A computational approach for mapping electrochemical activity of multi-principal element alloys

Abstract Multi principal element alloys (MPEAs) comprise an atypical class of metal alloys. MPEAs have been demonstrated to possess several exceptional properties, including, as most relevant to the present study a high corrosion resistance. In the context of MPEA design, the vast number of potential alloying elements and the staggering number of elemental combinations favours a computational alloy design approach. In order to computationally assess the prospective corrosion performance of MPEA, an approach was developed in this study. A density functional theory (DFT) – based Monte Carlo method was used for the development of MPEA ‘structure’; with the AlCrTiV alloy used as a model. High-throughput DFT calculations were performed to create training datasets for surface activity/selectivity towards different adsorbate species: O2-, Cl- and H+. Machine-learning (ML) with combined representation was then utilised to predict the adsorption and vacancy energies as descriptors for surface activity/selectivity. The capability of the combined computational methods of MC, DFT and ML, as a virtual electrochemical performance simulator for MPEAs was established and may be useful in exploring other MPEAs.