Asymmetrically Coordinated Calcium Single Atom for High-Performance Oxygen Reduction Reaction.
Inorg Chem
; 63(28): 13086-13092, 2024 Jul 15.
Article
em En
| MEDLINE
| ID: mdl-38937860
ABSTRACT
S-block single atoms represent an ideal catalyst for the oxygen reduction reaction (ORR) as they can suppress the Fenton reaction. However, the symmetry of the s/p orbitals tends to generate either an excessively strong or weak interaction with intermediates. Herein, Ca single atoms coordinated with -S, -OP, and three N atoms (Ca/NPS-HC) were fabricated to modulate the adsorption of intermediates and promote the efficiency of s-block ORR catalysts. The experimental results from ORR demonstrated that the Ca/NPS-HC catalyst exhibited outstanding catalytic capability with a half-wave potential of 0.89 V, a kinetic current density of 56.6 mA cm-2 at 0.85 V, and a Tafel slope of 42 mV dec-1, outperforming commercial Pt/C. The detailed mechanistic studies revealed that the asymmetric coordination of Ca single atoms led to the symmetry-breaking of electron distribution in Ca single atoms, attenuating the s-p hybridization from the intermediate adsorption process, and thereby minimizing the energy barrier of the whole ORR.
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Bases de dados:
MEDLINE
Idioma:
En
Revista:
Inorg Chem
Ano de publicação:
2024
Tipo de documento:
Article
País de afiliação:
China