts, showing how to estimate uncertainties in such calculations. The analysis demonstrates that correlations between DFT errors reduce predicted rate errors, that uncertainties depend strongly on reaction conditions and catalyst material, and that relative rates between catalysts are better described than absolute rates.

Abstract

We introduce a general method for estimating the uncertainty in calculated materials properties based on density functional theory calculations. We illustrate the approach for a calculation of the catalytic rate of ammonia synthesis over a range of transition-metal catalysts. The correlation between errors in density functional theory calculations is shown to play an important role in reducing the predicted error on calculated rates. Uncertainties depend strongly on reaction conditions and catalyst material, and the relative rates between different catalysts are considerably better described than the absolute rates. We introduce an approach for incorporating uncertainty when searching for improved catalysts by evaluating the probability that a given catalyst is better than a known standard.