Predicting the Stability of Single-Atom Catalysts in Electrochemical Reactions

• DOI: 10.1021/acscatal.3c04801
• Publication Date: 2023-12-09T13:58:32Z
• Authors: Giovanni Di Liberto; Livia Giordano; Gianfranco Pacchioni
• Keywords: Chemical Stability; Pourbaix diagram; Catalytic cycle

The attention toward single-atom catalysts (SACs) for electrochemical processes is growing at an impressive pace. Electronic structure calculations play important role in this race by providing proposals of potentially relevant based on screening studies or the identification descriptors chemical activity. So far, almost all these predictions ignore a crucial aspect design catalyst: its stability. We propose simple yet general first-principles approach to predict stability SACs under working conditions pH and applied voltage. This construction thermodynamic cycle, where part information taken from experiment rest density functional theory (DFT) calculations. In particular, we make use formalism Pourbaix diagrams investigate reductive oxidative identify those that show pronounced tendency dissolve form other species. Applying procedure four transition metal atoms, Cr, Mn, Fe, Co, three supports, N-doped graphene, carbon nitride, covalent organic frameworks, key factor determining final binding energy free atom support. results several very good reactions are, fact, dramatically prone dissolution transformation species, suggesting every prediction SAC's catalytic activity should be accompanied parallel investigation