Synergistic dual sites of Zn-Mg on hierarchical porous carbon as an advanced oxygen reduction electrocatalyst for Zn-air batteries.

The development of cost-effective and high-performance non-noble metal catalysts for the oxygen reduction reaction (ORR) holds substantial promise for real-world applications. Introducing a secondary metal to design bimetallic sites enables effective modulation of a metal-nitrogen-carbon (M-N-C) catalyst's electronic structure, providing new opportunities for enhancing ORR activity and stability. Here, we successfully synthesized an innovative hierarchical porous carbon material with dual sites of Zn and Mg (Zn/Mg-N-C) using polymeric ionic liquids (PILs) as precursors and SBA-15 as a template through a bottom-up approach. The hierarchical porous structure and optimized Zn-Mg bimetallic catalytic centers enable Zn/Mg-N-C to exhibit a half-wave potential of 0.89 V, excellent stability, and good methanol tolerance in 0.1 M KOH solution. Theoretical calculations indicated that the Zn-Mg bimetallic sites in Zn/Mg-N-C effectively lowered the ORR energy barrier. Furthermore, the Zn-air batteries assembled based on Zn/Mg-N-C demonstrated an outstanding peak power density (298.7 mW cm-2) and superior cycling stability. This work provides a method for designing and synthesizing bimetallic site catalysts for advanced catalysis.