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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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Published in: | Angewandte Chemie International Edition 2020-12, Vol.59 (52), p.23678-23683 |
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Main Authors: | , , , , , , , , , , , |
Format: | Article |
Language: | English |
Subjects: | |
Online Access: | Get full text |
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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. |
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ISSN: | 1433-7851 1521-3773 |
DOI: | 10.1002/anie.202008325 |