Rational design of single atom catalysts through factor-based study: From formulating electronic factors to tailoring materials properties

Abstract

Recently, single-atom catalysis (SACs) has been extensively studied due to the high activity and efficiency of using all atoms as catalysts. Even though SACs are ideal catalysts that can utilize the advantages of both homogeneous and heterogeneous catalysts, they cannot be used in large quantities due to agglomeration issues caused by the increasing chemical potential as the catalyst size decreases, and therefore there is a need to develop rationally SACs with excellent properties. In this study, we attempted to unveil a factor that is a link between catalysts and descriptors that represent their properties. Based on these proposed design factors, we designed and verified catalysts with expected excellent properties. In the first part, graphene-based SACs for oxygen reduction reaction were studied. The frontier orbital energy level of the single atom and the Fermi energy level of the catalyst were proposed as factors affecting the descriptors of catalytic activity and stability, and we studied the control of the factors through doping strategies. In the second part, hybrid oxide interface-supported SACs for low-temperature water gas shift reactions were studied, the reducibility of the oxides was proposed as a factor affecting the catalytic activity and stability descriptors, and the modulation of the design factor was studied.