Revealing Isolated M−N3C1 Active Sites for Efficient Collaborative Oxygen Reduction Catalysis

Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limite...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2020-12, Vol.59 (52), p.23678-23683
Main Authors: Li, Feng, Han, Gao‐Feng, Bu, Yunfei, Noh, Hyuk‐Jun, Jeon, Jong‐Pil, Shin, Tae Joo, Kim, Seok‐Jin, Wu, Yuen, Jeong, Hu Young, Fu, Zhengping, Lu, Yalin, Baek, Jong‐Beom
Format: Article
Language:English
Subjects:
active sites
Atomic properties
Atomic structure
Catalysis
Catalysts
Cobalt
Collaboration
collaborative catalysis
Copper
Energy technology
Iron
Oxygen
oxygen reduction reaction
Renewable energy technologies
single atom catalyst
Transition metals
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Summary:Single atom catalysts (SACs) are of great importance for oxygen reduction, a critical process in renewable energy technologies. The catalytic performance of SACs largely depends on the structure of their active sites, but explorations of highly active structures for SAC active sites are still limited. Herein, we demonstrate a combined experimental and theoretical study of oxygen reduction catalysis on SACs, which incorporate M−N3C1 site structure, composed of atomically dispersed transition metals (e.g., Fe, Co, and Cu) in nitrogenated carbon nanosheets. The resulting SACs with M−N3C1 sites exhibited prominent oxygen reduction catalytic activities in both acidic and alkaline media, following the trend Fe−N3C1 > Co−N3C1 > Cu−N3C1. Theoretical calculations suggest the C atoms in these structures behave as collaborative adsorption sites to M atoms, thanks to interactions between the d/p orbitals of the M/C atoms in the M−N3C1 sites, enabling dual site oxygen reduction. Isolated M−N3C1 active sites were engineered into the single atom catalysts for efficient oxygen reduction catalysis. Theoretical calculations proposed that the M/C atoms in the active sites served as dual adsorption sites, enabling more efficient collaborative catalysis.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202008325