Vacancy Defects Inductive Effect of Asymmetrically Coordinated Single-Atom Fe─N3 S1 Active Sites for Robust Electrocatalytic Oxygen Reduction with High Turnover Frequency and Mass Activity
© 2023 Wiley-VCH GmbH.
Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 11 vom: 01. März, Seite e2308243 |
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Auteur principal: | |
Autres auteurs: | , , , , , , , , , , , , , , , |
Format: | Article en ligne |
Langue: | English |
Publié: |
2024
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Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
Sujets: | Journal Article controllable synthesis electrocatalysis oxygen reduction reaction single-atom catalyst |
Résumé: | © 2023 Wiley-VCH GmbH. The development of facile, efficient synthesis method to construct low-cost and high-performance single-atom catalysts (SACs) for oxygen reduction reaction (ORR) is extremely important, yet still challenging. Herein, an atomically dispersed N, S co-doped carbon with abundant vacancy defects (NSC-vd) anchored Fe single atoms (SAs) is reported and a vacancy defects inductive effect is proposed for promoting electrocatalytic ORR. The optimized catalyst featured of stable Fe─N3 S1 active sites exhibits excellent ORR activity with high turnover frequency and mass activity. In situ Raman, attenuated total reflectance surface enhanced infrared absorption spectroscopy reveal the Fe─N3 S1 active sites exhibit different kinetic mechanisms in acidic and alkaline solutions. Operando X-ray absorption spectra reveal the ORR activity of Fe SAs/NSC-vd catalyst in different electrolyte is closely related to the coordination structure. Theoretical calculation reveals the upshifted d band center of Fe─N3 S1 active sites facilitates the adsorption of O2 and accelerates the kinetics process of *OH reduction. The abundant vacancy defects around the Fe─N3 S1 active sites balance the OOH* formation and *OH reduction, thus synergetically promoting the electrocatalytic ORR process |
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Description: | Date Revised 14.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202308243 |