Density Functional Theory Calculations to Increase the Efficiency of Oxygen Electrode Catalysts from Ytterbium Single Atom Catalysts Using Nitrogen Solid Supports

The research and design of oxygen electrode catalysts are of great significance for achieving carbon peak and carbon neutrality goals. In this study, a comprehensive study, including detailed stability, adsorption properties, electronic characteristics, and activity center configuration of ytterbium single-atom catalysts (YbN_x-gra) loaded on two-dimensional nanomaterials under acidic conditions, was conducted according to density functional theory calculations. The results indicated that with the increase of nitrogen content, the efficiency of the ytterbium single-atom oxygen electrode catalysts using nitrogen solid supports was improved. There are several good linear relationships between the adsorption free energy of intermediates, such as ΔG_OH* and ΔG_OOH*, ΔG_OH*, and ΔG_O*. This provides a basis for the drawing of volcano maps and the rapid prediction of highly active catalysts. Due to the reaction selectivity of catalysts, the O* intermediates and 2OH* intermediates accompany the catalytic reaction. For catalytic activity, the YbN₄-II catalyst showed the lowest overpotential of ORR which η^ORR = 0.42 V. In particular, the η^ORR and η^OER of the YbN₃-IV catalyst were as low as 0.58 and 0.41 V, respectively. The linear relationships and volcano plots indicate the feasibility of some YbN_x-gra catalysts, making them promising candidates for oxygen electrode catalysts.