Ce Single‐Atoms Modulation of Cu Atomic Clusters for Enhanced Oxygen Reduction and Durable Zn‐Air Batteries

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Abstract Atomically dispersed electrocatalysts represent promising alternatives to Pt‐based catalysts for the oxygen reduction reaction (ORR), yet their performance remains constrained by suboptimal electronic configurations and instability. A heteroatomic catalyst featuring Ce single atoms and Cu clusters anchored on nitrogen‐doped carbon (Ce‐N‐C/Cu clu ) is presented and synthesized through a facile one‐step pyrolysis approach. The optimized Ce‐N‐C/Cu clu exhibits exceptional ORR activity in alkaline media, along with remarkable stability (92% current retention after 30 000 s). When employed as an air cathode in Zn‐air batteries, it achieves both high specific capacity (729.9 mAh g Zn −1 ) and unprecedented cycling stability (1600 h). Combined experimental and theoretical analyses reveal that Ce single‐atoms with distinctive 4 f electrons serve as electronic modulators, inducing charge redistribution and upshifting the d ‐band center of adjacent Cu clusters. This electronic synergy optimizes O 2 adsorption energy and intermediate binding energy, thereby substantially enhancing ORR kinetics. This work establishes a universal strategy for rare‐earth‐mediated electronic modulation of transition metal catalysts toward the design of high‐performance electrocatalysts.

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