Synergistic Effects of Ruthenium and Zinc Active Sites Fine Tune the Electronic Structures of Augmented Electrocatalysis

Abstract As the demand for cleaner energy becomes a paramount objective of sustainable development, the advancement of cutting‐edge engineered materials for a wide range of applications becomes increasingly vital. Tailoring catalyst properties through precise design and electronic state tuning is essential for adapting these materials to large‐scale energy applications. Given this, an effective electronic fine‐tuning (EFT) strategy is presented to optimize the electronic structures of single‐atom Zn site and Ru species, synergistically enhancing the both electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Benefiting from the interaction between Ru species anchored on hierarchically layered nanosheets and isolated Zn atoms (Ru@Zn‐SAs/N‐C), the catalyst exhibits superior ORR and HER activities compared to the benchmark Pt/C catalyst. X‐ray absorption spectroscopy and density functional theory (DFT) calculations confirm a novel EFT effect between a single Zn site and Ru species, that enables the Ru@Zn‐SAs/N‐C approaches the optimal scaling relation between * OOH and * OH, breaking the universal ORR scaling limitation. Additionally, the optimal G H* value positions Ru@Zn‐SAs/N‐C near the apex of the theoretical HER volcano model. This work provides an innovative avenue for regulating the electronic localization of catalytic active centers by virtue of carbon substrate and offers valuable insights for designing high‐efficiency electrocatalysts.