Assessing Catalytic Rates of Bimetallic Nanoparticles with Active Site Specificity - A Case Study using NO Decomposition

Bimetallic alloys have emerged as an important class of catalytic materials, spanning a wide range of shapes, sizes, and compositions. The combinatorics across this wide materials space makes predicting catalytic turnovers of individual active sites challenging. Herein, we introduce the stability of active sites as a descriptor for site-resolved reaction rates. The site stability unifies structural and compositional variations in a single descriptor. We compute this descriptor using coordination-based models trained with DFT calculations. Our approach enables instantaneous predictions of catalytic turnovers for nanostructures up to 12 nm in size. Using NO dissociation as probe reaction, we identify that octahedral Au-Pt core-shell nanoparticles and 3 nm 0.5:0.5 AuPt random alloys yield greater than 10 times higher compared to monometallic Pt nanoparticles. By prescribing specific sizes, morphologies, and compositions of optimal catalytic nanoparticles, our method provides tailored guidance to experiments for rationally designing bimetallic catalysts.