Regulating Electronic Structure of Single-Atom Catalysts toward Efficient Bifunctional Oxygen Electrocatalysis

Electronic structure of single-atom catalysts (SACS) is critical for bifunctional oxygen electrocatalysis by adjusting the binding energy in oxygen-containing intermediates. However, the regulation of electronic structure has always been a challenge to improve catalytic reactivity. Herein, by introducing a heterogenous metal, the electronic structure through a direct bonding interaction to the active center atom is effectively adjusted. Partial charge transfer between the two atoms optimizes the binding energy of intermediates and reducing the energy barrier of the catalytic reaction. Theoretical calculations confirm these effects and the uniform distribution of 3d orbitals, leading to the improvement of bifunctional oxygen electrocatalytic reactivity. Benefiting from these attributes, the as-constructed bifunctional catalyst enables outstanding electrocatalytic performances in both oxygen reduction and hydrogen oxidation in various energy storage systems. The generality and expandability of this strategy is demonstrated by further successful development of other dual-metal catalysts systems with various active metals.

Automated summary

The electronic structure of single-atom catalysts (SACS) plays a critical role in bifunctional oxygen electrocatalysis. In this study, the electronic structure was effectively adjusted by introducing a heterogenous metal that bonded directly to the active center atom. This adjustment resulted in optimized binding energy and reduced energy barriers for catalytic reactions. Theoretical calculations confirmed these effects and the uniform distribution of 3d orbitals, which improved the bifunctional oxygen electrocatalytic reactivity. The constructed bifunctional catalyst exhibited outstanding electrocatalytic performances in various energy storage systems. The generality and expandability of this strategy were demonstrated by the successful development of other dual-metal catalysts systems with different active metals.