Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts.

The oxygen reduction reaction (ORR) is critical for energy conversion technologies like fuel cells and metal-air batteries. However, advancing efficient and stable ORR catalysts remains a significant challenge. Iron-based single-atom catalysts (Fe SACs) have emerged as promising alternatives to precious metals. However, their catalytic performance and stability remain constrained. Introducing a second metal (M) to construct Fe─M dual-atom catalysts (Fe─M DACs) is an effective strategy to enhance the performance of Fe SACs. This review provides a comprehensive overview of the recent advancements in Fe-based DACs for ORR. It begins by examining the structural advantages of Fe─M DACs from the perspectives of electronic structure and reaction pathways. Next, the precise synthetic strategies for DACs are discussed, and the structure-performance relationships are explored, highlighting the role of the second metal in improving catalytic activity and stability. The review also covers in situ characterization techniques for real-time observation of catalytic dynamics and reaction intermediates. Finally, future directions for Fe─M DACs are proposed, emphasizing the integration of advanced experimental strategies with theoretical simulations as well as artificial intelligence/machine learning to design highly active and stable ORR catalysts, aiming to expand the application of Fe─M DACs in energy conversion and storage technologies.