Exploring Metal Nanocluster Catalysts for Ammonia Synthesis Using Informatics Methods: A Concerted Effort of Bayesian Optimization, Swarm Intelligence, and First-Principles Computation.

This paper details the use of computational and informatics methods to design metal nanocluster catalysts for efficient ammonia synthesis. Three main problems are tackled: defining a measure of catalytic activity, choosing the best candidate from a large number of possibilities, and identifying the thermodynamically stable cluster catalyst structure. First-principles calculations, Bayesian optimization, and particle swarm optimization are used to obtain a Ti 8 nanocluster as a catalyst candidate. The N 2 adsorption structure on Ti 8 indicates substantial activation of the N 2 molecule, while the NH 3 adsorption structure suggests that NH 3 is likely to undergo easy desorption. The study also reveals several cluster catalyst candidates that break the general trade-off that surfaces that strongly adsorb reactants also strongly adsorb products.