Synergistic Combination Inspired by the Steaming of Buns of Ce “Flour” and Zn “Baking Soda” Punches up the Oxygen Reduction

Abstract Ce‐based single‐atomic catalysts (SACs) are highly promising as the oxygen reduction reaction (ORR) catalysts due to the unique 4f orbital, whereas the modulating the coordination environment of single‐atomic Ce sites remains challenging using simple strategies for enhancing the ORR performance. Inspired by the process of bun steaming, a composite catalyst comprising CeO ₂ nanoparticles and single‐atomic Ce sites within nitrogen‐doped carbon matrix (CeO ₂ /CeZn SACs@NC) is successfully prepared by utilizing cerium salt as the primary material of flour and zinc salts as the leavening agent. X‐ray absorption spectroscopy confirms that the induces the transformation from Ce─O coordination (Ce‐O ₅ ) to Ce─N coordination (Ce‐N ₅ ), which is verified to reduce reaction energy barriers of the hydrogenation of ^* OH as the rate‐determining step during the ORR process from the theoretical calculation results. Notably, the optimal CeO ₂ /CeZn SACs@NC achieves a remarkable ORR performance with half‐wave potential of 0.85 V in 0.1 m KOH and excellent Zn‐air battery performance with the specific capacity of 806 mAh g _Zn ⁻¹ at 10 mA cm ⁻² , as well as remarkable long‐term stability.