期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202301833
关键词
Acid Electrolytes; Dissociative Mechanism; Distance Effect; Dual-Atomic Structure Engineering; Oxygen Reduction Reaction
We accelerate the kinetics of acid oxygen reduction reaction (ORR) by using a bi-functional ligand-assisted strategy to pre-control the distance of hetero-metal atoms. The synthesized Fe-Zn diatomic pairs on carbon substrates show outstanding ORR performance with an ultrahigh half-wave potential of 0.86 V vs. RHE in acid electrolyte. The specific distance range of around 3 angstrom between Fe-Zn diatomic pairs is the key to their ultrahigh activity, averaging the interaction between hetero-diatomic active sites and oxygen molecules.
The oxygen reduction reaction (ORR) on transition single-atom catalysts (SACs) is sustainable in energy-conversion devices. However, the atomically controllable fabrication of single-atom sites and the sluggish kinetics of ORR have remained challenging. Here, we accelerate the kinetics of acid ORR through a direct O-O cleavage pathway through using a bi-functional ligand-assisted strategy to pre-control the distance of hetero-metal atoms. Concretely, the as-synthesized Fe-Zn diatomic pairs on carbon substrates exhibited an outstanding ORR performance with the ultrahigh half-wave potential of 0.86 V vs. RHE in acid electrolyte. Experimental evidence and density functional theory calculations confirmed that the Fe-Zn diatomic pairs with a specific distance range of around 3 angstrom, which is the key to their ultrahigh activity, average the interaction between hetero-diatomic active sites and oxygen molecules. This work offers new insight into atomically controllable SACs synthesis and addresses the limitations of the ORR dissociative mechanism.
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