Charting the Electronic States of Intermetallic Catalysts

The electronic structure-based descriptors, such as nth moment theory and DOS similarity, have been widely used to rationalize catalytic performance. However, their effectiveness remains unclear. In this study, we selected intermetallic compounds as a platform to examine the variety of electronic states that can be catalytically active. Utilizing high-throughput density functional theory (DFT) calculations, we enumerated all possible low-index surfaces from the reported intermetallic compounds in the ICSD and Materials Project Database. This high-throughput screening yielded a computational database with over 10,000 surfaces. Based on this DFT dataset, we compared the typical electronic structure-based descriptors with well-known HER/ORR catalysts, such as Pt and Ir, to identify promising new catalysts for HER or ORR. Among all the promising candidates screened, the electrochemical stability of these catalysts is also discussed using Pourbaix diagrams.