Using a general method for estimating the exchange-correlation uncertainty in density functional theory calculations we estimate the uncertainty on catalytic rate of ammonia synthesis over a range of transition metal catalysts. In general the estimated error is significantly reduced due to correlations in the error between various intermediates and surfaces, highlighting the need for systematic methods of error estimation. Uncertainties are shown to be a complex function of reaction condition and catalyst material, and we demonstrate that relative rates between different catalysts are better described than the absolute rates. A new approach is introduced where catalysts can be screened based on the probability that their rate will be an improvement over a given standard, rather than on the basis of absolute predicted rates. The implications and challenges of analyzing sources of uncertainty beyound exchange-correltaion energy are discussed, along with the potential opportunities for application of the probabilistic approach to other areas of computational materials design.

Implications of uncertainty on computationally predicted rates and trends in catalytic ammonia synthesis

248th National Meeting (2014)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.