Clusters Induced Electron Redistribution to Tune Oxygen Reduction Activity of Transition Metal Single‐Atom for Metal–Air Batteries. (31st January 2022)

• Record Type: Journal Article
• Authors: Huang, Hongjiao; Yu, Deshuang; Hu, Feng; Huang, Shao‐Chu; Song, Junnan; Chen, Han‐Yi; Li, Lin Lin; Peng, Shengjie
• Is Part Of: Angewandte Chemie. Volume 134:Number 12(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-01-31
• Subjects: Clusters -- Metal–Air Battery -- Oxygen Reduction Reaction -- Single-Atom -- Synergistic Effect; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202116068
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: 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. Abstract : A general strategy of metal clusters regulating metal single‐atom sites is developed to boost the activities of oxygen reduction reaction (ORR) electrocatalysts (Fe, Co, Ni). Benefiting from the electron redistribution between active sites and substrate, the optimized catalyst exhibits remarkable activity with a half‐wave potential of 0.9 V vs. RHE and achieves high discharge voltages in various metal–air batteries.