Rigid Ligand Confined Synthesis of Carbon Supported Dimeric Fe Sites with High-performance Oxygen Reduction Reaction Activity for Quasi-solid-state Rechargeable Zn-air Batteries

Dimeric metal sites (DiMSs) in carbon-based single atom catalysts (SACs) offer distinct advantages in optimizing the adsorption energies of the catalytic intermediates and reaction pathways over single atom sites, and thus inspires the investigations on the rational design of DiMSs-based SACs and th...

Full description

Saved in:
Bibliographic Details
Published in:Angewandte Chemie International Edition 2024-10, p.e202413933
Main Authors: Zong, Lingbo, Li, Mengke, Li, Ping, Fan, Kaicai, Wang, Lei
Format: Article
Language:English
Citations: Items that this one cites
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:Dimeric metal sites (DiMSs) in carbon-based single atom catalysts (SACs) offer distinct advantages in optimizing the adsorption energies of the catalytic intermediates and reaction pathways over single atom sites, and thus inspires the investigations on the rational design of DiMSs-based SACs and the accurate discernment of catalytic mechanisms. Here, dimeric Fe sites on carbon blacks (DiFe-N/CBs) are prepared using the precursor of metal-organic complex with a controlled structure, and the rigid ligand confinement secures the preservation of dimeric Fe sites during the thermal treatment. DiFe-N/CBs shows excellent electrocatalytic performance for oxygen reduction reaction (ORR) with a positive half-wave potential of 0.917 V, and excellent durability with negligible activity decay. Theoretical studies reveal that the dimeric Fe sites have an optimal adsorption of OOH* with the Yeager-type binding, illustrating the advantages of DiMSs over SAs in catalyzing ORR. The rechargeable aqueous and quasi-solid-state Zn-air battery assembled using DiFe-N/CBs-based air cathodes achieve small voltage gaps after long term charge/discharge test, showing great promises for practical applications. This synthetic strategy serves a novel platform to produce a scope of catalysts incorporating multimeric metal sites, and studies on the catalytic mechanism lay the foundation for establishing cooperative effect for multidentate adsorption reactions.
ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202413933