Density functional study of electrochemical small-molecule conversion on single-atom catalysts

Abstract

The electrochemical small molecule conversion reaction is a promising strategy for research on global warming, air pollution, and renewable energy. In an electrochemical reaction, it is important to design a catalyst suitable for the purpose. Among them, single-atom catalysts can maximize atomic efficiency and enhance catalytic performance by controlling the coordinating ligand environment, so they are used in various small molecule conversion reactions. However, the origin of the high performance has not been determined yet. In this thesis, the nature of single-atom electrochemical catalysts was studied through atomic-level analysis through density functional theory. Furthermore, a comprehensive understanding of the effect of the entire electrochemical reaction system on the catalytic reaction was presented through a study on the effect of the coordination environment and electrode on the catalytic performance. In particular, the reaction mechanism in the actual operating environment was studied through the calculation of the constant potential scheme as well as the common constant charge scheme calculation. Through this, it was possible to present guidelines for the design of a single-atom catalyst suitable for each small molecule conversion reactions.