Breaking the activity–stability trade-off in single-atom catalysts via CoFe dual-sites for efficient zinc–air batteries

Rational design and the development of efficient bifunctional oxygen electrocatalysts play a vital role in advancing zinc–air batteries. Single-atom catalysts (SACs) have demonstrated high turnover frequency and site density, while their practical implementation is fundamentally limited by the persistent activity–stability trade-off, that is, the rigid scaling relationships governing oxygen redox intermediates. To address these challenges, density functional theory (DFT) calculations are firstly carried out to reveal that heterometallic coordination induces electronegativity-driven charge redistribution at Co centers, and subsequently, a series of atomically dispersed CoM/NC catalysts are synthesized via a scalable movable type printing method. The optimized CoFe/NC configuration holds an exceptional bifunctional activity with small potential gap between oxygen reduction and evolution as 0.641 V, which outperforms those of the Pt/C-RuO 2 . The CoFe/NC catalyst exhibits exceptional bifunctional activity in rechargeable Zn–air batteries, delivering a peak power density of 227 mW cm −2 alongside robust stability exceeding 350 h of continuous cycling. This work establishes a universal paradigm for breaking the intrinsic limitations of SACs through electronic-structure engineering in dual-metal architectures. • Density functional theory was used to establish a dual-function database for Co-based catalysts. • Various Co-based catalysts with dual metals were synthesized by a universal strategy. • The optimized CoFe/NC catalyst exhibited high performance in zinc–air batteries. • A synergetic mechanism for improving electrocatalytic performance was uncovered comprehensively.