Cluster (spacecraft)

Nanotechnology

Organic chemistry

Covalent bond

Atom (system on chip)

Redistribution (election)

Politics

Electron transfer

Transition metal

Catalysis

Political science

Embedded system

Nanoparticle

Chemical physics

Chemistry

Metallurgy

Materials science

Programming language

Computer science

Metal

Oxygen

Photochemistry

Angewandte Chemie International Edition

Oxygen reduction reaction (ORR) activity can be effectively tuned by modulating the electron configuration and optimizing the chemical bonds. Herein, a general strategy to optimize the activity of metal single-atoms is achieved by the decoration of metal clusters via a coating-pyrolysis-etching route. In this unique structure, the metal clusters are able to induce electron redistribution and modulate M-N species bond lengths. As a result, M-ACSA@NC exhibits superior ORR activity compared with the nanoparticle-decorated counterparts. The performance enhancement is attributed to the optimized intermediates desorption benefiting from the unique electronic configuration. Theoretical analysis reinforces the significant roles of metal clusters by correlating the ORR activity with cluster-induced charge transfer. As a proof-of-concept, various metal-air batteries assembled with Fe-ACSA@NC deliver remarkable power densities and capacities. This strategy is an effective and universal technique for electron modulation of M-N-C, which shows great potential in application of energy storage devices.

Clusters Induced Electron Redistribution to Tune Oxygen Reduction Activity of Transition Metal Single‐Atom for Metal–Air Batteries