Site-Specific Electron-Driving Observations of CO2 -to-CH4 Photoreduction on Co-Doped CeO2 /Crystalline Carbon Nitride S-Scheme Heterojunctions
© 2022 Wiley-VCH GmbH.
| Publié dans: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 27 vom: 27. Juli, Seite e2200929 |
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| Auteur principal: | |
| Autres auteurs: | , , |
| Format: | Article en ligne |
| Langue: | English |
| Publié: |
2022
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| Accès à la collection: | Advanced materials (Deerfield Beach, Fla.) |
| Sujets: | Journal Article CO2-to-CH4 photoreduction S-scheme heterojunctions bimetallic co-catalyst regulation crystalline carbon nitride directional charge transfer |
| Résumé: | © 2022 Wiley-VCH GmbH. Photoexcited dynamic modulation, maximizing the effective utilization of photoinduced electron-hole pairs, dominates the multiple electrons-involving reduction pathways for terminal CH4 evolution during CO2 photoreduction. Yet, the site-specific regulation of directional charge transfer by modification of an S-scheme heterojunction has seldom been discussed. Herein, an atomic-level tailoring strategy by anchoring single-atomic Co into CeO2 co-catalyst rather than carbon nitride supports, which can selectively favor CO2 -to-CH4 photoreduction, is reported. Through in situ dynamic tracking investigations, this study identifies that surface Co-embedded bimetallic CeCo conjunction is the key feature driving a strong interconnection of dynamical charge states through S-scheme heterojunctions. The Co-embedded modification into CeO2 co-catalysts is demonstrated to have a critical effect on directional charge control, accelerating the driving of electrons from the carbon nitride donations to site-specific Co hubs, which thereby promotes electronic transferability for electrons-involving CH4 formation. As a result, an unprecedented CH4 yield (181.7 µmol g-1 ) is obtained with a high turnover number (411.4) through a fully gas-solid reaction, demonstrating its potential toward targeted CH4 formation without adding any sacrificial agent |
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| Description: | Date Revised 07.07.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202200929 |