Efficient Machine-Learning-Aided Screening of Hydrogen Adsorption on Bimetallic Nanoclusters

Nanoclusters add an additional dimension in which to look for promising catalyst candidates, since catalytic activity of materials often changes at the nanoscale. However, the large search space of relevant atomic sites exacerbates the challenge for computational screening methods and requires the development of new techniques for efficient exploration. We present an automated workflow that systematically manages simulations from the generation of nanoclusters through the submission of production jobs, to the prediction of adsorption energies. The presented workflow was designed to screen nanoclusters of arbitrary shapes and size, but in this work the search was restricted to bimetallic icosahedral clusters and the adsorption was exemplified on the hydrogen evolution reaction. We demonstrate the efficient exploration of nanocluster configurations and screening of adsorption energies with the aid of machine learning. The results show that the maximum of the <i>d</i>-band Hilbert-transform ϵ_<i>u</i> is correlated strongly with adsorption energies and could be a useful screening property accessible at the nanocluster level.