New theoretical publication on CO hydrogenation over Rh nanocatalysts, explaining experimentally observed trends in the selectivity of different types of active sites found at nanoparticles toward C1 and C2 species, i.e., methane, acetaldehyde and ethanol.

In this work, we employ accelerated first-principles kinetic Monte Carlo (KMC) simulations and explicitly and systematically account for lateral adsorbate-adsorbate interactions at the catalyst surface through a cluster expansion approach. The results are compared to corresponding microkinetic simulations employing the mean-field approximation parametrized to include a dependence on the adsorbate coverage in the rate equations. We show that the subtle selectivity trends observed in experiments can only be reproduced using the KMC approach and highlight the different roles lateral interactions can play for different catalytic systems. The results are important for understanding and designing active and selective heterogeneous catalysts.

https://pubs.acs.org/articlesonrequest/AOR-GSESM5CUVHRFQH5FJJKK